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Superb adsorption capacity of ferrocene-based covalent organic frameworks towards Congo red with high-pH resistance
Shenglin Wang, Qianqian Yan, Jiaxin Yang, Hui Hu, Songtao Xiao, Yanan Gao
, Available online  , doi: 10.1016/j.gee.2024.11.008
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Porous materials are excellent adsorbents for the removal of organic dyes from sewage and play a significant role in environmental restoration. Herein, two ferrocene (Fc)-based covalent organic frameworks (Fc-COFs), namely FcTF-COF and FcBD-COF, are successfully synthesized for the first time through a solvothermal method, and the obtained Fc-COFs powders are used to adsorb Congo red (CR) from water. The results show that both FcTF-COF and FcBD-COF have superb adsorption performance towards CR with ultrahigh adsorption capability of 1672.2 mg g–1 and 1983.7 mg g–1 at pH = 4.0, respectively, outperforming the majority of the reported solid porous adsorbents. The maximum adsorption of both Fc-COFs agrees with the Sips adsorption isothermal model, indicating that their adsorption was dominated by heterogeneous adsorption. The Coulombic interactions, hydrogen bonding, π-π interactions and ion-dipolar interactions should all contribute to their ultrahigh CR adsorption capability and high-pH resistance performance regardless of the pH in the range of 4 to 9. In addition, after five cycles, both COFs still remain their exceptional high CR adsorption capabilities. This study offers a prospective organic porous adsorbent with promising applications for organic dye removal in sewage processing.
Tricycloquinazoline-based monolayer conjugated metal–organic frameworks as promising hydrogen storage media: A theoretical investigation
Zhaoshun Meng, Qingyu Li, Huilin Sun, Yunhui Wang, Xing'ao Li
, Available online  , doi: 10.1016/j.gee.2024.12.009
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The pursuit of sustainable energy has driven a significant interest in hydrogen (H2) as a clean fuel alternative. A critical challenge is the efficient storage of H2, which this study addresses by examining the potential of tricycloquinazoline-based monolayer metal–organic frameworks (MMOFs with the first “M” representing metal species). Using density functional theory, we optimized the structures of MMOFs and calculated H2 adsorption energies above the open metal sites, identifying ScMOF, TiMOF, NiMOF, and MgMOF for further validation of their thermodynamic stability via ab-initio molecular dynamics (AIMD) simulations. Force field parameters were fitted via the Morse potential, providing a solid foundation for subsequent grand canonical Monte Carlo simulations. These simulations revealed that the maximum of saturated excess gravimetric H2 uptake exceeds 14.16 wt% at 77 K, surpassing other reported MOFs, whether they possess open metal sites or not. At 298 K and 100 bar, both the planar and distorted structures derived from our AIMD simulations demonstrated comparable excess gravimetric H2 uptake within the range of 3.05 wt% to 3.94 wt%, once again outperforming other MOFs. Furthermore, lithium (Li) doping significantly enhanced the excess H2 uptake, with Li-TiMOF achieving an impressive 6.83 wt% at 298 K and 100 bar, exceeding the ultimate target set by the U.S. Department of Energy. The exceptional H2 adsorption capacities of these monolayer MOFs highlight their potential in H2 storage, contributing to the design of more efficient hydrogen storage materials and propelling the sustainable hydrogen economy forward.
Techno-Economic Assessment of Plasma-driven Air Oxidation Coupled with Electroreduction Synthesis of Ammonia
Lei Xiao, Shiyong Mou, Xiaoyu Lin, Keying Wu, Siyuan Liu, Weidong Dai, Weiping Yang, Chiyao Tang, Chang Long, Fan Dong
, Available online  , doi: 10.1016/j.gee.2025.03.009
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Recently, the plasma-driven air oxidation coupled with electrocatalytic NOx reduction reaction (pAO-eNOxRR) technology for sustained NH3 synthesis displays the promise in tackling the high energy-consumption and carbon-emission associated with the Haber-Bosch process. Here, a technical and economic assessment of pAO-eNOxRR technology is comprehensively undertaken to determine its feasibility as a potential substitute for the Haber-Bosch process. The technical assessment suggests that, in terms of both environmental impact and energy efficiency, N2-NO-NH3 and N2-NO2--NH3 are presently the most effective pathways. The deep analysis of the current state-of-the-art technological performance indicates that the pAO-eNOxRR technology is competitive with commercial processes in achieving large-scale NH3 synthesis. However, lower energy efficiency of pAO-eNOxRR technology leads to the high electricity costs that surpass the current market price of NH3. Subsequently, we conducted a comprehensive analysis which reveals that, for the economic viability of NH3 synthesis, an energy efficiency in the range of 33.8-38.6% must be attained. The expenses associated with plasma equipment, electrolyzer, catalysts, and NH3 distillation also contribute significantly to the economic burden. The further development of pAO-eNOxRR technology should be centered around advancements in plasma catalysts, electrocatalysts, reactors, as well as the exploration for energy-efficient cathode-anode synergistic catalytic systems.
Regulating WOx coordination environment improves proton transfer for catalytic amine regeneration in CO2 capture
Zanbu Geng, Yang Yang, Wenqing Xu, Yixi Wang, Yiren Li, Chaoqun Li, Juan Liu, Tingyu Zhu
, Available online  , doi: 10.1016/j.gee.2024.12.002
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Catalyst-aided regeneration is a promising method for reducing the high regeneration energy consumption of amine-based CO2 capture technologies. However, the intrinsic relationship between the properties of the acidic sites and their catalytic activity is controversial. In this study, a series of W-based catalysts supported by ZrTiOx were synthesised, and the effects of the intensity, distribution, and type of acid sites were systematically investigated by quantitatively regulating the acidic site properties. The results indicate stronger acidic sites play a more important role in the catalytic reaction. Moreover, the catalysts showed excellent performance only if the Brønsted acid sites (BASs) and Lewis acid sites (LASs) coexisted. During the catalytic reaction, the BASs facilitated deprotonation, and the LASs promoted the decomposition of carbamates. The ratio of BASs to LASs (B/L) was a critical factor for catalytic activity, wherein optimal performance was achieved when the B/L ratio was close to 1. The 10% HPW/ZrTiOx composite performed better than WO3/ZrTiOx and HSiW/ZrTiOx because it had a stronger acid intensity and a suitable B/L ratio. As a result, the relative heat duty was reduced by 47% compared to 30% aqueous MEA, and the maximum CO2 desorption rate was increased by 83%. The Bader charge indicated that the W atoms of HPW/ZrTiOx lost more electrons (0.18) than those of WO3/ZrTiOx, which can weaken the O–H bond energy. Consequently, the calculated deprotonation energy is as low as 257 kJ/mol for HPW/ZrTiOx.
Ru single atoms in Mn2O3 efficiently promote the catalytic oxidation of 5-hydroxymethylfurfural through dual activation of lattice and molecular oxygen
Peiya Chen, Xinghao Li, Yuhan Liu, Huai Liu, Rui Zhang, Wenlong Jia, Junhua Zhang, Yong Sun, Lincai Peng
, Available online  , doi: 10.1016/j.gee.2025.01.001
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Concurrent activation of lattice oxygen (OL) and molecular oxygen (O2) is crucial for the efficient catalytic oxidation of biomass-derived molecules over metal oxides. Herein, we report that the introduction of ultralow-loading of Ru single atoms (0.42 wt%) into Mn2O3 matrix (0.4%Ru–Mn2O3) greatly boosts its catalytic activity for the aerobic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA). The FDCA productivity over the 0.4%Ru–Mn2O3 (5.4 mmolFDCA·gcat-1·h-1) is 4.9 times higher than the Mn2O3. Especially, this FDCA productivity is also significantly higher than that of existing Ru and Mn-based catalysts. Experimental and theoretical investigations discovered that the Ru single atom facilitated the formation of oxygen vacancy (Ov) in the catalyst, which synergistically weakened the Mn–O bond and promoted the activation of OL. The co-presence of Ru single atoms and Ov also promote the adsorption and activation of both O2 and HMF. Consequently, the dehydrogenation reaction energy barrier of the rate-determining step was reduced via both the OL and chemisorbed O2 dehydrogenation pathways, thus boosting the catalytic oxidation reactions.
Recent progress on the development of non-fluorinated proton exchange membrane-A review
Peng Song, Yi Zhang, Xue Zhang, Jiaye Liu, Liang Wu, Adrian C. Fisher, Quan-Fu An
, Available online  , doi: 10.1016/j.gee.2025.03.003
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Proton exchange membranes (PEMs) are widely employed in energy conversion and storage devices including fuel cells (FCs), redox flow batteries (RFBs) and PEM water electrolysis (PEMWE). As one of the main components of these devices, a high-performance PEM is always desirable considering the cost challenges from both energy utilization efficiency and production cost. From this century, governments of countries worldwide have introduced PFAS (per-and polyfluoroalkyl substances) restriction related policies, which facilitate the extensive research on non-fluorinated PEMs. Besides, non-fluorinated PEMs become hot topics of all kinds of PEMs due to the advantages including excellent conductivity, high mechanical property, reduced swelling, low cost and reduced ion permeation of electrochemical active species. In this review, various types of non-fluorinated PEMs including main-chain-type hydrocarbon membranes, microphase separation membranes and membranes with rigid-twisted structure are comprehensively summarized. The basic properties of different types of non-fluorinated PEMs including water uptake, swelling ratio, oxidative stability, tensile strength and conductivity are compared and the corresponding application performance in FCs, RFBs and PEMWE are discussed. The state-of-the-art of the structural design in both monomers and polymers are reviewed for the construction of fast ion transport channels and high resistance of free radical attacks. Also, future challenges and possibilities for the development of non-fluorinated PEMs are comprehensively foretasted.
Stable and high-safety fast-charging lithium metal battery enabled by a polydopamine-functionalized hydroxyapatite/aramid hybrid nanofibers separator
Long Cheng, Ying-Jie Zhu, Yaxin Zhang, Han-Ping Yu, Sida Xie, Dandan Li, Heng Li, Shiyou Zheng
, Available online  , doi: 10.1016/j.gee.2024.12.007
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Severe lithium dendrite growth and elevated thermal runaway risks pose significant hurdles for fast-charging lithium metal batteries (LMBs). This study reports a polydopamine-functionalized hydroxyapatite/aramid (PDA@HA) hybrid nanofibers separator to synchronously improve the fast-charging LMB's stability and safety. (1) The separator's surface, enriched with lithiophilic carbonyl and hydroxyl groups, accelerates Li+ ion desolvation, while electrophilic imine groups impede anion movement. This dual mechanism optimizes the Li+-ion flux distribution on the anode, mitigating dendrite formation. (2) The polar PDA modification layer fosters the development of a Li3N/LiF-rich solid electrolyte interface, further enhancing Li anode stability. Consequently, Li//Li symmetric cells with PDA@HA separators exhibit extended cycle life in Li plating/stripping tests: 5000 h at 1 mA cm-2 and 700 h at 20 mA cm-2, respectively, outperforming PP separators (80 h and 8 h). In LiFePO4 (LFP, ∼2.1 mg cm-2)//Li full cell evaluation, the PDA@HA separator enables stable operation for 11,000 cycles at 18.2C with 87% capacity retention, significantly outperforming existing fast-charging LMB counterparts in literature. At a high LFP loading of 15.5 mg cm-2, the cell maintains 137.6 mAh g-1 (2.13 mAh cm-2) over 250 cycles at 3C, achieving 98% capacity retention. Moreover, the PDA@HA separator increases threshold temperature for thermal runaway and reduces the exothermic rate, intensifying the battery's thermal safety. This research underscores the importance of functional separator design in improving Li metal anode reversibility, fast-charging performance, and thermal safety of LMBs.
Surface-enhanced light harvesting over MOF-derived porous ZnO films for highly efficient QDs-based photoelectrochemical hydrogen generation
Yi Tao, Zikun Tang, Linjie Xie, Xiaolan Xu, Wei Zhao, Wenxuan Xu, Dequan Bao, Yihong Zhong, Zhenqiu Gao, Zhen Wen, Kanghong Wang, Hao Zhang, Xuhui Sun
, Available online  , doi: 10.1016/j.gee.2024.12.005
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Rational design of porous metal oxide films that serve as not only the scaffolds for light absorbers but also the transfer layer of photogenerated charges is essential for fabricating highly efficient photoanodes for photoelectrochemical (PEC) hydrogen generation. In this work, we report a facile one-step pyrolysis method which can convert Zn-based MOF to porous ZnO (m-ZnO) with rough surface and abundant oxygen vacancies (Ov). When incorporating core-shell quantum dots (QDs) as the light absorbers, the obtained photoanodes (m-ZnO@QDs) achieved outstanding PEC performance for hydrogen generation, exhibiting 1.6 times and 5.8 times higher saturated photocurrent density (Jsc) than those of conventional TiO2@QDs and ZnO@QDs photoanodes, respectively. Comprehensive optical and electrochemical measurements reveal that the rough surface of m-ZnO can significantly improve the light-harvesting capacity of corresponding photoanodes through surface-enhanced light scattering. Moreover, the Ov in m-ZnO facilitate the interfacial transfer of photogenerated electrons. Our findings indicate that the MOFs are valuable precursors for the preparation of porous films, offering a promising route to develop high-performance QDs-based PEC devices.
Tailor of frustrated Lewis pairs in Ag/CeO2 for producing 4-aminophenol
Huaiquan Zhao, Hongye Bai, Zhenzhen Huang, Guanhua Wang, Hongliang Dai, Xuliang Pang, Hongping Li, Weiqiang Fan
, Available online  , doi: 10.1016/j.gee.2025.02.006
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Catalytic reduction of 4-nitrophenol (4-NP) pollutant to the high-value 4-aminophenol (4-AP) with a clean hydrogen donor holds significant importance yet great challenges owing to the difficult activation of nitro and H species. In this work, Ag tailoring Frustrated Lewis pairs (FLPs) of CeO2 (Ag/CeO2) were successfully fabricated for electrochemical reduction reaction of 4-NP (4-NP ERR). As a result, the bond of Ag with O atom changed the state of the Ce–O bond and electron density, where the tailored FLPs were the key factor for enhancing absorption and activation. The reaction rate of Ag/CeO2 reached up to 4.70 μmol·min-1 (Faraday efficiency: 99.5%), which was about four times of CeO2. Additionally, this study delved into the proton-coupled electron processes to further understand the mechanism of 4-NP ERR. Therefore, in this study, we have endeavored to investigate the role of tailored FLPs sites and utilize this structure–function relationship to achieve environmental-friendly chemical synthesis.
Recent progress in hydrophobic pervaporation membranes for phenol recovery
Chao Sang, Chang Liu, Yunpan Ying, Lu Lu, Chenlin Zhang, Jan Baeyens, Zhihao Si, Xinmiao Zhang, Peiyong Qin
, Available online  , doi: 10.1016/j.gee.2025.03.006
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Phenol is extensively utilized in various industries involving paints, rubber, textiles, explosives, plastics, etc. Compared to the conventional distillation or extraction technologies, pervaporation (PV) membrane process can be operated at a low temperature and has a low energy consumption as well as a high separation efficiency for phenol recovery. Thus, to meet the high demand for phenol recovery, the application of PV has been encouraged, and reached a new height. The PV process is governed by the properties of the membrane materials that significantly influence the energy costs associated with the separation unit, and the membrane types include polymer membranes, inorganic membranes, and mixed matrix membranes. Although recent literatures show that PV membranes are been continuously updated, no review reported the latest development about it. In this work, the material types, separation properties and preparation methods of hydrophobic PV membranes for phenol recovery are summarized. Furthermore, the key preparation methods and application challenges associated with membranes are summarized, along with an overview of the opportunities and challenges posed by hydrophobic PV membranes for phenol recovery.
The crucial role of intrinsic properties in determining the biological effects of CeO2 nanocrystals
Min Sun, Wanqin Dai, Yuhui Ma, Mengyao Liu, Xiao He, Zhuda Song, Yun Wang, Jiaqi Shen, Fang Yang, Zhiyong Zhang
, Available online  , doi: 10.1016/j.gee.2025.03.001
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Nano ceria (nano-CeO2) has been widely applied in various fields of industry and daily life, however, knowledge regarding the biological effects of nano-CeO2 with different intrinsic physicochemical properties remains limited. In this study, we investigated the impact of nano-CeO2 with different properties on the growth of a typical environmental species (romaine lettuce, Lactuca sativa L.) by exposing the plant to four types of CeO2 (rod-like nano-CeO2 (RNC), cubic nano-CeO2 (CNC), spherical nano-CeO2 (SNC) and commercial irregular CeO2 (CIC)) during the germination stage. The results indicated that different types of CeO2 exhibited varying inhibitory effects on plant growth. RNC and SNC significantly inhibited the elongation of roots and shoots, while CNC and CIC did not have a significant impact. We further examined the distribution and biotransformation of the four CeO2 in plant tissues using transmission electron microscopy (TEM) and synchrotron X-ray absorption near edge structure (XANES). Specifically, the positively charged RNC and SNC were more readily adsorbed onto the root surface, and needle-like nanoclusters were deposited in the intercellular space inside the roots. The absolute content of Ce(III) in the roots romaine lettuce was in the order of RNC > SNC >> CNC >> CIC. The size and shape (i.e., exposed crystal surface) of the materials affected their reactivity and dissolution ratios, and zeta potentials affected their bioavailability, both of which influenced the overall contents of Ce3+ ions in plant tissues. Thus, these characteristics together led to different biological effects. These findings highlight the importance of considering the intrinsic properties of nano-CeO2 when assessing their environmental and biological effects.
Photothermal dry reforming of methane reaction over (Ni/Ce0.8Zr0.2O2)@SiO2 catalysts: The Ni content regulation
Xiaoyan Tian, Yu Shi, Jianming Zhang, Fagen Wang
, Available online  , doi: 10.1016/j.gee.2025.02.008
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Dry reforming of methane (DRM) converts CH4 and CO2 to syngas. Photothermal DRM, which integrates temperature and light, is a sustainable method for storing solar energy in molecules. However, challenges such as limited light absorption, low photocarrier separation efficiency, Ni sintering, and carbon deposition hinder DRM stability. Herein, we regulated Ni contents in (Ni/Ce0.8Zr0.2O2)@SiO2 catalysts to enhance the optical characteristics while addressing Ni sintering and carbon deposition issues. The (3Ni/Ce0.8Zr0.2O2)@SiO2 catalyst had insufficient Ni content, while the (9Ni/Ce0.8Zr0.2O2)@SiO2 catalyst showed excessive carbon deposition, leading to lower stability compared to the (6Ni/Ce0.8Zr0.2O2)@SiO2 catalyst, which achieved CH4 and CO2 rates to 231.0 μmol/(gcat·s) and 294.3 μmol/(gcat·s), respectively, at 973 K, with only 0.2 wt.% carbon deposition and no Ni sintering. This work adjusted Ni contents in (Ni/Ce0.8Zr0.2O2)@SiO2 catalysts to enhance DRM performance, which has implications for improving other reactions.
Engineering of copper sulfide-based nanomaterials for thermoelectric application
Binqi He, Kai Zhang, Maiyong Zhu
, Available online  , doi: 10.1016/j.gee.2024.11.010
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In the context of diminishing energy resources and worsening greenhouse effect, thermoelectric materials have great potential for sustainable development due to their green and environmentally friendly characteristics. Among inorganic thermoelectric materials, copper sulfide compounds have greater potential than others due to their abundant element reserves on Earth, lower usage costs, non-toxicity, and good biocompatibility. Compared to organic thermoelectric materials, the "phonon liquid-electron crystal" (PLEC) feature of copper sulfide compounds makes them have stronger thermoelectric performance. This review summarizes the latest research progress in the synthesis methods and thermoelectric modification strategies of copper sulfide compounds. It first explains the importance of the solid-phase method in the manufacture of thermoelectric devices, and then focuses on the great potential of nanoscale synthesis technology based on liquid-phase method in the preparation of thermoelectric materials. Finally, it systematically discusses several strategies for regulating the thermoelectric performance of copper sulfide compounds, including adjusting the chemical proportion of Cu2-xS and introducing element doping to regulate the crystal structure, phase composition, chemical composition, band structure, and nanoscale microstructure of copper sulfide compounds, and directly affecting ZT value by adjusting conductivity and thermal conductivity. In addition, it discusses composite engineering based on copper sulfide compounds, including inorganic, organic, and metal compounds, and discusses tri-component compounds derived from sulfide copper. Finally, it discusses the main challenges and prospects of the development of copper sulfide-based thermoelectric materials, hoping that this review will promote the development of copper sulfide-based thermoelectric materials.
MOF membrane boosts electrocatalytic nitrogen reduction on perovskite oxides
Tan Zhang, Qi Wang, Yuhan Sun, Jinping Li, Guang Liu
, Available online  , doi: 10.1016/j.gee.2025.02.002
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The electrochemical nitrogen reduction reaction (NRR) under ambient conditions presents a promising approach for the eco-friendly and sustainable synthesis of ammonia, with a continuous emergence of potential electrocatalysts. However, the low solubility and limited diffusion of N2 significantly hinder the achievement of satisfactory performance. In this context, we report an effective strategy to enhance NRR activity by introducing a metal–organic framework (MOF) membrane, specifically MIL-53(Al), onto a perovskite oxide (LiNbO3), denoted as LN@MIL-X (X = 0.2, 0.4 and 0.6). The MIL-53(Al) membrane selectively recognizes and concentrates N2 at the catalyst interface while simultaneously repelling water molecules, thereby inhibiting the hydrogen evolution reaction (HER). This ultrathin nanostructure significantly improves the NRR performance of LN@MIL-X compared to pristine LiNbO3. Notably, LN@MIL-0.4 exhibits a maximum NH3 yield of 45.25 μg h-1 mgcat.-1 with an impressive Faradaic efficiency (FE) of 86.41% at -0.45 V versus RHE in 0.1 mol L-1 Na2SO4. This work provides a universal strategy for the design and synthesis of perovskite oxide electrocatalysts, facilitating high-efficiency ammonia synthesis.
MOFs-based porous liquids for CO2 capture and utilization
Xun Wang, Yuxi Liu, Hongxing Dai, Zhen Wei, Shaohua Xie, Jiguang Deng
, Available online  , doi: 10.1016/j.gee.2025.01.002
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Due to the greenhouse effect caused by carbon dioxide (CO2) emission, much attention has been paid for the removal of CO2. Porous liquids (PLs), as new type of liquid materials, have obvious advantages in mass and heat transfer, which are widely used in gas adsorption and separation. Metal–organic frameworks (MOFs) with the merit like large surface area, inherent porous structure and adjustable topology have been considered as one of the best candidates for PLs construction. This review presents the state-of-the-art status on the fabrication strategy of MOFs-based PLs and their CO2 absorption and utilization performance, and the positive effects of porosity and functional modification on the absorption-desorption property, selectivity of target product, and regeneration ability are well summarized. Finally, the challenges and prospects for MOFs-based PLs in the optimization of preparation, the coupling of multiple removal techniques, the in situ characterization methods, the regeneration and cycle stability, the environmental impact as well as expansion of application are proposed.
Hydrothermal liquefaction for preparation of liquid fuels and chemicals: Solvent effects, catalysts regulation and thermochemical conversion processes
Bingbing Qiu, Xuedong Tao, Yanfang Wang, Donghui Zhang, Huaqiang Chu
, Available online  , doi: 10.1016/j.gee.2024.11.009
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Hydrothermal liquefaction technology is an effective method for the resource utilization and energy conversion of biomass under the dual-carbon context, facilitating the conversion of biomass into liquid fuels and high-value chemicals. This paper reviews the latest advancements in the production of liquid fuels and chemicals from biomass hydrothermal liquefaction. It briefly introduces the effects of different types of biomass, such as organic waste, lignocellulosic materials, and algae, on the conversion efficiency and product yield during hydrothermal liquefaction. The specific mechanisms of solvent and catalyst systems in the hydrothermal liquefaction process are analyzed in detail. Compared to water and organic solvents, the biphasic solvent system yields higher concentrations of furan platform compounds, and the addition of an appropriate amount of NaCl to the solvent significantly enhances product yield. Homogeneous catalysts exhibit advantages in reaction rate and selectivity but are limited by high costs and difficulties in separation and recovery. In contrast, heterogeneous catalysts possess good separability and regeneration capabilities and can operate under high-temperature conditions, but their mass transfer efficiency and deactivation issues may affect catalytic performance. The direct hydrothermal catalytic conversion of biomass is also discussed for the efficient production of chemicals and fuels such as hexanol, ethylene glycol, lactic acid, and C5/C6 liquid alkanes. Finally, the advantages and current challenges of producing liquid fuels and chemicals from biomass hydrothermal liquefaction are thoroughly analyzed, along with potential future research directions.
Heteroatom-Functionalized Carbon Nanoarchitectonics: Unlocking the Doping Effects for High-Performance Supercapacitor Electrode Design
Pragati A. Shinde, Lok Kumar Shrestha, Katsuhiko Ariga
, Available online  , doi: 10.1016/j.gee.2025.02.007
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This review focuses on the significant impact of heteroatom doping in enhancing the electronic properties and electrochemical performance of carbon materials for supercapacitors (SCs). Incorporating heteroatoms such as nitrogen, sulfur, phosphorus, fluorine, and boron modifies the carbon structure, creating defects and increasing active sites, which improves electronic conductivity, ion accessibility, and surface wettability and reduces ion diffusion barriers. Additionally, certain heteroatoms can participate in electrochemical reactions, further enhancing SC performance. Although research in this area is still emerging, a deeper understanding of the mechanisms behind single and multi-doping systems is essential for developing next-generation materials. Future strategies for improving heteroatom-doped carbon materials include increasing heteroatom content to enhance specific capacitance, selecting suitable heteroatoms to expand the potential window and improve energy density, utilizing advanced in situ characterization techniques, and exploring the use of these materials in cost-effective SCs. The future potential of heteroatom-doped carbon materials for SCs is promising, with their ability to improve energy density, power density, and cycling stability, making them competitive with other energy storage technologies. These advancements will be key to broadening their practical applications, including electric vehicles, portable electronics, and grid energy storage, and will contribute to more efficient, long-lasting, and environmentally friendly energy storage solutions.
Heavy Metal Challenge in NH3-SCR DeNOx Catalysts: Poisoning Deactivation Mechanisms and Enhanced Resistance Strategies
Yu Xia, Fengyu Gao, Jiajun Wen, Tingkai Xiong, Honghong Yi, Qingjun Yu, Shunzheng Zhao, Yuansong Zhou, Xiaolong Tang
, Available online  , doi: 10.1016/j.gee.2024.11.007
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Ammonia selective catalytic reduction (NH3-SCR) is the most widely used technology in the field of industrial flue gas denitrification. However, the presence of heavy metals in flue gas can seriously affect the performance of SCR catalysts, leading to their deactivation or even failure. Therefore, it is of great significance to deeply study the poisoning mechanism of SCR catalysts under the action of heavy metals and how to enhance their resistance to poisoning. This article reviews the reaction mechanism of NH3-SCR technology, compares the impact of heavy metals on the activity of different SCR catalysts, and then discusses in detail the poisoning mechanism of SCR catalysts by heavy metals, including pore blockage, reduction of specific surface area, and destruction of active centers caused by heavy metal deposition, all of which jointly lead to the physical or chemical poisoning of the catalyst. Meanwhile, the mechanism of action when multiple toxicants coexist was analyzed. To effectively address these challenges, the article further summarizes various methods to improve the catalyst's resistance to heavy metal poisoning, such as element doping, structural optimization, and carrier addition, which significantly enhance the heavy metal resistance of the catalyst. Finally, the article provides a prospective analysis of the challenges faced by NH3-SCR catalysts in anti-heavy metal poisoning technology, emphasizing the necessity of in-depth research on the poisoning mechanism, exploration of the mechanism of synergistic action of multiple pollutants, development of comprehensive anti-poisoning strategies, and research on catalyst regeneration technology, in order to promote the development of efficient anti-heavy metal poisoning NH3-SCR catalysts.
Oxidation Mechanism and Performance Control of Manganese-Based Catalysts in Soot Oxidation
Tingyi Zhao, Yuanjun Li, Chengchun Wu, Wen Cao, Jiahao Gong, Menglan Xiao, Zuguo Song, Zhihui Shao, Mingqin Zhao, Bing Cui
, Available online  , doi: 10.1016/j.gee.2024.12.004
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The extensive use of diesel engines has led to significant emissions of pollutants, especially soot particles, which pose serious risks to both the environment and human health. At present, developing catalysts with low-temperature activity, low cost, and high stability remains the core challenge in eliminating soot from diesel engine exhaust. This paper first reviews the mechanisms of soot catalytic oxidation. Based on these mechanisms, the current design directions for soot catalysts are summarized and discussed. On the one hand, the effects of modification methods such as doping, loading, and solid solution on the performance of manganese-based catalysts are reviewed from the perspective of intrinsic activity. On the other hand, the research progress on manganese-based catalysts with specific morphological structures for soot oxidation is explored. Following the identification of design strategies, the commonly used preparation methods to achieve these designs are also outlined. Finally, the paper highlights the challenges associated with manganese-based catalysts in soot catalysis and discusses future research and development directions.
Cooperative α-C–H activation enabled quantitative and partial photooxidation of biomass-derived 5-hydroxymethylfurfural
Jie Li, Ye Meng, Yu Wen, Yinyin He, Putla Sudarsanam, Song Yang, Hu Li
, Available online  , doi: 10.1016/j.gee.2024.11.004
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Photocatalytic activation of C-H bonds is versatile but challenging for undergoing oriented conversion processes. Herein, a spatially site-isolated heterojunction (ZS-Vs/ZIS) of ZnIn2S4 with strong Lewis acidity (ZIS) and ZnS with S-vacancy (ZS-Vs) is constructed for activating α-C-H bond and forming ·O2- to cleave the C-H bond, respectively. ZS-Vs/ZIS displays outstanding performance in visible-light partial photooxidation of bio-based 5-hydroxymethylfurfural (HMF) to 2,5-diformylfuran (DFF) in an unprecedented yield of 95.7% at 25 ºC. In-situ experiments and calculations reveal that Zn sites of ZIS serve as hole enrichment to adsorb HMF for α-C-H activation via ligand-to-metal charge transfer. Shallow trap states introduced by S-vacancy in ZS-Vs act as an electron pool to realize directed O2 activation into ·O2- for breaking pre-activated α-C-H bond in HMF to exclusively give DFF. Moreover, ZS-Vs/ZIS has good recyclability and universality in the photooxidation of various alcohols to carbonyls (86.4-95.6% yields). The synergistic C-H activation/breaking strategy exhibits high potential in targeted photocatalytic transformations.
Enhanced degradation of ciprofloxacin via Co-doped Bi2Fe4O9 photocatalysis under peroxydisulfate activation
Zizhen Wu, Jiawei Liu, Li Zhen, Jun Shi, Huiping Deng
, Available online  , doi: 10.1016/j.gee.2024.12.008
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The synergistic degradation of contaminants in water by photocatalysis and peroxydisulfate (PDS) activation has been proven to be a promising combined advanced oxidation technology. Consequently, the development of highly efficient photocatalysts that are activated by visible light and PDS is of immense importance. Herein, different proportions of cobalt-doped Bi2Fe4O9 (BFO@Co-x) photocatalysts were effectively synthesized for elimination of ciprofloxacin (CIP). The degradation efficiency of CIP achieved by the BFO@Co/Vis/PDS system attained 84.49% (k = 0.0516 min-1) under 40 min light irradiation, outperforming the BFO@Co/Vis and PDS/Vis systems by a factor of 1.45 and 3.6, respectively. Characterization and photoelectric performance assessments revealed that the fabrication of BFO@Co-0.5 was successful, enhancing the photocatalytic degradation efficiency under the synergistic effect of PDS. Moreover, the BFO@Co/Vis/PDS system demonstrated favorable adaptability to various pH, inorganic anions, and humic acid in solution. Additionally, the degradation pathways of CIP and the toxicity of products were evaluated using LC/MS and T.E.S.T software, indicating a reduction in the toxicity of CIP degradation products. This study may provide insights into the application of photocatalyst/Vis/PDS combined systems in the field of water environmental treatment.
In situ converting the native passivation layer into a fast ion transport interphase to boost the stability of zinc anodes
Zi-Long Xie, Yunhai Zhu, Jia-Yi Du, Dong-Yue Yang, Hao Chen, Zhi Wang, Gang Huang, Xin-Bo Zhang
, Available online  , doi: 10.1016/j.gee.2025.02.004
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Aqueous zinc batteries offer significant potential for large-scale energy storage, wearable devices, and medium-to low-speed transportation due to their safety, affordability, and environmental friendliness. However, the uneven zinc deposition at the anode side caused by localized reaction activity from the passivation layer presents challenges that significantly impact the battery's stability and lifespan. In this study, we have proposed an expandable and maneuverable gel sustained-release (GSR) treatment to polish the Zn metal, which in situ converts its native passivation layer into a composite interphase layer with nanocrystal zinc phosphate and flexible polyvinyl alcohol. Such a thin and uniform interface contributes to fast and homogeneous Zn ion transport and improved anti-corrosion ability, enabling uniform zinc deposition without dendrite growth and thereby improving the battery performance with high-rate ability and long cycle life. This GSR treatment method, characterized by its simplicity, low cost, and universality, facilitates the widespread application of aqueous zinc batteries.
Progress and prospect of transition metal compound cathode materials with stable metal ion storage effect in various battery systems
Dongfang Guo, Bin Zhang
, Available online  , doi: 10.1016/j.gee.2025.02.001
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The field of energy storage devices is primarily dominated by lithium-ion batteries (LIBs) due to their mature manufacturing processes and stable performance. However, immature lithium recovery technology cannot stop the continuous increase in the cost of LIBs. Along with the rapid development of electric transportation, it has become inevitable to trigger a new round of competition in alternative energy storage systems. Some monovalent rechargeable metal ion batteries (sodium ion batteries (SIBs) and potassium ion batteries (PIBs), etc.) and multivalent rechargeable metal-ion batteries (magnesium ion batteries (MIBs), calcium ion batteries (CIBs), zinc ion batteries (ZIBs), and aluminum ion batteries (AIBs), etc.) are potential candidates, which can replace LIBs in some of the scenarios to alleviate the pressure on supply. The cathode material plays a crucial role in determining the battery capacity. Transition metal compounds dominated by layered transition metal oxides as key cathode materials for secondary batteries play an important role in the advancement of various battery energy storage systems. In summary, this manuscript aims to review and summarize the research progress on transition metal compounds used as cathodes in different metal ion batteries, with the aim of providing valuable guidance for the exploration and design of high-performance integrated battery systems.
Recent advances in cellulose-based separators for zinc-based batteries: performances, mechanism and perspectives
Zekun Zhang, Yongjun Li, Xuejing Yin, Siwen Li, Bin Li, Ningning Zhao, Jing Zhu, Lei Dai, Ling Wang, Zhangxing He, Zemin Feng
, Available online  , doi: 10.1016/j.gee.2025.03.010
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Zinc-based batteries have attracted widespread attention due to their inherent safety, notable cost-effectiveness and consistent performance, etc. However, the advancement of zinc-based battery technology encounters significant challenges, including the formation of zinc dendrites and irreversible side reactions. Separators are vital in batteries due to its role in preventing electrode contact and facilitating rapid movement of ions within the electrolyte. The incorporation of cellulose in battery enables uniform ion transport and a stable electric field, attributed to its excellent hydrophilicity, strong mechanical strength, and abundant active sites. Herein, the latest research progress of cellulose-based separators on various zinc-based batteries is systematically summarized. To begin with, the accomplishments and inherent limitations of traditional separators are clarified. Next, it underscores the advantages of cellulose-based materials in battery technology, thoroughly examining their utilization and merits as separators in zinc-based batteries. Lastly, the review offers prospective insights into the future trajectory of cellulose-based separators in zinc-based batteries. Through a comprehensive analysis of the present landscape, the review establishes a framework for the future design and enhancement of cellulose-based separators, thereby fostering the progression of associated industries.
Multicomponent high-entropy assisted high-rate and air-stable layered cathode for sodium ion batteries
Renyi Ma, Jiaqi Wang, Guohua Zhu, Yongguang Liu, Ling Wang, Xiaoyan Zhang, Linzhe Wang, Lei Dai, Shan Liu
, Available online  , doi: 10.1016/j.gee.2025.03.008
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Sodium-based O3-type layered oxide materials are attractive for Sodium-ion batteries (SIBs) due to their simple synthesis, affordability, and high capacity. However, challenges remain, including limited reversible capacity and poor cycling stability caused by detrimental phase transitions during cycling and the tendency to form sodium carbonate upon air exposure. In this study, based on O3-type NaNi1/3Fe1/3Mn1/3O2 (NNFM), a high-entropy strategy was introduced to successfully synthesize O3-type NaNi0.25Fe0.21Mn0.18Co0.21Ti0.1Mg0.05O2 (HE-NNFM). The introduction of Co, Ti, and Mg ions increases the system's disorder, highlighting the synergistic interactions among inert atoms. The delayed phase transformation effect in high-entropy materials alleviates the destruction of the O3 structure by the insertion and extraction of sodium ions. Simultaneously, the narrower sodium layer in HE-NNFM acts as a physical barrier, effectively preventing adverse reactions with H2O and CO2 in the air, resulting in excellent reversibility and air stability of the HE-NNFM material. Consequently, the HE-NNFM material exhibits a reversible capacity of 110 mAh g-1 with a capacity retention of 97.3% after 200 cycles at 1 C. This work provides insights into the design of high-entropy sodium layered oxides for high-power density storage systems.
Environmentally benign process for valorization of lignocellulosic bamboo residues with green solvent propylene carbonate
Jie Liang, Jingcong Xie, Jianchun Jiang, Yan Ma, Jun Ye, Xianhai Zeng, Kui Wang
, Available online  , doi: 10.1016/j.gee.2025.03.002
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A novel environmentally benign biphasic system composed of propylene carbonate (PC) and aqueous solution of p-toluenesulfonic acid (p-TsOH aq) was designed for the efficient valorization of lignocellulosic bamboo residues, resulting in more than 95.5% of hemicellulose and 97.2% of lignin digested under mild conditions of 130 °C for 1 h. Meanwhile, 91.9% of cellulose was retained with loose structure, followed by 95.8% enzyme hydrolysis yield and 347.9 mg/g of glucose yield. Notably, the synergistic effect between PC and p-TsOH on efficiency and selectivity was proposed by a control group experiment and subsequently verified, which is believed to be responsible for the simultaneous degradation and separation of lignin and hemicelluloses into oligomeric phenols and pentose, also facilitating subsequent valorization. Furthermore, the novel PC/p-TsOH aq biphasic system demonstrated excellent retrievability and adaptability to different feedstocks, offering a promising green strategy for the efficient valorization of lignocellulosic biomass in industrial biorefineries.
Limiting cationic mixing and lattice oxygen loss of single-crystalline Ni-rich Co-poor cathodes for high-voltage Li-ion batteries
Hujun Zhang, Haifeng Yu, Ling Chen, Muslum Demir, Qilin Cheng, Hao Jiang
, Available online  , doi: 10.1016/j.gee.2025.03.004
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Developing cost-effective single-crystalline Ni-rich Co-poor cathodes operating at high-voltage is one of the most important ways to achieve higher energy Li-ion batteries. However, the Li/O loss and Li/Ni mixing under high-temperature lithiation result in electrochemical kinetic hysteresis and structural instability. Herein, we report a highly-ordered single-crystalline LiNi0.85Co0.05Mn0.10O2 (NCM85) cathode by doping K+ and F- ions. To be specific, the K-ion as a fluxing agent can remarkably decrease the solid-state lithiation temperature by ∼30 °C, leading to less Li/Ni mixing and oxygen vacancy. Meanwhile, the strong transitional metal (TM)-F bonds are helpful for enhancing de-/lithiation kinetics and limiting the lattice oxygen escape even at 4.5 V high-voltage. Their advantages synergistically endow the single-crystalline NCM85 cathode with a very high reversible capacity of 222.3 mAh g-1. A superior capacity retention of 91.3% is obtained after 500 times at 1 C in pouch-type full cells, and a prediction value of 75.3% is given after cycling for 5000 h. These findings are reckoned to expedite the exploitation and application of high-voltage single-crystalline Ni-rich cathodes for next-generation Li-ion batteries.
Enhanced and selective photocatalytic reduction of CO2 to CH4 using a Pt-loaded CuPc/g-C3N4 Z-scheme heterojunction catalyst
Jinshan Chen, Jiangfeng Lu, Ran Lang, Chi Wang, Shuangyou Bao, Yuan Li, Kai Li, Maohong Fan
, Available online  , doi: 10.1016/j.gee.2025.01.006
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In this study, a novel Pt-loaded CuPc/g-C3N4 (PtCuCN) composite was synthesized for the selective photocatalytic reduction of CO2 to CH4 under visible light. The PtCuCN catalyst achieved a CH4 yield of 39.8 μmol g-1 h-1, significantly outperforming bulk g–C3N4 and CuPc alone by factors of 2.5 and 3.1, respectively, with a high selectivity of 90%. In comparison with other commonly studied photocatalysts, such as g–C3N4–based catalysts, the PtCuCN composite exhibited superior CH4 yield and product selectivity, demonstrating its potential as a more efficient photocatalyst for CO2 reduction. X-ray photoelectron spectroscopy (XPS), density functional theory (DFT) calculations, and in-situ infrared (IR) analysis revealed that the Pt0 species effectively lower the activation energy for CH4 formation, while CuPc extends the light absorption range and enhances charge separation. The combined effects of these components in a Z-scheme heterojunction provide new insights into designing highly selective CO2-to-CH4 photocatalysts. This work demonstrates the potential of PtCuCN as a highly efficient and stable catalyst for CO2 reduction to CH4 under visible light.
Enhanced CO2 Methanation through Electronic Modification of Ru to Ni in Ni-Al Hydrotalcite-derived Catalysts
Junming Zeng, Yongbin Yao, Fang Wang, Jiajian Gao, Lili Zhang, Guangwen Xu, Ziyi Zhong, Fabing Su
, Available online  , doi: 10.1016/j.gee.2024.12.006
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Nickle-based catalysts are commonly used for CO2 methanation. However, there is still potential to improve their catalytic performance under mild conditions. In this study, we synthesized a series of Ru-Ni-Al catalysts from Ru-doped NiAl-hydrotalcite using a hydrothermal method. The Ru-Ni-Al catalyst demonstrated much higher activity for CO2 methanation than the Ni-Al catalyst that did not have Ru doping. Both experimental results and theoretical calculations indicate that the enhanced performance of the Ru-Ni-Al catalyst is related to electronic interactions between nickel (Ni) and ruthenium (Ru). The Ru sites transfer electrons to the Ni sites, increasing the local electron density of Ni, which enhances the adsorption and activation of H2. Furthermore, the Ru-Ni metal interface sites improve the adsorption and activation of CO2. In situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) analysis indicates that adjusting the electronic structure of Ni sites can accelerate the production of intermediates HCOO*, while Ru-Ni intermetallic interface sites can directly dissociate CO2 into CO*. In addition, CO2 methanation on the Ru-Ni-Al catalyst follows HCOO*- and CO*-mediated pathways. This study underscores the potential for enhancing CO2 methanation performance by modulating the electronic structure of Ni sites.
Eco-friendly synthesis coupled with predictive analytics: developing hierarchical lignin-derived ordered mesoporous carbon for advanced supercapacitors
Xiaolan Zhao, Xiaoqi Wang, Pei Gao, Peng Zhao, Jingjing Wang, Yingna Li, Zhibin Han, Boxiong Shen
, Available online  , doi: 10.1016/j.gee.2024.11.006
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Hierarchical lignin-derived ordered mesoporous carbon (HOMC) was significant for advanced supercapacitors. However, achieving controllable fabrication and optimizing electrochemical behavior were challenging. In this work, an eco-friendly HOMC was synthesized using lignin as carbon precursors and Zn2+ as cross-linking and pore-forming agents, followed by KHCO3 activation, eliminating the need for toxic phenolic resins and acid treatments for metal removal. Machine learning technology, specifically an Artificial Neural Network (ANN) model, was utilized to assist the experimental design and prediction. The ANN model suggested an ideal hierarchical structure and optimized oxygen level, achieved through the adjustment of Zn2+ additive concentration, carbonization temperature, and subsequent KHCO3 activation to maximize capacitance. The HOMC electrode, with a micropore-to-mesopore ratio (Smicro/Smeso) of 1.01 and an oxygen content of 8.81 at%, acquired a specific capacitance of 362 F·g-1 at 0.5 A·g-1 in 6 mol·L-1 KOH electrolyte. The assembled HOMC//HOMC supercapacitor could afford a high energy density of 33.38 Wh·kg-1 with a corresponding specific power density of 300 W·kg-1 in TEATFB/PC electrolyte. Meanwhile, the long-term cycle stability of 94.33% was achieved after 20,000 cycles. This work provides an ANN-assisted strategy for the synthesis of HOMC, highlighting its potential to valorize biomass and agricultural waste in sustainable energy storage solutions.
Highly efficient photoelectrocatalytic degradation for ciprofloxacin with a new polyoxometalate-based metal–organic hybrid/BiVO4 photoanode
Yuting Song, Tao Bo, Ji-Cheng Ma, Jian-Fang Ma
, Available online  , doi: 10.1016/j.gee.2025.01.007
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Efficient removal of antibiotics is of great significance for the sustainability of aquatic ecosystems. In this work, a new polyoxometalate-based metal–organic hybrid material [Ag3L0.5(HSiW12O40)]·2C2H5OH·2CH3CN ( Ag-L-SiW 12) was prepared by using Keggin-type polyoxometalate anion and thiacalix[4]arene-based ligand (L) via solvothermal method. Subsequently, a composite heterojunction Ag-L-SiW 12@BiVO4 photoanode was fabricated by loading Ag-L-SiW 12 on the surface of BiVO4. The photoelectrocatalytic degradation performance of ciprofloxacin (CIP) was explored under the simulated solar radiation. Remarkably, the CIP degradation efficiency reached 93% within 240 min using the optimal Ag-L-SiW @BiVO4 photoanode, which is approximately 2 and 23 times those of pristine BiVO4 and Ag-L-SiW 12, respectively. Furthermore, density functional theory (DFT) calculations were conducted to elucidate the role of Ag-L-SiW 12 during the photoelectrocatalytic process. This work offers an example of the efficient composite photoelectrocatalysts for the treatment of antibiotic wastewater.
Boosting charge transfer of BiOBr/AgBr S-scheme heterojunctions via interface Br atom co-sharing for enhanced visible-light photocatalytic activity
Junhao Ma, Liang Xu, Zhaoyi Yin, Zhifeng Li, Zhiguo Song, Jianbei Qiu, Yongjin Li
, Available online  , doi: 10.1016/j.gee.2024.11.003
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Efficient interfacial charge transfer and robust interfacial interactions are crucial for achieving the superior spatial separation of carriers and developing efficient heterojunction photocatalysts. Herein, BiOBr/AgBr S-scheme heterojunctions are synthesized via the co-sharing of Br atoms using an ion-exchange approach, which involves the in-situ growth of AgBr nanoparticles on the surfaces of BiOBr nanosheets. It is revealed that successful construction of a high-quality interface with strong interactions via Br atom bridge between BiOBr and AgBr, which provided a rapid migration channel for charge carriers. In addition, in-situ XPS, Kelvin probe force microscopy, and electron spin resonance evaluations confirmed the establishment of an S-scheme charge-transfer pathway in this tightly contacted heterojunction, which could efficiently prevent the recombination of photogenerated carriers while retaining carriers with a high redox capacity. Finally, the photocatalytic test confirmed that the BiOBr/AgBr heterojunction showed excellent photocatalytic performance and wide applicability thanks to the construction of high quality heterojunction. Overall, this work highlights the importance of rational design of heterogeneous interfaces at the atomic level in photocatalysis, and contributes to rationally design BiOBr-based S-scheme heterojunctions photocatalytic materials with high quality atomic co-sharing interfaces.
Construction of imidazole-based ionic liquid modified MoO3-x for enhancing photocatalytic oxidation desulfurization in diesel
Suhang Xun, Chenchao Hu, Bohan Yang, Wei Jiang, Minqiang He, Wenshuai Zhu, Huaming Li
, Available online  , doi: 10.1016/j.gee.2025.02.005
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Development of clean desulfurization process that combines both efficient and environmentally friendly remains a significant challenge for diesel production. The photocatalytic oxidation desulfurization technology is regarded as a promising process depending on the superior electron transfer and visible light utilization of photocatalyst. Herein, the nonstoichiometry MoO3-x with outstanding photoresponse ability is prepared and modified by imidazole-based ionic liquid [C12mim]Cl to upgrade electronic structure. The interface H-bonding between MoO3-x and [C12mim]Cl regard as electronic transfer channel and the recombination of e--h+ pairs is effectively inhibited with the modification of [C12mim]Cl. Deep desulfurization rate of 96.6 % can be reached within 60 min and the MoO3-x/[C12mim]Cl (MoC12) photocatalyst demonstrated outstanding cyclic stability within 7 cycles in an extraction coupled photocatalytic oxidation desulfurization (ECPODS) system. The study provides a new perspective on enhancing photocatalytic desulfurization through defect engineering and surface modification.
A practical milling route for highly dispersed and tunably loaded Pt in NiFe hydroxides as bifunctional water-splitting electrocatalysts
Jinyang Wang, Peiyan Feng, Chenxiao Yang, Jiahao Yao, Zhe Deng, Menggai Jiao, Lili Zhang, Wei Ma, Zhen Zhou
, Available online  , doi: 10.1016/j.gee.2024.12.001
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Noble metal-loaded layered hydroxides exhibit high efficiency in electrocatalyzing water splitting. However, their widespread use as bifunctional electrocatalysts is hindered by low metal loading, inefficient yield, and complex synthesis processes. In this work, platinum atoms were anchored onto nickel-iron layered double hydroxide/carbon nanotube (LDH/CNT) hybrid electrocatalysts by using a straightforward milling technique with K2PtCl6·6H2O as the Pt source. By adjusting the Pt-to-Fe ratio to 1/3 and 1/10, excellent electrocatalysts—Pt1/6-Ni2/3Fe1/3-LDH/CNT and Pt1/30-Ni2/3Fe1/3-LDH/CNT—were achieved with superior performance in hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), outperforming the corresponding commercial Pt/C (20 wt%) and RuO2 electrocatalysts. The enhanced electrochemical performance is attributed to the modification of Pt's electronic structure, which exhibits electron-rich states for HER and electron-deficient states for OER, significantly boosting Pt's electrochemical activity. Furthermore, the simple milling technology for controlling Pt loading offers a promising approach for scaling up the production of electrocatalysts.
Advances in Cu-based catalysts for electroreduction of CO2 to C2H4 in flow cells
Yunxia Zhao, Yunxin Dai, Yunfei Bu
, Available online  , doi: 10.1016/j.gee.2025.01.003
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Global investment in ethylene (C2H4) production via nonpetroleum pathways is rising, highlighting its growing importance in the energy and environmental sectors. The electroreduction of carbon dioxide (CO2) to C2H4 in flow cells is emerging as a promising technology with broad practical applications. Direct delivery of gaseous CO2 to the cathode catalyst layer overcomes mass transfer limitations, enhancing reaction rates and enabling high current density. This review summarizes recent research progress in the electrocatalytic CO2 reduction reaction (eCO2RR) for selective C2H4 production in flow cells. It outlines the principles of eCO2RR to C2H4 and discusses the influence of copper-based catalyst morphology, crystal facet, oxidation state, surface modification strategy, and synergistic effects on catalytic performance. In addition, it highlights the compositional structure of the flow cell, and the selection and optimization of operating conditions, including gas diffusion electrodes, electrolytes, ion exchange membranes, and alternative anode reaction types beyond the oxygen evolution reaction. Finally, advances in machine learning are presented for accelerating catalyst screening and predicting dynamic changes in catalysts during reduction. This comprehensive review serves as a valuable reference for the development of efficient catalysts and the construction of electrolytic devices for the electrocatalytic reduction of CO2 to C2H4.
Advanced microwave synthesis strategies for innovative photocatalyst design
Shunda Li, Hao Ma, Ping Ouyang, Yuhan Li, Youyu Duan, Yunqiao Zhou, Wee-Jun Ong, Fan Dong
, Available online  , doi: 10.1016/j.gee.2024.11.005
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Amidst environmental pollution and the energy crisis, photocatalytic technology has emerged as a potent tool for promoting clean energy and environmental preservation. However, the promotion and widespread adoption of photocatalysis encounter the formidable challenge of synthesizing high-quality photocatalysts in a cost-effective and expedited manner. Thus, we have compiled an analysis elucidating the efficacy and heating mechanisms of microwaves, validating their superiority as a heat source. Furthermore, this review presents a comprehensive overview of microwave-assisted synthesis techniques for photocatalysts, marking the inaugural attempt to do so, and extensively discusses the merits of diverse microwave-based preparation methodologies. Moreover, we systematically examine approaches for modifying photocatalysts using microwave-assisted methods, providing insights into their pivotal role in photocatalyst enhancement. We aspire that this review will serve as a seminal reference, facilitating the judicious application of microwave-assisted synthesis techniques for the controlled and efficient production of photocatalysts, thereby advancing the dissemination and adoption of photocatalysis.
Carbon nitride quantum dots decorated with cyano groups for boosting photocatalytic hydrogen peroxide production
Ke Kong, Hong Zhong, Dejian Chen, Fushuai Zhang, Xiaoju Li, Ruihu Wang
, Available online  , doi: 10.1016/j.gee.2025.01.004
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The photocatalytic hydrogen peroxide (H2O2) production by graphitic carbon nitride is a sustainable and environment-benign alternative approach of conventional anthraquinone autoxidation technology, but it is great challenges to promote two-electron O2 reduction and water oxidation. Herein, we present the well-dispersed graphitic carbon nitride quantum dots decorated with cyano groups (Na-CNQD and K-CNQD) by thermal polymerization of melamine in the presence of metal fluoride. The quantum confinement and edge effect have endowed the photocatalysts with rich active sites, wide light absorption range and the inhibited charge recombination. The cyano moieties function as O2 reduction centers to accept the photogenerated electrons and facilitate their rapid transfer to O2 molecules. This process enables the selective two-electron reduction of O2, leading to the production of H2O2. Concurrently, the valence band holes on the heptazine moiety oxidize water into H2O2. These synergistic effects promote photocatalytic H2O2 production from O2 and H2O without the need for additional photosensitizers, organic scavengers and co-catalysts. In contrast, pristine carbon nitride nanosheets remain inactive under the same conditions. This study offers new strategies for rational design of carbon-based materials for solar-to-chemical energy conversion.
Biomass-derived single atom catalysts with phosphorus-coordinated Fe-N3P configuration for efficient oxygen reduction reaction
Peng-Peng Guo, Abrar Qadir, Chao Xu, Kun-Zu Yang, Yong-Zhi Su, Xin Liu, Ping-Jie Wei, Qinggang He, Jin-Gang Liu
, Available online  , doi: 10.1016/j.gee.2024.11.002
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Exploiting non-precious metal catalysts with excellent oxygen reduction reaction (ORR) performance for energy devices is paramount essential for the green and sustainable society development. Herein, low-cost, high-performance biomass-derived ORR catalysts with an asymmetric Fe-N3P configuration was prepared by a simple pyrolysis-etching technique, where carboxymethyl cellulose (CMC) was used as the carbon source, urea and 1,10-phenanthroline iron complex (FePhen) as additives, and Na3PO4 as the phosphorus dopant and a pore-forming agent. The CMC-derived FeNPC catalyst displayed a large specific area (BET:1235 m2 g-1) with atomically dispersed Fe-N3P active sites, which exhibited superior ORR activity and stability in alkaline solution (E1/2 = 0.90 V vs. RHE) and Zn-air batteries (Pmax = 149 mW cm-2) to commercial Pt/C catalyst (E1/2 = 0.87 V, Pmax = 118 mW cm-2) under similar experimental conditions. This work provides a feasible and cost-effective route toward highly efficient ORR catalysts and their application to Zn-air batteries for energy conversion.
Activation of persulfate using a biochar polyacrylic acid composite loaded with nanoscale zero-valent iron for the in situ remediation of anthracene-contaminated soil
Fengjun Li, Dongyun Chen, Shihong Dong, Najun Li, Qingfeng Xu, Hua Li, Jianmei Lu
, Available online  , doi: 10.1016/j.gee.2025.03.007
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Synthesizing highly efficient, low toxicity catalysts for the remediation of polycyclic aromatic hydrocarbons (PAHs) contaminated soils is crucial. Nanoscale zero-valent iron (n-ZVI) is widely used in the treatment of pollutants due to its high catalytic activity. However, n-ZVI is prone to aggregation and passivation. Therefore, to design an environmentally friendly, efficient, and practical catalyst material, this study designed a nanoscale zero-valent iron-loaded biochar (BC) polyacrylic acid (PAA) composite materials. Biochar and polyacrylic acid can prevent the aggregation of zero-valent iron and provide a large number of functional groups. The iron on the carrier is uniformly distributed, exposing active sites and activating persulfate to remove anthracene (ANT) pollutants from the soil. The BC/PAA/Fe0 system can achieve an anthracene degradation efficiency of 93.7% in soil, and the degradation efficiency of anthracene remains around 90% under both acidic and alkaline conditions. Free radical capture experiments indicate that the degradation of anthracene proceeds through the radical pathways SO4·-, ·OH, O2·- and the non-radical pathway 1O2. In addition, possible degradation pathways for anthracene have been proposed. Plant planting experiments have shown that the catalyst designed in this study has low toxicity and has excellent application prospects in the field of soil remediation.
Ambient temperature catalyzed air-oxidation of 5-hydroxymethylfurfural via ternary metal and oxygen vacancies
Yunlei Zhang, Yiran Liu, Qinghua Xia, Yao Chen, Lingzhao Kong, Xingchen Yan, Wen Guan, Jianming Pan
, Available online  , doi: 10.1016/j.gee.2025.02.003
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Catalytic oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA, an alternative bioplastic monomer to petroleum-derived terephthalic acid), has been identified as an important biomass conversion reaction in bio-based polyester industry. However, it is still challenging to acquire a high FDCA yield from the selective oxidation of HMF at low temperatures. Herein, a ternary metal-based catalyst was prepared by loading AuPdPt noble metal nanoparticles on the oxygen-rich vacancy titanium dioxide layer deposited on natural clay mineral kaolin nanotubes (HNTs), and the catalytic activity was examined for air-oxidation of HMF to FDCA in water at ambient temperature (30 °C). By adjusting the Au/Pd/Pt ratio, a 93.6% FDCA yield was achieved with the optimal Au0.5Pd0.2Pt0.3/TiO2@HNTs catalyst, which revealed an impressive FDCA formation rate of 67.58 mmol g-1 h-1 and an excellent TOF value of 17.54 h-1 under normal air pressure at 30 °C, surpassing the performance of mono- and bimetallic-based catalysts. Theoretical calculation and catalytic performance study clarified the structure–activity relationship. It was found that the ternary metal and oxygen vacancies revealing synergistic enhancement of ambient temperature catalyzed HMF air-oxidation via electronic structure tuning and adsorption intensification. DFT and kinetics study demonstrated that the presence of ternary metal significantly improved the adsorption capacity of substrate and enhanced the rate-determining step of the key intermediate 5-hydroxymethyl-2-furanocarboxylic acid (HMFCA) oxidation when compared to mono- and bimetal. Additionally, the TiO2@HNTs support with high oxygen vacancy concentration facilitated the adsorption of oxygen, synergistically working with the ternary metal to activate and low the energy barriers for the generation of superoxide radical, thus enhancing the FDCA formation. This work offers a novel strategy for designing ternary metal-based catalysts for low-energy catalytic oxidation reactions.
Constructing multiple sites porous organic polymers for highly efficient and reversible adsorption of triiodide ion from water
Zhiyong Li, Yibo Fu, Yilong Li, Ruipeng Li, Yuanchao Pei, Yunlei Shi, Huiyong Wang
, Available online  , doi: 10.1016/j.gee.2025.03.005
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The utilization of nuclear power will persist as a prominent energy source in the foreseeable future. However, it presents substantial challenges concerning waste disposal and the potential emission of untreated radioactive substances, such as radioactive 129I and 131I. The transportation of radioactive iodine poses a significant threat to both the environment and human health. Nevertheless, effectively, rapidly removing iodine ion from water using porous adsorbents remains a crucial challenge. In this work, three kinds of multiple sites porous organic polymers (POPs, POP-1, POP-2, and POP-3) have been developed using a monomer pre-modification strategy for highly efficient and fast I3- absorption from water. It is found that the POPs exhibited exceptional performance in terms of I3- adsorption, achieving a top-performing adsorption capacity of 5.25 g·g-1 and the fastest average adsorption rate (K80% = 4.25 g·g-1·h-1) with POP-1. Moreover, POP-1 exhibited exceptional capacity for the removal of I3- from flowing aqueous solutions, with 95% removal efficiency observed even at 0.0005 mol·L-1. Such results indicate that this material has the potential to be utilized for the emergency preparation of potable water in areas contaminated with radioactive iodine. The adsorption process can be effectively characterized by the Freundlich model and the pseudo-second-order model. The exceptional I3- absorption capacity is primarily attributed to the incorporation of a substantial number of active adsorption sites, including bromine, carbonyl, and amide groups.
Interfacial regulation for zinc metal anode of aqueous zinc-ion battery
Jing Zhu, Xumeng Ge, Zhi Peng, Liang Pan, Ziyu Peng, Yingqiao Jiang, Wei Meng, Zekun Zhang, Ningning Zhao, Bin Li, Lei Dai, Ling Wang, Zhangxing He
, Available online  , doi: 10.1016/j.gee.2024.11.001
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Aqueous zinc-ion batteries (AZIBs) have attracted significant attention due to their high energy density, low cost, high efficiency, and environmental friendliness. Nevertheless, the development of AZIBs has been significantly hindered by the unavoidable issues with zinc dendrites and the side reactions of the anode. The strategies for stable and controllable interfacial regulation have recently made rapid progress, due to their dual function of improving zinc ion transport dynamics and preventing direct contact of zinc with electrolytes. Therefore, it’s imperative to conduct a comprehensive summary of the interfacial regulation of zinc anodes and to engage in in-depth research into the underlying mechanisms. Subsequently, the interfacial regulation was classified based on battery structure, including anode coating strategy, electrolyte engineering, and separator optimization. Eventually, the current limitations of interfacial regulation and a deep outlook on AZIBs interface engineering are summarized.
Valorization of spent lithium-ion battery cathode materials for energy conversion reactions
Jin Zhang, Ding Chen, Jixiang Jiao, Weihao Zeng, Shichun Mu
, Available online  , doi: 10.1016/j.gee.2024.10.006
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With large-scale commercial applications of lithium-ion batteries (LIBs), lots of spent LIBs will be produced and cause huge waste of resources and greatly increased environmental problems. Thus, recycling spent LIB materials is inevitable. Due to high added-value features, converting spent LIB cathode materials into catalysts exhibits broad application prospects. Inspired by this, we review the high-added-value reutilization of spent LIB materials toward catalysts of energy conversion. First, the failure mechanism of spent LIB cathode materials are discussed, and then the transformation and modification strategies are summarized and analyzed to improve the transformation efficiency of failed cathode materials and the catalytic performance of catalysts, respectively. Moreover, the electrochemical applications of failed cathode material derived catalysts are introduced, and the key problems and countermeasures are analyzed and proposed. Finally, the future development trend and prospect of high-added-value reutilization for spent LIB cathode materials toward catalysts are also given. This review will predictably advance the awareness of valorizing spent lithium-ion battery cathode materials for catalysis.
Dual-bonded Polyethyleneimine Network with Electron-withdrawing Groups at α, β-sites for Ultra-stable and Low-energy CO2 Capture in Harsh Environments
Tong Zhou, Yunxia Wen, Zhinan Wu, Shuailong Song, Bohong Wu, Hongwei Guo, Huanhao Chen, Xin Feng, Liwen Mu, Xiaohua Lu, Tuo Ji, Jiahua Zhu
, Available online  , doi: 10.1016/j.gee.2024.10.005.
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As an innovative approach to addressing climate change, significant efforts have been dedicated to the development of amine sorbents for CO2 capture. However, the high energy requirements and limited lifespan of these sorbents, such as oxidative and water stability, pose significant challenges to their widespread commercial adoption. Moreover, the understanding of the relationship between adsorption energy and adsorption sites is not known. In this work, a dual-bond strategy was used to create novel secondary amine structures by a polyethyleneimine (PEI) network with electron-extracted (EE) amine sites at adjacent sites, thereby weakening the CO2 binding energy while maintaining the binding ability. In-situ FT-IR and DFT demonstrated the oxygen-containing functional groups adjacent to the amino group withdraw electrons from the N atom, thereby reducing the CO2 adsorption capacity of the secondary amine, resulting in lower regeneration energy consumption of 1.39 GJ·t-1-CO2. In addition, the EE sorbents demonstrated remarkable performance with retention of over 90% of their working capacity after 100 cycles, even under harsh conditions containing 10% O2 and 20% H2O. DFT calculations were employed to clarify for the first time the mechanism that the oxygen functional group at the α-site hinders the formation of the urea structure, thereby being an antioxidant. These findings highlight the promising potential of such sorbents for deployment in various CO2 emission scenarios, irrespective of environmental conditions.
Heterointerface of Nickel-ferric Hydroxide/Cobalt-phosphide-boride Boosting Hydrazine-assisted Water Electrolysis
Jiayi Wang, Shaojun Qing, Xili Tong, Ting Xiang, Guangnan Luo, Kun Zhang, Liangji Xu
, Available online  , doi: 10.1016/j.gee.2024.10.003
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Sustainable H2 production based on hydrogen evolution reaction (HER) and hydrazine oxidation reaction (HzOR) has attracted wide attention due to minimal energy consumption compared to overall water electrolysis. The present study focuses on the design and construction of heterostructured CoPB@NiFe-OH applied as efficient bifunctional catalysts to sustainable produce hydrogen and remove hydrazine in alkaline media. Impressively, CoPB@NiFe-OH heterointerface exhibits an HzOR potential of -135 mV at the current density of 10 mA cm-2 when the P to B atom ratio was 0.2, simultaneously an HER potential of -32 mV toward HER when the atom ratio of P and B was 0.5. Thus, hydrogen production without an outer voltage accompanied by a small current density output of 25 mA cm-2 is achieved, surpassing most reported catalysts. In addition, DFT calculations demonstrate the Co sites in CoPB upgrades H* adsorption, while the Ni sites in NiFe-OH optimizes the adsorption energy of N2H4* due to electron transfer from CoPB to NiFeOH at the heterointerface, ultimately leading to exceptional wonderful performance in hydrazine-assistant water electrolysis via HER coupled with HzOR.
Eco-friendly and facile nanomanufacturing of amorphous Co-Ce-Fe trimetallic molybdates composites for accelerated anodic oxygen evolution in alkaline water electrolysis: Evaluation of active sites performance
Jiejie Feng, Liling Wei, Huayi Li, Jianquan Shen
, Available online  , doi: 10.1016/j.gee.2024.09.012
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Currently, endeavors to scale up the production of amorphous catalysts are still impeded by intricate synthesis conditions. Here, we have prepared a series of metal-based molybdate via one-step coprecipitation method. After ingredient optimization, amorphous Co2CeFe2-MoO4 was identified as exhibiting the highest intrinsic activity among its counterparts. Modulation of electron structure enables Co2CeFe2-MoO4 to balance the adsorption behavior towards reactive intermediates. Ultimately, the obtained Co2CeFe2-MoO4 molybdate demonstrated a captivating OER performance, showcasing a low overpotential of 230 mV at 10 mA cm-2. Moreover, the alkaline electrolyzer employing the Co2CeFe2-MoO4 anode exhibited a low cell voltage of 1.50 V for water splitting and underwent an acceptable attenuation of 4.99% after 165 hours of continuous operation, demonstrating its favorable catalytic activity and durability. This work provides a facile and eco-friendly synthesis pathway for crafting cost-effective and durable earth-abundant OER electrocatalysts tailored for water splitting to produce clean hydrogen.
Coupling adsorption and in-situ Fenton-like oxidation by iron-containing low-grade attapulgite clay towards organic pollutant removal: From batch experiment to continuous operation
Chao Jiang, Xiaoli Liu, Xingpeng Wang, Qihui Wang, Huiyu Li, Weiliang Tian, Saeed Ahmed, Yongjun Feng
, Available online  , doi: 10.1016/j.gee.2024.10.004
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Coupling adsorption and in-situ Fenton-like oxidation process was developed for Methylene blue (MB) using refined iron-containing low-grade attapulgite (ATP) clay, and the removal mechanism was investigated. The MB was initially adsorbed on the porous ATPs, and then the enriched MB was removed by the H2O2-assisted Fenton-like oxidation with the iron-containing ATP catalyst. Under optimal conditions, the ATP powder exhibits the maximum removal efficiency of 100% with negligible iron leaching (1.5 mg L-1) and no sludge formation. Furthermore, polysulfone/ATP (PSF/ATP) pellets were fabricated through a water-induced phase separation process to construct a fixed-bed reactor (FBR) for continuous contaminant removal. For the first cycle, the maximum adsorption capacity was 15.5 L with an outlet MB concentration of 1.973 mg L-1 (< 2 mg L-1, GB4287-2012) using the PSF/ATP pellets containing 50.0 g of ATP powders, and the maximum Fenton-like oxidation capacity was 35.5 L with the outlet concentration of 0.831 mg L-1. After five cycles, the total treated volume of the MB solution was ca. 255 L, and the efficiency remained above 99%. After 10 hours of continuous treatment towards practical resin industrial wastewater, the chemical oxygen demand (COD) removal efficiency was still measured at 83.05%, costing 0.398 $ m-3. These results demonstrate the practical applicability of iron-containing low-grade ATP clay for textile water treatment.
Solvent-free Synthesis of Highly Dispersed Zinc-doped Porous Carbons as Efficient Dibenzothiophene Adsorbents
Ping Lu, Zhenhua Sun, Xinrong Ke, Changshen Ye, Zhixian Huang, Ting Qiu
, Available online  , doi: 10.1016/j.gee.2024.09.010
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Designing efficient adsorbents for the deep removal of refractory dibenzothiophene (DBT) from fuel oil is vital for addressing environmental issues such as acid rain. Herein, zinc gluconate and urea-derived porous carbons SF-ZnNC-T (T represents the carbonization temperature) were synthesized without solvents. Through a temperature-controlled process of “melting the zinc gluconate and urea mixture, forming H-bonded polymers, and carbonizing the polymers,” the optimal carbon, SF-ZnNC-900, was obtained with a large surface area (2280 m2/g), highly dispersed Zn sites, and hierarchical pore structures. Consequently, SF-ZnNC-900 demonstrated significantly higher DBT adsorption capacity of 43.2 mg S/g, compared to just 4.3 mg S/g for the precursor. It also demonstrated good reusability, a fast adsorption rate, and the ability for ultra-deep desulfurization. The superior DBT adsorption performance resulted from the evaporation of residual zinc species, which generated abundant mesopores that facilitated DBT transformation, as well as the formation of Zn-N sites that strengthened the host-guest interaction (ΔE = -1.466 eV). The solvent-free synthesized highly dispersed Zn-doped carbon shows great potential for producing sulfur-free fuel oil and for designing metal-loaded carbon adsorbents.
Fe-O-Bi efficient electron transfer channels and photo-Fenton synergy in S-scheme heterojunctions: insights into interfacial interactions and ofloxacin degradation
Jiawei Liu, Jun Shi, Huiping Deng
, Available online  , doi: 10.1016/j.gee.2024.09.008
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Fenton method combined with light to accelerate the production of free radicals from H2O2 can achieve more efficient pollutant degradation. In this paper, a novel BiOI/FeWO4 S-scheme heterojunction photocatalyst was obtained by in situ synthesis, which can activate H2O2 and degrade the organic pollutant OFC (ofloxacin) under visible light. The S-scheme charge transfer mechanism was confirmed by XPS spectroscopy, in situ KPFM and theoretical calculation. The photogenerated electrons were transferred from FeWO4 to BiOI driven by the built-in electric field and band bending, which inhibited carrier recombination and facilitated the activation of H2O2.The BiFe-5/Vis/H2O2 system degraded OFC up to 96.4% in 60 min. This study provides new systematic insights into the activation of H2O2 by S-scheme heterojunctions, which is of great significance for the treatment of antibiotic wastewater.
Lamellar COF Solid-state Electrolytes for Robust Ambient-temperature Lithium-ion transfer enhanced by PEI-driven Channel Alignment
Yafang Zhang, Xinji Zhang, Jiajia Huang, Zhirong Yang, Shiyue Zhou, Chenye Wang, Wenjia Wu, Jingtao Wang
, Available online  , doi: 10.1016/j.gee.2024.09.009
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Ionic covalent organic framework (COF) lamellar membranes are the alternative materials as promising Li+ conductors for all-solid-state lithium batteries. However, COF lamellar membrane suffers from poor structural stability and inevitable cross-layer transfer resistance due to the weak interaction at interface of adjacent nanosheets. Herein, a lamellar polymer-threaded ionic COF (PEI@TpPa-SO3Li) composite electrolyte with single Li+ conduction was prepared by assembling lithium sulfonated COF (TpPa-SO3Li) nanosheets and then threading them with polyethyleneimine (PEI) chains. It reveals that the threaded PEI chains induce the oriented permutation of pore channel of PEI@TpPa-SO3Li electrolyte through electrostatic interaction between -NH2/-NH- and -SO3Li groups. This enables the construction of continuous and aligned -SO3-...Li+...-NH2/-NH- pairs along pore channels, which act as efficient Li+ conducting sites and afford high Li+ hopping conduction (1.4×10-4 S cm-1 at 30 ℃) with a high Young's modulus of 408.7 MP and wide electrochemical stability window of 0~4.7 V. The assembled LiFePO4Li and LiNi0.8Mn0.1Co0.1O2Li half-cells achieve high discharge capacities of 155.0 mAh g-1 and 167.2 mAh g-1 at 30 ℃ under 0.2 C, respectively, with high capacity retention of 98% after 300 cycles. This study provides an alternative route to highly ion-conductive lamellar porous electrolytes for high-performance energy devices.
Study on the effect of controlled disproportionation pore-forming and relative vacuum mechanism on the reduction rate of continuous magnesium smelting process
Jing-zhong Xu, Ting-an Zhang, Yan Liu, Zhihe Dou, Yishan Liu, Baiao Feng, Hongxuan Liu
, Available online  , doi: 10.1016/j.gee.2024.09.006
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Compared with the vacuum continuous magnesium smelting process (RVCMS), its excellent energy saving and emission reduction performance provides a feasible method for green magnesium smelting. In the process of industrialization, the reduction rate of prefabricated pellets affects the yield of metal magnesium and the utilization of reducing slag. In this paper, the reduction mechanism under different carbonate structures is analyzed by controlled disproportionation of prefabricated pellets and micro-nano simulation. The results show that the low temperature decomposition of NH4·HCO3 pore-forming, improve the reduction rate (99.72 %) effect is remarkable. Combined with thermodynamics and relative vacuum mechanism, a theoretical model of the relationship between disproportionation pore-forming and reduction rate was established. It was concluded that the energy consumption required to produce per ton of magnesium by adding NH4·HCO3 to the prefabricated pellets was reduced by 0.29 ~ 0.34 tce, and the carbon emission was reduced by 1.069 ~ 1.263 t. The reduction slag had good compressive strength (Side 101.19 N/cm2, Bottom 466.4 N/cm2). Compared with the 20 MPa reduction slag sample without pore-forming agent, the side compressive strength increased by 51.66 %, and the bottom compressive strength increased by 119.10 %. The amount of single furnace filler is increased by more than 50 %.
Recent progress in carbon-based composite materials for advanced sodium ion batteries: from storage mechanism to structural design to applications as flexible electrodes
Ao Song, Yunchao Li, Dingkun Yuan, Jie Wu, Hailin Gu, Guangxue Zhang, Angjian Wu, Jiangrong Xu
, Available online  , doi: 10.1016/j.gee.2024.09.007
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Sodium ion batteries (SIBs) are one of the most prospective energy storage devices recently. Carbon materials have been commonly used as anode materials for SIBs because of their wide sources and low price. However, pure carbon materials still have the disadvantage of low theoretical capacity. New design and preparation strategies for carbon-based composites can overcome the problems. Based on the analysis of Na+ storage mechanism of carbon-based composite materials, the factors influencing the performance of SIBs are discussed. Adjustment methods for improving the electrochemical performance of electrodes are evaluated in detail, including carbon skeleton design and composite material selection. Some advanced composite materials, i.e., carbon-conversion composite and carbon-MXene composite, are also being explored. New advances in flexible electrodes based on carbon-based composite on flexible SIBs is investigated. The existing issues and future issues of carbon-based composite materials are discussed.
Cyclic Ethers-Based Solid Electrolyte Derived from In Situ Ring-Opening Polymerization Strategy
Wubin Du, Yong Wu, Hao Cheng, Ran Bu, Kang Shen, Yuanzhong Tan, Zhijun Wu, Hongge Pan, Yifan Wang, Yingying Lu
, Available online  , doi: 10.1016/j.gee.2024.09.005
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Although solid-state polymer electrolytes (SPEs) are expected to solve the safety hazards and limited energy density in the energy storage systems, they still encounter an inferior electrode/electrolyte interface when prepared via an ex situ manner. Recently, in situ polymerization of SPEs favors high interfacial infiltrability, improved interface contact, and reduced interface resistance, owing to the formation of a "super-conformal" interface between electrode and electrolyte. Especially, in situ strategies employing ring-opening polymerization (ROP) are emerging as a dazzling star, further enabling moderate polymerization conditions, controllable molecular structure, and reduced interfacial side reaction. As the main monomers which can be in situ polymerized via ROP strategy, cyclic ethers have been used to construct the CE-SPEs with many merits including good battery electrochemical performances and simple assembly process. Here, as a systematic summarization to the existing reports, this review focuses the polymerization mechanism of ROP, the design principles of CE-SPEs electrolytes, and recent application of in situ CE-SPEs. In particular, this review thoroughly discusses the selection of different cyclic monomers, initiators and various modification approaches in in situ fabricating CE-SPEs. Ending with offering the future challenges and perspectives, this review envisions shedding light on the profound understanding and scientific guidance for further development of high-performance in situ CE-SPEs.
Recent progress on photothermal nanomaterials: Design, mechanism, and applications
Xiao Yu, Shilin Fan, Bin Zhu, Soliman I. El-Hout, Jian Zhang, Chunlin Chen
, Available online  , doi: 10.1016/j.gee.2024.09.002
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Photothermal energy conversion represents a cornerstone process in the renewable energy technologies domain, enabling the capture of solar irradiance and its subsequent transformation into thermal energy. This mechanism is paramount across many applications, facilitating the exploitation of solar energy for different purposes. The photothermal conversion efficiency and applications are fundamentally contingent upon the characteristics and performance of the materials employed. Consequently, deploying high-caliber materials is essential for optimizing energy capture and utilization. Within this context, photothermal nanomaterials have emerged as pivotal components in various applications, ranging from catalysis and sterilization to medical therapy, desalination, and electric power generation via the photothermal conversion effect.
This review endeavors to encapsulate the current research landscape, delineating both the developmental trajectories and application horizons of photothermal conversion materials. It aims to furnish a detailed exposition of the mechanisms underlying photothermal conversion across various materials, shedding light on the principles guiding the design of photothermal nanomaterials. Furthermore, addressing the prevailing challenges and outlooks within the field elucidates potential avenues for future research and identifying priority areas. This review aspires to enrich the understanding of photothermal materials within the framework of energy conversion, offering novel insights and fostering a more profound comprehension of their role and potential in harnessing solar energy.
Sustainable Aviation Fuels from Biomass and Biowaste via Bio- and Chemo-Catalytic Conversion: Catalysis, Process Challenges, and Opportunities
Junyan Zhang, Matthew S. Webber, Yunqiao Pu, Zhenglong Li, Xianzhi Meng, Michael L. Stone, Bingqing Wei, Xueqi Wang, Sainan Yuan, Bruno Klein, Bhogeswararao Seemala, Charles E. Wyman, Karthikeyan K. Ramasamy, Mike Thorson, Matthew H. Langholtz, Joshua S. Heyne, Aibolat Koishybay, Shiba Adhikari, Sufeng Cao, Andrew Sutton, Gerald A. Tuskan, Yuriy Román-Leshkov, Arthur J. Ragauskas, Tao Ling, Brian H. Davison
, Available online  , doi: 10.1016/j.gee.2024.09.003
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Sustainable aviation fuel (SAF) production from biomass and biowaste streams is an attractive option for decarbonizing the aviation sector, one of the most-difficult-to-electrify transportation sectors. Despite ongoing commercialization efforts using ASTM-certified pathways (e.g., lipid conversion, Fischer-Tropsch synthesis), production capacities are still inadequate due to limited feedstock supply and high production costs. New conversion technologies that utilize lignocellulosic feedstocks are needed to meet these challenges and satisfy the rapidly growing market. Combining bio- and chemo-catalytic approaches can leverage advantages from both methods, i.e., high product selectivity via biological conversion, and the capability to build C-C chains more efficiently via chemical catalysis. Herein, conversion routes, catalysis, and processes for such pathways are discussed, while key challenges and meaningful R&D opportunities are identified to guide future research activities in the space. Bio- and chemo-catalytic conversion primarily utilize the carbohydrate fraction of lignocellulose, leaving lignin as a waste product. This makes lignin conversion to SAF critical in order to utilize whole biomass, thereby lowering overall production costs while maximizing carbon efficiencies. Thus, lignin valorization strategies are also reviewed herein with vital research areas identified, such as facile lignin depolymerization approaches, highly integrated conversion systems, novel process configurations, and catalysts for the selective cleavage of aryl C–O bonds. The potential efficiency improvements available via integrated conversion steps, such as combined biological and chemo-catalytic routes, along with the use of different parallel pathways, are identified as key to producing all components of a cost-effective, 100% SAF.
Recent advances on the electrocatalytic oxidation of biomass-derived aldehydes
Zhikeng Zheng, Ke Li, Lu Lin, Zhiwei Jiang, Yuchen Wang, Kai Yan
, Available online  , doi: 10.1016/j.gee.2024.09.004
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The escalating demand for sustainable and environmentally benign chemical processes has driven the exploration of biomass as an alternative to non-renewable resources. Electrocatalytic upgrading of biomass-derived aldehydes plays a crucial role in biomass refining, and has become a frontier of mainstream research. This paper reviews the recent advances on the electrocatalytic oxidation of typical biomass-derived aldehydes (5-hydroxymethylfurfural, furfural, glucose, xylose, vanillin and benzaldehyde, etc.). The research presented in this review covers a wide range of oxidation mechanisms for each aldehyde. It is evident from the current literature that challenges related to the comprehensiveness of mechanistic studies, catalyst stability, and reaction scalability remain, but the rapid progress offers hope for future advancements. Finally, we elucidate the challenges in this domain and provide the perspectives on future developments. This review corroborates the significance of investigating the electrocatalytic oxidation of biomass-derived aldehydes and emphasizes the need for continued research to refine these processes for industrial applications.
Construction of two-dimensional heterojunctions based on metal-free semiconductor materials and Covalent Organic Frameworks for exceptional solar energy catalysis
Haijun Hu, Daming Feng, Kailai Zhang, Hui Li, Hongge Pan, Hongwei Huang, Xiaodong Sun, Tianyi Ma
, Available online  , doi: 10.1016/j.gee.2024.09.001
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Covalent organic frameworks (COFs) are newly developed crystalline substances that are garnering growing interest because of their ultra-high porosity, crystalline nature, and easy modified architecture, showing promise in the field of photocatalysis. However, it is difficult for pure COFs materials to achieve excellent photocatalytic hydrogen production due to their severe carrier recombination problems. To mitigate this crucial issue, establishing heterojunction is deemed an effective approach. Nonetheless, many of the metal-containing materials that have been used to construct heterojunctions with COFs own a number of drawbacks, including small specific surface area and rare active sites (for inorganic semiconductor materials), wider bandgaps and higher preparation costs (for MOFs). Therefore, it is necessary to choose metal-free materials that are easy to prepare. Red phosphorus (RP), as a semiconductor material without metal components, with suitable bandgap, moderate redox potential, relatively minimal toxicity, is affordable and readily available. Herein, a range of RP/TpPa-1-COF (RP/TP1C) composites have been successfully prepared through solvothermal method. The two-dimensional structure of the two materials causes strong interactions between the materials, and the construction of heterojunctions effectively inhibits the recombination of photogenic charge carrier. As a consequence, the 9% RP/TP1C composite, with the optimal photocatalytic ability, achieves a photocatalytic H2 evolution rate of 6.93 mmol·g-1·h-1, demonstrating a 10.19-fold increase compared to that of bare RP and a 4.08-fold improvement over that of pure TP1C. This article offers a novel and innovative method for the advancement of efficient COFs-based photocatalysts.
Recent advancements in two-dimensional transition metal dichalcogenide materials towards hydrogen-evolution electrocatalysis
Jianmin Yua, Gongao Peng, Lishan Peng, Qingjun Chen, Chenliang Su, Lu Shang, Tierui Zhang
, Available online  , doi: 10.1016/j.gee.2024.08.009
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Hydrogen evolution reaction (HER) plays a crucial role in developing clean and renewable hydrogen energy technologies. However, conventional HER catalysts rely on expensive and scarce noble metals, which is a significant challenge for practical application. Recently, twodimensional transition metal dichalcogenides (2D-TMDs) have emerged as attractive and costeffective alternatives for efficient electrocatalysis in the HER. Substantial efforts have been dedicated to advancing the synthesis and application of 2D-TMDs. This review highlights the design and synthesis of high-performance 2D-TMDs-based HER electrocatalysts by combining theoretical calculations with experimental methods. Subsequently, recent advances in synthesizing different types of 2D TMDs with enhanced HER activity are summarized. Finally, the conclusion and perspectives of the 2D TMDs-based HER electrocatalysts are discussed. We expect that this review will provide new insights into the design and development of highly efficient 2D TMDs-based HER electrocatalysts for industrial applications.
Research on the application of defect engineering in the field of environmental catalysis
Sirui Gao, Shunzheng Zhao, Xiaolong Tang, Long Sun, Qiyu Li, Honghong Yi
, Available online  , doi: 10.1016/j.gee.2024.08.008
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Researchers have recently developed various surface engineering approaches to modify environmental catalysts and improve their catalytic activity. Defect engineering has proved to be one of the most promising modification methods. Constructing defects on the surface of catalytic materials can effectively modulate the coordination environment of the active sites, affecting and changing the electrons, geometry, and other important properties at the catalytic active sites, thus altering the catalytic activity of the catalysts. However, the conformational relationship between defects and catalytic activity remains to be clarified. This dissertation focuses on an overview of recent advances in defect engineering in environmental catalysis. Based on defining the classification of defects in catalytic materials, defect construction methods, and characterization techniques are summarized and discussed. Focusing on an overview of the characteristics of the role of defects in electrocatalytic, photocatalytic, and thermal catalytic reactions and the mechanism of catalytic reactions. An elaborate link is given between the reaction activity and the structure of catalyst defects. Finally, the existing challenges and possible future directions for the application of defect engineering in environmental catalysis are discussed, which are expected to guide the design and development of efficient environmental catalysts and mechanism studies.
Challenges and strategies for production of diesel-like hydrocarbons by deoxygenation of biomass-derived fatty acids
Hongju Lin, Xiyan Chen, Yanchang Chu, Jie Fu, Le Yang
, Available online  , doi: 10.1016/j.gee.2024.08.005
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The valorization of biomass to produce biofuels has become a heavily investigated field due to the depletion of fossil fuels and environmental concerns. Among them, the research on deoxygenation of fatty acids or esters derived from biomass as well as municipal sludge organics to produce diesel-like hydrocarbons has become a hot topic. Fatty acid is a key intermediate derived from ester hydrolysis, therefore has attracted more attention as a model compound. In this review, we first introduce and compare the three reaction pathways of hydrodeoxygenation, decarboxylation and decarbonylation, for the deoxygenation of fatty acids and esters. The preference of reaction pathway is closely related to the type of raw materials and catalysts as well as reaction conditions. The special purpose of this review is to summarize the dilemma and possible strategies for deoxygenation of fatty acids, which is expected to provide guidance for future exploration and concentrates. The atom utilization along with stability during reaction in a long time is the most important index for commercial economy. Herein, we propose that the rational design and delicate synthesis of stable single-atom non-noble catalysts may be the best solution. The ultimately goal is aiming to develop sustainable production of green diesel hydrocarbons.
Ti3C2 MXene nanosheets integrated cobalt-doped nickel hydroxide heterostructured composite: An efficient electrocatalyst for overall water-splitting
Amaranadha Reddy Manchuri, Kamakshaiah Charyulu Devarayapalli, Bolam Kim, Youngsu Lim, Dae Sung Lee
, Available online  , doi: 10.1016/j.gee.2024.08.006
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Developing an efficient electrocatalyst for superior electrochemical water splitting (EWS) is crucial for achieving comprehensive hydrogen production. A heterostructured electrocatalyst, free of noble metals, Ti3C2 MXene nanosheet-integrated cobalt-doped nickel hydroxide (NHCoMX) composite was synthesized via a hydrothermal method. The abundant pores in the Ti3C2 MXene nanosheet (MX)-integrated microarchitecture increased the number of active sites and facilitated charge transfer, thus enhancing electrocatalysis. Specifically, the MX- enhanced charge transfer considerably transformed the microelectronic structure of cobalt-doped Ni(OH)2 (NHCo), which promoted its hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Hence, as an EWS catalyst, NHCoMX exhibited an exceptional electrocatalytic activity, demonstrating OER and HER overpotentials of 310 mV and 73 mV, respectively, with low Tafel slopes of 65 mV dec-1 and 85 mV dec-1, respectively; it exhibited a current density of 10 mV cm-2 in 1.0 mol L-1 KOH, representing the closest efficiency to the noble state-of-the-art RuO2 and Pt/C catalyst. Furthermore, the developed electrocatalyst improved the activities of both HER and OER, leading to an overall EWS current density of 10 mA cm-2 at 1.72 V in an alkaline electrolyte with two electrodes. This study describes an efficient heterostructured NHCoMX composite electrocatalyst. It is significantly comparable to the noble state-of-the-art electrocatalysts and can be extended to fabricate resourceful catalysts for large-scale EWS applications.
2,6-Diaminoanthraquinone modified MXene (Ti3C2Tx)/graphene as the negative electrode materials for ionic liquid-based asymmetric supercapacitors
Li Sun, Lujia Chai, Liangqi Jing, Yujuan Chen, Kelei Zhuo, Jianji Wang
, Available online  , doi: 10.1016/j.gee.2024.08.004
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Due to insufficient energy density, supercapacitors (SCs) with preeminent-power and long cycle stability cannot be implemented in some practical applications. Exploring hybrid materials with redox activity to emerge high specific capacitance in ionic liquid (IL) electrolytes can solve this problem. Herein, we report a redox-organic molecule 2,6-diaminoanthraquinone (DAAQ) modified MXene (2,6-Diaminoanthraquinone modified MXene (Ti3C2Tx)/graphene as the negative electrode materials for ionic liquid-based asymmetric supercapacitors)/Graphene (DAAQ-M/G) composite material. With the assist of graphene oxide (GO), MXene and graphene fabricate a three-dimensional (3D) interconnected structure as a conductive framework, which inhibits self-stacking of MXene monolayers and ensures high electronic conductivity. Meanwhile, DAAQ is loaded onto the M/G framework through covalent/non-covalent functionalization. The DAAQ as a spacer effectively enlarges the interlayer spacing of MXene nanosheets, and meanwhile produces reversible redox reactions during charge/discharge processes to provide additional Faradaic contribution to capacity. Therefore, the specific capacitance (capacity) of the DAAQ-M/G as the negative electrode material reaches to 226 F g-1 (306 C g-1) at 1 A g-1 in 1-ethyl-3-methylimidazolium tetrafluoroborate (EmimBF4) electrolyte. Furthermore, an asymmetric supercapacitor (ASC) is assembled using DAAQ-M/G as the negative electrode and self-prepared organic molecule hydroquinone modified reduced graphene oxide (HQ- RGO) material as the positive electrode, with a high energy density of 43 Wh kg-1 at high power density of 1669 W kg-1. The ASC can maintain 80% of initial specific capacitance after 9000 cycles. This research can provide better support to develop advanced organic molecules-modified MXene composite materials for ionic liquid-based SCs.
Mechano-driven chemical reactions
Shaoxin Li, Jiajin Liu, Zhong Lin Wang, Di Wei
, Available online  , doi: 10.1016/j.gee.2024.08.001
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Traditional chemical processes often generate substantial waste, leading to significant pollution of water, air, and soil. Developing eco-friendly chemical methods is crucial for economic and environmental sustainability. Mechano-driven chemistry, with its potential for material recyclability and minimal byproducts, is well-aligned with green chemistry principles. Despite its origins over 2000 years ago and nearly 200 years of scientific investigation, mechano-driven chemistry has not been widely implemented in practice. This is likely due to a lack of comprehensive understanding and the complex physical effects of mechanical forces, which challenge reaction efficiency and scalability. This review summarizes the historical development of mechano-driven chemistry and discusses its progress across various physical mechanisms, including mechanochemistry, tribochemistry, piezochemistry, and contact electrification (CE) chemistry. CE-induced chemical reactions, involving ion transfer, electron transfer, and radical generation, are detailed, emphasizing the dominant role of radicals initiated by electron transfer and the influence of ion transfer through electrical double layer (EDL) formation. Advancing efficient, eco-friendly, and controllable green chemical technologies can reduce reliance on traditional energy sources (such as electricity and heat) and toxic chemical reagents, fostering innovation in material synthesis, catalytic technologies, and establishing a new paradigm for broader chemical applications.
Superhydrophobic Ceramic Membrane Coupled with a Biphasic Solvent for Efficient CO2 Capture
Kaili Xue, Zhen Chen, Xiaona Wu, Heng Zhang, Haiping Chen, Junhua Li
, Available online  , doi: 10.1016/j.gee.2024.07.010
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An innovative strategy was proposed by integration of membrane contactor (MC) with biphasic solvent for efficient CO2 capture from flue gas. The accessible fly ashbased ceramic membrane (CM) underwent hydrophobic modification through silane grafting, followed by fluoroalkylsilane decoration, to prepare the superhydrophobic membrane (CSCM). The CSCM significantly improved resistance to wetting by the biphasic solvent, consisting of amine (DETA) and sulfolane (TMS). Morphological characterizations and chemical analysis revealed the notable enhancements in pore structure and hydrophobic chemical groups for the modified membrane. Predictions of wetting/bubbling behavior based on static wetting theory referred the liquid entry pressure (LEP) of CSCM increased by 20 kPa compared to pristine CM. Compared with traditional amine solvents, the biphasic solvent presented the expected phase separation. Performance experiments demonstrated that the CO2 capture efficiency of the biphasic solvent increased by 7%, and the electrical energy required for desorption decreased by 32%. The 60-h continuous testing and supplemental characterization of used membrane confirmed the excellent adaptability and durability of the CSCMs. This study provides a potential approach for accessing hydrophobic ceramic membranes and biphasic solvents for industrial CO2 capture.
Electronic structure modulation of high entropy materials for advanced electrocatalysis
Luoluo Qi, Jingqi Guan
, Available online  , doi: 10.1016/j.gee.2024.07.009
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High-entropy materials (HEMs) have managed to make their mark in the field of electrocatalysis. The flexibly adjustable component, unique configuration and proprietary core effect endow HEMs with excellent functional feature, superior stability and fast reaction kinetics. Recently, the relationship between the compositions and structures of high-entropy catalysts and their electrocatalytic performances has been extensively investigated. Based on this motivation, we comprehensively and systematically summarize HEMs, outline their intrinsic properties and electrochemical advantages, generalize current state-of-the-art synthetic methods, analyze electrochemical active centers in conjunction with characterization techniques, utilize theoretical research to conduct a high-throughput screening of the targeted high-entropy catalyst and the exploration of the reaction mechanisms, and importantly, focus specially on the electrochemical applications of high-entropy catalysts and propose strategies for regulating electronic structure to accelerate electrochemical reaction kinetics, including morphological control, defect engineering, element regulation, strain engineering and so forth. Finally, we provide our personal views on the challenges and further technical improvements of high-entropy catalysts. This work can provide valuable guidance for future research on high-entropy electrocatalysts.
Enhanced interlayer interaction in sulfonated CONs membrane by amino-rich CONs enabling ultrafast proton transport
Ping Li, Bo He, Xuan Li, Yunfei Lin, Shaokun Tang
, Available online  , doi: 10.1016/j.gee.2024.07.008
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Covalent organic framework nanosheets (CONs) with porous crystalline features and ultrathin thickness are ideal candidates as membrane building blocks to form well-defined transfer nanochannels. The formidable challenge behind self-supporting CONs membrane lies in weak non-covalent interlayer interactions and thus loose stacking, insufficient strength and structure stabilities. Herein, we propose the fabrication of interlayer force-strengthened freestanding CONs membrane through the electrostatic attraction bridge effect of positively-charged amino-rich CONs (CON-NH2) to negatively-charged sulfonated CONs (CON-SO3H). Ultrathin and large lateral sized CON-SO3H and CON-NH2 are synthesized, followed by restacking to prepare freestanding CONs membrane with CON-SO3H as the membrane bulk. Benefiting from effective interlayer interconnection due to strong electrostatic interaction, the obtained CON-SO3H/CON-NH2 membrane displays features of ultrahigh integrity, dense stacking, eminent water/acid/base/organic solvents stabilities and mechanical strength (109 MPa). The shortened −SO3H distance contributes to construct site-continuous transfer pathways, and the deprotonated −SO3H and protonated –NH2 form acid-base pairs to decrease interfacial resistance, which impart membrane superior proton conductivity of 486 mS cm-1 (80 ℃, 100% RH). This interlayer force enhancement strategy offers a promising perspective on achieving densely-stacked CONs membrane with ultrahigh mechanical property and conduction performance for fuel cell application.
Antibiotics-heavy metals combined pollution in agricultural soils: Sources, fate, risks, and countermeasures
Yuanxiang Shu, Donghao Li, Tong Xie, Ke Zhao, Lu Zhou, Fengxiang Li
, Available online  , doi: 10.1016/j.gee.2024.07.007
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Agricultural soil is related to food security and human health, antibiotics and heavy metals (HMs), as two typical pollutants, possess a high coexistence rate in the environmental medium, which is extremely prone to inducing antibiotic-HMs combined pollution. Recently, frequent human activities have led to more prominent antibiotics-HMs combined contamination in agricultural soils, especially the production and spread of antibiotic resistance genes (ARGs), heavy metal resistance genes (MRGs), antibiotic resistant bacteria (ARB), and antibiotics-HMs complexes (AMCs), which seriously threaten soil ecology and human health. This review describes the main sources (Intrinsic and manmade sources), composite mechanisms (co- selective resistance, oxidative stress, and Joint toxicity mechanism), environmental fate and the potential risks (soil ecological and human health risks) of antibiotics and HMs in agricultural soils. Finally, the current effective source blocking, transmission control, and attenuation strategies are classified for discussion, such as the application of additives and barrier materials, as well as plant and animal remediation and bioremediation, etc., pointing out that future research should focus on the whole chain process of “source-process-terminal”, intending to provide a theoretical basis and decision-making reference for future research.
Boosting electrochemical reduction of CO2 to CO using molecule-regulated Ag nanoparticle in ionic liquids
Fangfang Li, Kuilin Peng, Chongyang Jiang, Shaojuan Zeng, Xiangping Zhang, Xiaoyan Ji
, Available online  , doi: 10.1016/j.gee.2024.07.005
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Electrochemical reduction of CO2 is a promising approach to convert CO2 to high-valued chemicals and fuels. However, developing efficient electrocatalysts featuring desirable activity and selectivity is still a big challenge. In this work, a strategy of introducing functionalized molecules with desirable CO2 affinity to regulate Ag catalyst for promoting electrochemical reduction of CO2 was proposed. Specifically, 3-mercapto-1,2,4-triazole was introduced onto the Ag nanoparticle (Ag-m-Triz) for the first time to achieve selectively converting CO2 to carbon monoxide (CO). This Ag-m-Triz exhibits excellent performance for CO2 reduction with a high CO Faradaic efficiency (FECO) of 99.2% and CO partial current density of 85.0 mA/cm2 at -2.3 V vs. Ag/Ag+ in H-cell when combined with the ionic liquid-based electrolyte, 30 wt% 1-butyl-3-methylimidazolium hexafluorophosphate ([Bmim][PF6])-65 wt% acetonitrile (AcN)-5 wt% H2O, which is 2.5-fold higher than the current density in Ag-powder under the same condition. Mechanism studies confirm that the significantly improved performance of Ag-mTriz originates from (i) the stronger adsorption ability of CO2 molecule and (ii) the weaker binding energy to form the COOH* intermediate on the surface of Ag-m-Triz compared with the Ag-powder catalyst, which boosts the conversion of CO2 to CO. This research provides a facile way to regulate electrocatalysts for efficient CO2 reduction by introducing functionalized molecules.
Heterogeneous iron-based catalysts for a sustainable photoinduced nitrogen fixation
Amalia M. Grigoras, Federica Valentini, Loredana Latterini, Luigi Vaccaro
, Available online  , doi: 10.1016/j.gee.2024.07.003
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Ammonia is nowadays one of the most important commodities chemicals intensively produced at about 175 million tons per year, contributing to 1.8 % of the global energy demand. The constantly increasing NH3 demand is also paralleled to the high CO2 emissions associated with its production. Therefore, decarbonizing NH3 synthesis is one of the most urgent contemporary challenges. Taking inspiration from Nature, solar-driven nitrogen fixation under mild conditions is one of the most promising yet challenging alternatives to classic methods. In this review, we focused our attention on the photocatalytic methods for the synthesis of ammonia; in particular, we concentrated on stable and recyclable heterogeneous Fe-based photocatalysts for the production of NH3. Indeed, recoverable and widely abundant and low-cost iron catalysts may represent a very promising tool for future sustainable access to this largely desired chemical target. After an overview of the pioneering works on Fe-driven nitrogen photofixation, the recent strategies on the use of Fe are herein reported. From the comparison with pristine photocatalysts, the addition of Fe as dopant or composite and heterojunction highly enhances the photocatalytic performances, opening the way to sustainable and low-cost nitrogen production.
Copper Silicate Nanoneedle Arrays on Reduced Graphene Oxide Like “Shelter Forest” Guiding Zn Gradient Deposition
Na Gao, Yang Wang, Zhanming Gao, Tianming Lv, Mengyu Rong, Xueying Dong, Dongzhi Chen, Changgong Meng, Yifu Zhang
, Available online  , doi: 10.1016/j.gee.2024.07.004
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With the sustainable and efficient development of aqueous zinc ion batteries (AZIBs), the research on addressing the issues of the adaptability and durability of zinc anodes has been hot-topic and is still of great challenge. In this work, inspired by the sand treatment and afforestation of the Gobi Beach in Northwest China to ameliorate the problem of wind and sand encroachment, we propose a material with a morphology similar to that of a “shelter forest”, CuSiO3 nanoneedles arrays grown on both sides of reduced graphene oxide (rGO@CuSi), as a coating layer on the zinc metal surface to guide Zn gradient deposition. The presence of rGO improves the electrical conductivity of CuSiO3, and the finite element simulation of the electric field and Zn2+ concentration proves that the electric field distribution can be effectively homogenized and the local current density can be reduced for the rGO@CuSi-Zn electrode with the surface presenting the shape of a protective forest. This is due to the abundant pores between the nano-needle array structures on the surface of the electrode, which provides high electron and ion transport paths, and are conducive to achieve uniform Zn deposition, like the principle of wind-sand stabilization by protective forest. Both electrochemical experiments and density functional theory calculations show that the negatively charged surface of rGO@CuSi with good Zn affinity is more capable of guiding Zn2+ transport. Thanks to its inherent material and structural characteristics, the rGO@CuSi-Zn anode has a high specific capacity and good cycling stability. This study provides an insight for interface engineering like protective forest to accelerate the commercialization of high-performance Zn-based batteries.
Rational engineering of triazine-benzene linked covalent-organic frameworks for efficient CO2 photoreduction
Yanghe Fu, Yijing Gao, Huilin Jia, Yuncai Zhao, Yan Feng, Weidong Zhu, Fumin Zhang, Morris D. Argyle, Maohong Fan
, Available online  , doi: 10.1016/j.gee.2024.07.002
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Three large π-conjugated and imine-based COFs, named TFP-TAB, TFP-TTA, and TTA-TTB, were synthesized via the ordered incorporation of benzene and triazine rings in the same host framework to study how the structural units affect the efficiency of CO2 photoreduction. Results from both experiments and density-functional theory (DFT) calculations indicate the separation and transfer of the photoinduced charges is highly related to the triazine-N content and the conjugation degree in the skeletons of COFs. High-efficiency CO2 photoreduction can be achieved by rationally adjusting the number and position of both benzene and triazine rings in the COFs. Specifically, TTA-TTB, with orderly interlaced triazine-benzene heterojunctions, can suppress the recombination probability of electrons and holes, which effectively immobilizes the key species (COOH) and lowers the free energy change of the potential-determining step, and thus exhibits a superior visible-light-induced photocatalytic activity that yields 121.7 μmol HCOOH g-1 h-1. This research, therefore, helps to elucidate the effects of the different structural blocks in COFs on inherent heterogeneous photocatalysis for CO2 reduction at a molecular level.
Synergistic Li6PS5Cl@Li3OCl Composite Electrolyte for High-Performance AllSolid-State Lithium Batteries
Yuzhe Zhang, Haolong Chang, Aiguo Han, Shijie Xu, Xinyu Wang, Shunjin Yang, Xiaohu Hu, Yujiang Sun, Xiao Sun, Xing Chen, Yongan Yang
, Available online  , doi: 10.1016/j.gee.2024.07.001
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Li6PS5Cl is a highly wanted sulfide-solid-electrolyte (SSE) for developing allsolid-state lithium batteries, due to its high ionic conductivity, good processability and abundant compositional elements. However, its cyclability is poor because of harmful side reactions at the Li6PS5Cl/Li interface and growth of lithium dendrites inside Li6PS5Cl phase. Herein, we report a simple interface-engineering remedy to boost the electrochemical performance of Li6PS5Cl, by coating its surface with a Li-compatible electrolyte Li3OCl having low electronic conductivity. The obtained Li6PS5Cl@Li3OCl core@shell structure exhibits a synergistic effect. Consequently, compared with the bare Li6PS5Cl, this composite electrolyte exhibits great performance improvements: 1) In Li|electrolyte|Li symmetric cells, the critical current density at 30℃ gets increased from 0.6 mA/cm2 to 1.6 mA/cm2, and the lifetime gets prolonged from 320 h to 1400 h mA/cm2; 2) In Li|electrolyte|NCM721 full cells running at 30°C, the cycling capacity at 0.2 C (or 0.5 C) gets enhanced by 20% (or from unfeasible to be feasible) for 100 cycles and the rate capability reaches up to 2 C from 0.2 C; and in full cells running at 60°C, the cycling capacity is increased by 7% at 0.2 C and the rate capability is enhanced to 3.0 C from 0.5 C. The experimental studies and theoretical computations show that the performance enhancements are due to the confined electron penetration and suppressed lithium dendrites growth at the Li6PS5Cl@Li3OCl interface.
2D/2D homojunction-mediated charge separation: Synergistic effect of crystalline C3N5 and g-C3N4 via electrostatic self-assembly for photocatalytic hydrogen and benzaldehyde production
Sue-Faye Ng, Joel Jie Foo, Peipei Zhang, Steven Hao Wan Kok, Lling-Lling Tan, Binghui Chen, Wee-Jun Ong
, Available online  , doi: 10.1016/j.gee.2024.06.008
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Homojunction engineering is a promising modification strategy to improve charge carrier separation and photocatalytic performance of carbon nitrides. Leveraging intrinsic heptazine/triazine phase and face-to-face contact, crystalline C3N5 (CC3N5) was combined with protonated g-C3N4 (pgCN) through electrostatic self-assembly to achieve robust 2D/2D homojunction interfaces. The highest photocatalytic performance was obtained through crystallinity and homojunction engineering, by controlling the pgCN:CC3N5 ratio. The 25:100 pgCN:CC3N5 homojunction (25CgCN) had the highest hydrogen production (1409.51 µmol h-1) and apparent quantum efficiency (25.04%, 420 nm), 8-fold and 180-fold higher than CC3N5 and pgCN, respectively. This photocatalytic homojunction improves benzaldehyde and hydrogen production activity, retaining 89% performance after 3 cycles (12 h ) on a 3D-printed substrate. Electron paramagnetic resonance demonstrated higher ·OH-, ·O2- and hole production of irradiated 25CgCN, attributed to crystallinity and homojunction interaction. Thus, electrostatic self-assembly to couple CC3N5 and pgCN in a 2D/2D homojunction interface ameliorates the performance of multifunctional solar-driven applications.
Conjugated polyaniline as “conveyor” in tungstate boosting cation storage for high-performance aqueous batteries
Yanyan Liu, Zirui Shao, Tianming Lv, Zilong Zhang, Zhenhua Zhou, Tao Hu, Changgong Meng, Yifu Zhang
, Available online  , doi: 10.1016/j.gee.2024.06.004
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Aqueous ion storage systems have motivated great interest by virtue of low reduction, high eco-sustainability and safety. Among various cathode candidates, transition metal compounds are featured with easy dissolution in aqueous solutions and inferior conductivity, which severely hinder their application. Herein, advantages are taken of the “conveyor effect” of conjugated polyaniline to prepare an oxygen defective tungstate-linked polyaniline (Od-WOP) material with chrysanthemum-like microstructure. By virtue of the high electronic conductivity derived from conductive conjugated polyaniline skeleton, unbalanced charge distribution triggered by the defective structure, and reversibly rapid ion (de)intercalation benefited from the open framework with porous chrysanthemum-like microstructure, it delivers outstanding rate capability with a maximum specific capacity of 162.2 mAh g-1 and great cycle stability for storing NH4+. Additionally, it also adopts a high reversible capacity of 140.4 mAh g-1 and outstanding cycling performance to store Ca2+. Consequently, the assembled Od-WOP//PTCDI flexible aqueous ammonium ion batteries and calcium ion batteries exhibit superior capacities, energy densities and flexibilities. Od-WOP achieves the NH4+ and Ca2+ storage capability by interacting with them through hydrogen and ionic bonds, respectively. The deep insight from this work sheds light upon a novel strategy to excavate greater potential of transition metal compounds for aqueous ion batteries.
NiCoMn-LDH with core-shell heterostructures based on CoS nanotube arrays containing multiple ion diffusion channels for boosted supercapacitor applications
Xiaojie Xu, Huachen Lin, Jinrui Ding, Pengjie Zhou, Yulong Ying, Hong Jia, Longhua Li, Yu Liu
, Available online  , doi: 10.1016/j.gee.2024.06.002
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Nanostructure engineering and composition rationalization are crucial for materials to become candidates for high-performance supercapacitor. Herein, a novel core-shell heterostructured electrode, combining CoS hollow nanorods with NiCoMn-layered double hydroxides (LDH) ternary metal nanosheets, were prepared on carbon cloth by reasonably controlled vulcanization and electrodeposition. By optimizing electrodeposition conditions, the material's structure and properties can be fine-tuned. The enhanced capacitance of the optimized carbon cloth (CC)@CoS/NiCoMn-LDH- 300 electrode (4256.0 F g-1) lies in the open space provided by CoS and the establishment of a new charge transfer channel across the interfaces of CC@CoS/NiCoMn-LDH-300 nanosheets. This is further demonstrated by Density functional theory (DFT) simulations based on OH- adsorption energy, which produces faster redox charge kinetics and significantly enhances the electrode’s energy storage capacity. The hybrid supercapacitor, integrating the optimized CC@CoS/NiCoMnLDH-300 electrode with active carbon, demonstrates the highest energy density of 86 Wh kg-1 (under the power density of 850 W kg-1) and the long cycle stability of 89.7%. This study aims to go beyond simple binary LDH by constructing a ternary LDH with a hierarchical core-shell heterostructure to provide an effective and feasible new concept for high-performance supercapacitor electrode materials via rational structure design.
Progress in the construction strategy of noble metal active sites for zeolite-based PNA and VOCs catalysts
Yuan Yao, Haodan Cheng, Guocai Zhong, Xiaolong Tang, Honghong Yi, Shunzheng Zhao, Fengyu Gao, Qingjun Yu
, Available online  , doi: 10.1016/j.gee.2024.06.001
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Zeolite-loaded noble metal catalysts have demonstrated excellent performance in addressing cold-start automotive exhaust NOx emissions and catalytic oxidation of VOCs applications. Pd and Pt are the most commonly used active metals in PNA and VOC catalysts, respectively. However, despite the same metal/zeolite composition, the efficient active sites for PNA and VOC catalysts have been viewed as mainly Pd2+ and Pd0, respectively, both of which are different from each other. As a result, various methods need to be applied to dope Pd and Pt in zeolitic support respectively for different usages. No matter which type of metal species is needed, the common requirement for both PNA and VOC catalysts is that the metal species should be highly dispersed in zeolite support and stay stable. The purpose of this paper is to review the progress of synthetic means of zeolite-coated noble metals (Pd, Pt, etc.) as effective PNA or VOC catalysts. To give a better understanding of the relationship between efficient metal species and the introduced methods, the species that contributed to the NOx adsorption (PNA) and VOCs deep catalytic oxidation were first summarized and compared. Then, based on the above discussion, the detailed construction strategies for different active sites in PNA and VOC catalysts, respectively, were elaborated in terms of synthetic routes, precursor selection, and zeolite carrier requirements. It is hoped that this will contribute to a better understanding of noble metal adsorption/catalysis in zeolites and provide promising strategies for the design of adsorption/catalysts with high activity, selectivity and stability.
Engineering crystal plane of NiCo2O4 to regulate oxygen vacancies and acid sites for alkali-free oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid
Hengli Qian, keyuan Zhang, Yongchuo He, Qidong Hou, Chao Xie, Ruite Lai, Guanjie Yu, Tianliang Xia, Xinyu Bai, Haijiao Xie, Meiting Ju
, Available online  , doi: 10.1016/j.gee.2024.05.002
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The catalytic oxidation of HMF involves a cascading reaction with multiple intermediate products, making it crucial to enhance the oriented adsorption capacity of specific functional groups for accelerating the entire process. To achieve the efficient selective oxidation of HMF to FDCA, a series of NiCo2O4 catalysts with different morphologies, such as flaky, echinoids, pompon and corolla, were prepared and characterized by XRD, SEM, TEM, BET, XPS, and FTIR. Among the four catalysts, flaky NiCo2O4 exhibited the most excellent catalytic activity and stability, with a FDCA yield of 60.1% within 12 h at 80 ℃ without alkali participation. The excellent performance of flaky NiCo2O4 catalyst is attributed to the oxygen vacancies and acid sites generated by the exposed (400) facets. The oxygen vacancies and acid sites on the catalyst surface can precisely adsorb -CHO and -CH2-OH of HMF, respectively, and this synergistic effect promotes the efficient production of FDCA. This work is of great significance for fundamentally study the effect of micro-topography or crystal-plane reaction properties on surfaces.
Potassium-doped hydrated manganese dioxide nanowires-carbon nanotube on graphene for high performance rechargeable zinc-ion battery
Ting-Hao Xu, Sin Liou, Fan-Lin Hou, Yuan-Yao Li
, Available online  , doi: 10.1016/j.gee.2021.10.006
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Aqueous rechargeable Zn-ion battery (ARZIB) is a great candidate for the next generation battery due to its high safety, low cost, and relatively high capacity. Here, we develop hydrated and potassium-doped manganese dioxide (MO) nanowires mixed with carbon nanotubes (CNT) on graphene substrates (hydrated KMO-CNT/graphene) for ARZIB. A simple polyol process (poly(ethyl glycol), KMnO4, CNTs, and graphene) is conducted to form the hydrated KMO-CNT/graphene. MnO2 nanowires with diameters of 15–25 nm have a high specific capacity with a short diffusion path. The intercalated K ions and hydrates in the layered MnO2 nanowires remain the MO structure during the charge and discharge process, while carbon nanomaterials (CNTs and graphene) enhance the conductivity of the materials. As a result, the hydrated KMOCNT/graphene demonstrates a good ARZIB performance. A high capacity of 359.8 mAh g-1 at 0.1 A g-1 can be achieved while, at a high current density of 3.0 A g-1, the capacity of 129 mAh g-1 can be obtained with 77% retention after 1000 cycles.

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