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Structure–Activity Relationship in Periodate Activation by Fe-MOFs: Why MIL-101(Fe) Outperforms Other MIL-Series in Antibiotic Degradation
Ning Liu, Jingwen Xu, Yixuan Zhai, Ziyi Zhang, Yi Dang, Yusong Cao, Zhe Li, Wenyuan Huang, Xiaodong Zhang, Liang Tang
, Available online  , doi: 10.1016/j.gee.2025.10.006
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Antibiotics are emerging pollutants that pose significant risks to environmental and human health. Periodate (PI)-based advanced oxidation processes have shown promise for their effective degradation. In this study, we systematically investigate the structure-activity relationship of four representative Fe-based metal-organic frameworks (Fe-MOFs)—MIL-101(Fe), MIL-88B(Fe), MIL-88A(Fe), and MIL-53(Fe)—as PI activators for tetracycline (TC) degradation. Among them, MIL-101(Fe) exhibited the highest catalytic performance, owing to its unique Fe3O-OH nodes and mesoporous architecture. The MIL-101(Fe)/PI system achieved 93.3% TC degradation and 55.9% mineralization rate within 60 minutes. Mechanistic studies combining scavenger quenching, sulfoxide probe transformation, X-ray photoelectron spectroscopy, and X-ray absorption fine structure confirmed the generation of multiple reactive oxygen species, and high-valent Fe(IV)=O and O2·- played major roles in the tetracycline degradation process. Density functional theory calculations further revealed that MIL-101(Fe) and MIL-88B(Fe) effectively interact with PI to form Fe(III)-superoxide (Fe(III)-O-O·-), a key intermediate in Fe(IV)=O generation. In contrast, the adsorption energy of MIL-53 (Fe) and MIL-88A (Fe) was relatively weak, with fewer binding sites, resulting in poor performance. The synergy between Fe(III)-O-O·- formation and the pore accessibility of MIL-101(Fe) accounted for its superior catalytic efficiency. This work not only clarifies the structural factors governing PI activation in Fe-MOFs, but also proposes a mechanistically informed strategy for designing high-performance catalysts for antibiotic degradation.
Unraveling the regulation rules of vanadium-site cation substitution for Na3V2(PO4)3 cathode materials toward high energy density sodium-ion batteries
Yi-Meng Wu, Jing-Yu Wang, Hao-Tian Guo, Peng-Fei Wang, Zong-Lin Liu, Yan-Rong Zhu, Jie Shu, Ting-Feng Yi
, Available online  , doi: 10.1016/j.gee.2025.10.009
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NASICON-type Na3V2(PO4)3 (NVP) materials are seen as highly promising cathode materials in the field of sodium-ion batteries due to their low cost, a solid three-dimensional skeleton and good theoretical capacity, as well as high ionic conductivity. Nevertheless, the problem of low intrinsic electronic conductivity and energy density has limited the practical application of the materials. To address this issue, the relevant research team has successfully achieved remarkable research results through unremitting exploration and practical innovation. In this work, the crystal structure, ion migration mechanism and sodium storage mechanism of NVP cathode materials are systematically reviewed, with a focus on summarizing the latest progress of V-site doping modification research, classifying and exploring V-site doping from the perspectives of electronic structure, lattice strain and entropy, and briefly describing the optimization mechanism of V-site doping on electrochemical performance. In addition, the challenges and prospects for the future development of NVP cathode materials are presented, which are believed to provide new thinking for the design and development of high-performance NVP cathode materials and contribute to the large-scale application of sodium-ion batteries.
High-Value Utilization of Waste Plastics: Transforming Plastic Polymers into Thin-Walled and Uniform Carbon Nanotubes via Catalytic Pyrolysis
Ning Cai, Siqian Jia, Kunpeng Sun, Jiahui Zhu, Chuanwen Zhao, Haiping Yang
, Available online  , doi: 10.1016/j.gee.2025.10.004
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The high-value utilization of waste plastics plays a crucial role in mitigating plastic pollution. In this work, transition metals were selected as active species, while magnesium oxide, derived from the calcination of basic magnesium carbonate, served as the support material for the generation of thin-walled carbon nanotubes (CNTs). The confined pore structure restricts the migration of reduced iron nanoparticles, promoting the nucleation and growth of small-diameter and thin-walled CNTs. The results show that over 10 wt.% carbon deposits were collected from various types of plastics. The CNTs generated from polyethylene exhibit a diameter of approximately 8 nm and a wall thickness of about 6 layers of graphite. Additionally, Ni-based and Co-based catalysts, polypropylene and polystyrene have also been studied and around 10 nm CNTs were produced. Moreover, this study further demonstrates that excessively high or low temperatures are detrimental to the growth of CNTs. To sum up, this work proposes a novel strategy for recycling waste plastics into smaller-diameters CNTs, offering significant potential for the high-value utilization of waste.
Boosting efficient C-C Coupling toward Electrocatalytic Acetate Synthesis from CO2 via Close Cu+/Ag Dual Active Sites
Ruifeng Wang, Yuchang Liu, Yandong Li, Yafen Kong, Qizhi Chen, Shuangliang Zhao
, Available online  , doi: 10.1016/j.gee.2025.10.005
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Efficiency of C-C bond coupling in highly inert CO2 is relatively low, which severely limits its efficient conversion to acetate. Here, we successfully developed a highly stable NF@CoMn2O4@Cu2O-Ag bimetallic active site catalyst by anchoring Ag on the Cu2O surface. In this catalyst, the Co3+/Mn3+-Mn4+ removes excess electrons from the Cu+ sites via strong electronic interactions, preventing the reduction of Cu2O to metallic Cu0, which ensures the NF@CoMn2O4@Cu2O-Ag exhibits a high resistance to deactivation. The Cu+ active sites of NF@CoMn2O4@Cu2O-Ag efficiently electroreduce CO2 to the *COatop intermediate, while the Ag active sites efficiently electroreduce CO2 to the *CObridge intermediate. The proximity of Cu+/Ag bimetallic sites shortens the distance for C-C bond coupling between the *COatop and *CObridge intermediates, facilitating the efficient electrocatalytic coupling of CO2 to synthesize acetate. DFT analysis indicates that the ΔG required for C-C bond coupling on the short-distance Cu+/Ag bimetallic sites of NF@CoMn2O4@Cu2O-Ag is significantly lower than that of NF@CoMn2O4@Cu2O, enabling a high Faradaic efficiency of 64.97% for acetate production at -0.3 V vs. RHE. This study provides an effective strategy for the rational design of synergistic catalysis between heterometallic catalytic sites to efficiently achieve C-C coupling for the synthesis of C2+ products.
Peroxymonosulfate activation on the S-scheme heterojunction Bi4O5I2/TiO2 photoanode of a photocatalytic fuel cell for degradation of tetracyclines with green power generation
Huizhong Wu, Ruiheng Liang, Yujie Chen, Xiuwu Zhang, Jingyang Liu, Zehua Xia, Ignasi Sirés, Minghua Zhou
, Available online  , doi: 10.1016/j.gee.2025.10.002
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Photocatalytic fuel cells (PFC) are green devices for simultaneous contaminant degradation and power generation. However, their performance is still limited due to the inefficient light capture and poor charge transfer at photoanodes. Here, a PFC has been successfully developed using a Bi4O5I2/TiO2 nanotube arrays (NTAs) S-scheme heterojunction as the photoanode, incorporating peroxymonosulfate (PMS) as synergistic precursor of reactive oxygen species (ROS). A 17-fold increase in rate constant for the degradation of tetracycline (TC) and 6.6-fold increase in maximum power generation was attained in comparison with the TiO2/light PFC system. A systematic analysis elucidating PMS-mediated regulation of ROS generation and electron transfer was performed. The photocatalytic mechanism, dominated by non-radical 1O2 and photogenerated holes (h+), led to a maximum photocurrent density (0.091 mA cm-2) and output power (0.99 mW cm-2). The current work demonstrates the great robustness of heterojunction-based PFC as new self-powered water decontamination systems.
Integrated reaction–separation in a pilot-scale catalytic membrane reactor for efficient continuous p-nitrophenol hydrogenation
Ziming Chen, Yuyan Gao, Zhihao Guo, Yan Du, Zhengyan Qu, Jiuxuan Zhang, Zhenchen Tang, Hong Jiang, Rizhi Chen
, Available online  , doi: 10.1016/j.gee.2025.10.001
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Hydrogenation reactions, vital in chemical engineering, are hampered by limitations including catalyst recovery, mass transfer issues, and scalability. Catalytic membrane reactors offer a promising alternative by integrating reaction and separation, boosting efficiency and simplifying catalyst handling. However, scaling these membranes to industrial levels while ensuring long-term stability and high efficiency remains a significant challenge. This study tackles this by developing and demonstrating a pilot-scale multi-channel ceramic catalytic membrane reactor system. This system, featuring three 19-channel ceramic catalytic membranes, achieved nearly 100% p-nitrophenol hydrogenation conversion consistently over 600 h of continuous liquid-phase operation. This underscores the multi-channel ceramic catalytic membrane superior catalytic efficiency, remarkable long-term stability, and strong scalability. This work establishes a robust platform for continuous-flow hydrogenation, providing a solid foundation for practical catalytic membrane reactors technology application in the chemical industry.
Advancements in synthesis strategies and environmental application of FAU-type zeolite: Bibliometric-driven review
Lin Chen, Bingqing Xu, Siying Wang, Shan Ren, Fan Yang, Wei Zhang, Yuanpei Lan, Chaoyi Chen, Junqi Li, Yanbing Su
, Available online  , doi: 10.1016/j.gee.2025.10.003
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FAU zeolites have emerged as multifunctional materials with broad applications in catalysis and adsorption, owing to their hierarchical pore architectures, elevated specific surface areas, and adjustable extra-framework cationic sites. This review provides a critical overview of recent advances in FAU zeolite research with emphasis on their roles in environmental pollutant mitigation. A bibliometric analysis was performed to ascertain worldwide research trends, cooperation networks, and principal theme areas. Strategies for synthesis and functionalization, including crystallization pathways, one-pot methods, and post-synthetic modifications, were systematically evaluated for their capacity to tailor structural and physicochemical properties. Environmental applications were discussed in detail, particularly in heavy metal extraction, CO2 capture, and catalytic NOx reduction. Despite these advances, challenges persisted, notably restricted chemical stability under extreme pH conditions, scalability obstacle from laboratory to industrial production, and the necessity for enhanced catalytic efficiency, were emphasized. By integrating fundamental understanding with application-oriented perspectives, this review identifies existing knowledge gaps and delineates future directions for the rational design of FAU zeolites toward sustainable environmental remediation.
Ionic Liquids for olefin extractive separation from fluid catalytic cracking naphtha: Thermodynamics and molecular mechanisms
Wen-Hai Zhang, Jian Gao, Yue Zhang, Christoph Held, Gangqiang Yu, Hong Meng
, Available online  , doi: 10.1016/j.gee.2025.09.005
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This study investigates the extractive separation of olefins from fluid catalytic cracking (FCC) naphtha using ionic liquids (ILs), from the perspectives of molecular thermodynamics and separation mechanisms. Initially, a representative binary mixture of benzene and 1-hexene was employed to screen various ILs for their separation performance, based on COSMO-RS calculations combined with relevant physicochemical property evaluations. Consequently, 1-ethyl-3-methylimidazolium thiocyanate ([EMIM][SCN]) was identified as the most promising extractant. Subsequently, the liquid-liquid equilibrium (LLE) behavior of ternary systems involving the selected IL and the benchmark solvent sulfolane (SUL) was quantitatively predicted using the Perturbed-Chain Statistical Associating Fluid Theory (PC-SAFT). In this modeling framework, ILs were treated as electrically neutral components due to the significant ion-pair electrostatic interactions in non-aqueous media, thus, the IL-related mixed systems are named as “complex strong electrostatic-hydrogen bonding organic systems”. Finally, quantum chemical (QC) calculations were conducted to elucidate the underlying molecular-level separation mechanism. The results indicate that [EMIM][SCN] exhibits significantly stronger intermolecular interactions with the organic components than SUL, thus accounting for its superior extraction performance. These findings provide valuable insights for the rational design of task-specific ILs for efficient olefin separation in petroleum refining processes.
Defect Engineering of TiO2 for Efficient Photocatalytic Transfer Hydrogenation with Palladium as Cocatalyst and Water as a Hydrogen Source
En Zhao, Jingyuan Su, Hehe Fan, Bing Nan, Lina Li, Haifeng Qi, Weiwei Fang, Wenjun Zhang, Zupeng Chen
, Available online  , doi: 10.1016/j.gee.2025.09.008
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Photocatalytic transfer hydrogenation using water as the proton source has emerged as an attractive and green approach for the catalytic reduction of unsaturated bonds. Herein, we report an oxygen-defective TiO2-supported palladium catalyst (Pd-TiO2-Ov) for efficient photocatalytic water-donating transfer hydrogenation of anethole towards 4-n-propylanisole in a high yield of 99.9%, which is significantly higher compared to the pristine TiO2-supported palladium catalyst (Pd-TiO2, 74%). The enhanced performance is ascribed to the presence of oxygen vacancies, which facilitate light absorption and suppress the recombination of photogenerated electron-hole pairs. Furthermore, the Pd-TiO2-Ov is versatile in hydrogenating various alkene substrates including those with hydroxyl, ether, fluoride, and chloride functional groups in full conversion, thus offering a green method for transfer hydrogenation of alkenes. This study provides new insights and advances in current hydrogenation technology with water as the proton source.
High-efficiency capacitive deionization: Freestanding carbon electrodes derived from fungal hyphae with in-situ oriented MOF growth
Jiao Chen, Kuichang Zuo, Jiajin Liang, Gang Wang, Lin Lin, Xiao-yan Li
, Available online  , doi: 10.1016/j.gee.2025.09.009
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High-performance electrode materials are critical for the development of the capacitive deionization (CDI) technology for efficient water desalination. In this study, binder-free porous carbon electrodes were successfully prepared from the fungal hyphae sheet with the formation and growth of metal-organic framework (MOF) crystals on the surface of hyphal fibers. The continuous fungal fibrous structure with abundant surface functional groups provided an ideal supporting substrate for in-situ oriented MOF growth. The MOF-fungal hyphae derived carbon (MOF-Fhy-C) exhibited an excellent property for CDI application, such as a large accessible surface area, excellent electrical conductivity, high porosity and hydrophilicity. The MOF-Fhy-C electrode achieved an outstanding CDI performance with a salt adsorption capacity of 40.8 mg/g and an average salt adsorption rate of 1.4 mg/(g·min) for treating 10 mmol/L NaCl solution at a cell voltage of 1.2 V, which are considerably higher than most of carbon-based electrodes reported in the literature. This research presents an effective strategy for fabricating freestanding CDI electrodes from fungal materials with MOF for high-performance desalination.
Lignin-derived High-quality Graphene Quantum Dots: Synthesis, Mechanistic Insights, and Emerging Applications
Zheyuan Ding, Kunye Zhang, Junzhong Xie, Cenkai Zhao, Haoyu Li, Yan Zhang, Min Wang, Mingbo Wu
, Available online  , doi: 10.1016/j.gee.2025.09.007
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Lignin-based graphene quantum dots (L-GQDs), serving as a bridge between renewable biomass resources and functional carbon materials. This review begins with the molecular structure of lignin, exploring various synthesis methods for L-GQDs. The precise elucidation of precursor-structure-property relationships could optimize their performance through the quantitative regulation of lignin unit properties and enable controllable synthesis. We elaborate on the photoluminescence mechanisms and fluorescence modulation strategies of L-GQDs, covering aspects such as structural design, synthesis pathways, and photophysical property optimization. Additionally, the review discusses the application prospects of L-GQDs in biology, energy conversion, and optoelectronics, and highlights the importance of synergistically aligning synthesis strategies with practical on-demands application. We also prospected research paradigm should focus on in-situ unveiling of nucleation kinetics during L-GQDs formation, photoluminescence mechanism decoding, toxicity regulation to enable green, sustainable and multidisciplinary cutting-edge applications.
Oriented Superhydrophobic Bimetallic MOF Composite Membrane for Efficient Ethanol-Water Separation
Fengkai Wang, Yushan Zhang, Yiming Zhong, Mengxin Shen, Hao Sun, Jie Li, Naixin Wang, Hong Meng, Quan-Fu An
, Available online  , doi: 10.1016/j.gee.2025.09.012
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Extracting ethanol from aqueous solutions is important but challenging in industry. Pervaporation membranes show great promise for separating ethanol from water, with the design of their structure being crucial for enhancing performance. In this study, we developed an oriented bimetallic metal-organic framework (MOF) membrane, designated as ZIF-CoZn, for the pervaporation separation of ethanol from water. During crystal growth, bimetallic salts provide specific nucleation sites, and the competitive coordination between Co and Zn ions shifts the energetically favorable (100) plane to the (211) plane. This orientation enables precise molecular-level control over hydrophobic ligand arrangement, effectively repelling water molecules. Meanwhile, bimetallic competition enlarges pore sizes, facilitating ethanol permeation. When compared to single-metal MOF membranes made of cobalt or zinc, the separation factor of the ZIF-CoZn membrane for ethanol/water mixtures increased by 127% and 160%, respectively. Benefiting from the high roughness and increased exposure of hydrophobic ligands due to the preferential (211) orientation, ZIF-CoZn exhibits superhydrophobicity after vinyl-polydimethylsiloxane coating. The oriented ZIF-CoZn membrane was also scaled up to an area of 1 m2. This work provides valuable insights into optimizing MOF membrane structure and lays the foundation for its promotion and application in the industry.
Carbon nitride-based single-molecular Van der Waals heterojunction for selective photocatalytic CO2 reduction to CO
Hongjun Dong, Chunhong Qu, Jiaming Li, Deping Wang, Min Zhang, Zuoyi Liu, Liqiu Zhang, Chunmei Li
, Available online  , doi: 10.1016/j.gee.2025.09.004
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Single-molecular heterojunctions have demonstrated significant application potential in the fields of photocatalysis due to prominent photoelectric properties, while the charge transfer behavior still need to be further discussed. In this work, a fresh single-molecular Van der Waals heterojunction is fabricated through self-assembly of dibromo(1,10-phenanthroline-κN1,κN10)nickel (NiphenBr) molecules on the surface PCN nanosheets, which dramatically boosts the performance of selective photocatalytic CO2 reduction to CO. This unique assembled architecture effectively regulates electronic band structure and promotes the interfacial transfer and separation of photogenerated carriers owing to the π-π coupling effect between NiphenBr and PCN. Meanwhile, the single-molecular dispersed NiphenBr molecules also prevent their aggregation on PCN under the strong π-π interaction, and further provide abundant single-atom active sites for CO2 reduction reaction. Therefore, the average rate of photocatalytic reduction of CO2 to CO for the optimal NiphenBr/PCN-1 sample reaches 5.46 and 2.73 times that of PCN and NiphenBr, respectively. This work opens a new avenue for the single-molecular heterojunction in the application of photocatalytic reactions.
CO2 Utilization and Fixation in Biomass-Derived Furanics Conversion: Thermochemical and Electrochemical Pathways
Saeideh Gharouni Fattah, Sabah Karimi, Shaoyu Yuan, Zheng Li, Mohammad Jalal Zohuriaan-Mehr, Lu Lin, Xianhai Zeng, Buxing Han
, Available online  , doi: 10.1016/j.gee.2025.09.011
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Carbon dioxide (CO2) is the main greenhouse gas (GHG) released by human activities. The substitution of fossil resources by biomass as a bio-renewable resource, has significant potential to reduce GHG emissions. The approach to biomass, as the only true full-scale alternative to fossil resources, is progressing rapidly. Converting biomass into furanic compounds, as versatile platform chemicals for synthesizing a wide range of bio-based products is the cornerstone of sustainable technologies. The extensive body of this review combines the biomass valorization to furanic compounds by CO2 utilization and furanic compounds conversion by CO2 fixation. These processes can be strategically applied through both 'thermochemical' and 'electrochemical' pathways, by utilizing CO2 from the atmosphere or industrial emission point and returning it to the natural carbon cycle. In the thermochemical pathway CO2 acts as a carbon source (carboxylation and polymerization) or active reaction assistant in the biomass conversion (CO2-assisted conversion), without altering its oxidation state, facilitating the synthesis of valuable products and polymers. Conversely, in the electrochemical pathway, CO2 can be used as a carbon source (electrocarboxylation) to give the corresponding carboxylic acid, or it can undergo reduction, yielding methanol, carbon monoxide (CO), formic acid, and analogous compounds, while on the other side, furanic compounds undergo oxidation yielding high-value-added chemicals. Finally, potential future research directions are suggested to promote CO2 utilization and fixation in the valorization of biomass-derived furanic compounds, and challenges facing further research are highlighted.
Enhancing High Volumetric Energy Density of Supercapacitors through Diatomic Reconstruction of Layered Double Hydroxides
Rong Zheng, Lin Sun, Yi Guo, Yu Liu, Qingjun Yang, Wei Zhang, Yulong Ying, Weidong Shi
, Available online  , doi: 10.1016/j.gee.2025.09.001
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Double atom regulation and synergistic phosphorus doping and oxygen vacancy (OV) engineering are effective strategies for optimizing the electronic structure of layered double hydroxides (LDHs). In this study, a self-supporting P-doped OV-(Co0.5Ni0.5)3V2O8 electrode with interpenetrating carbon nanotube networks was synthesized via cation/anion co-reconstruction. Leveraging vanadium's high valence states, the dual-atom system creates a microporous architecture that enables precise charge redistribution, enhancing both electrical conductivity and OH- adsorption capacity. Density functional theory confirms that P-OV synergy reduces charge transfer resistance while optimizing ion diffusion pathways and charge storage kinetics. The optimized electrode achieves outstanding performance: 3807.9 F cm-3 volumetric capacitance at 1 A g-1 and exceptional cycling stability (100% capacity retention over 10000 cycles). Assembled asymmetric supercapacitors deliver 158.1 Wh L-1 energy density at 992 W L-1 power density, surpassing most reported LDH-based devices. This dual-atom charge redistribution mechanism establishes a universal paradigm for designing high-capacity electrodes, addressing critical challenges in energy storage materials through simultaneous electronic structure modulation and microstructural stabilization.
Computational Screening of Covalent Organic Frameworks for He Purification with Adsorption or Membrane Separation
Zenan Shi, Lijun Liao, Shujun Peng, Yanying Wei, Libo Li
, Available online  , doi: 10.1016/j.gee.2025.09.002
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Separating He from CH4 or N2 is crucial for natural gas He extraction, a prevailing industrial approach. Herein, molecular simulation and machine learning (ML) were combined to screen 801 experimentally synthesized COFs for He/CH4 and He/N2 separation, either by means of adsorption or membrane separation. Top 10 COFs for 4 different gas separation purposes (CH4/He or N2/He separation with either adsorption or membrane) were identified respectively. The highest adsorption performance score (APSmix, defined as the product of working capacity and adsorption selectivity for mixture gas) reached 447.88 mol/kg and 49.45 mol/kg for CH4/He and N2/He, with corresponding adsorption selectivity of 115.56 and 30.33. He permeabilities of 1.5 × 106 or 1.2 × 106 Barrer were achieved for equimolar He/CH4 or He/N2 mixture gas separations, accompanied by permselectivity of 5.47 and 11.80 well surpassing 2008 Robeson’s upper bound. Best performing COFs for adsorption separation are 3D COFs with pore diameter below 0.8 nm while those for membrane separation are 2D COFs with large pores. Additionally, ML models were developed to predict separation performance, with key descriptors identified. The mechanism for how COFs’ structure affects their separation performance was also revealed.
Tailoring the Architecture of Metal-Organic Frameworks: Precision Etching for Engineered Defects and Surfaces
Yunfei Jiang, Ziyi Zhang, Yongjian Du, Jinwen Jiao, Ya Bian, Di Cai, Houchao Shan
, Available online  , doi: 10.1016/j.gee.2025.09.006
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Metal-organic frameworks (MOFs) have emerged as promising materials owing to their high surface areas, tunable pore sizes, and diverse functionalities. However, their practical deployment is frequently hindered by intrinsic microporosity and structural fragility. In this review, we systematically analyze recent advancements in MOF etching techniques, which strategically modify framework architectures to enhance mass transport, expose active sites, and improve stability. The discussion encompasses a range of methods—including acid, base, ion, solvent, vapor, selective, in-situ, pyrolysis, and physical etching—with emphasis on the underlying mechanisms that govern the formation of hierarchical pore structures, defect engineering, and heterojunction formation. Notably, etching approaches facilitate precise control over crystal morphology and surface chemistry, thereby optimizing MOF performance in catalysis, electrocatalysis, photocatalysis, adsorption, energy storage, sensing, and biomedical applications. We also outline challenges such as etchant toxicity, over-etching risks, and scalability, while highlighting emerging strategies and computational simulations to refine the etching process. Ultimately, this review underscores the transformative impact of etching on MOF properties, paving the way for the design of next-generation multifunctional materials that address critical issues in environmental remediation, energy conversion, and beyond.
Efficient cyclohexane dehydrogenation over Pt/B-ZrO2 for H2 production
Lipeng Guo, Jihui Yao, Xiaojun Bao, Haibo Zhu
, Available online  , doi: 10.1016/j.gee.2025.09.010
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The efficient storage and release of H2 are pivotal for the advancement of hydrogen energy technologies. Cyclohexane, as a promising liquid organic hydrogen carrier (LOHC), provides a safe and practical solution for H2 storage. However, the performance limitations of dehydrogenation catalysts have hindered the rapid development of LOHC technology. In this study, we successfully developed boron-modified Pt/ZrO2 catalysts, which exhibit exceptional catalytic performance in cyclohexane dehydrogenation. The optimal boron content is determined to be 0.5 wt.%, with the Pt/0.5B-ZrO2 catalyst achieving high turnover frequency (TOF) of 10,627.3 molH2·molPt-1·h-1 and benzene selectivity of 99% at 295 °C. The catalyst also demonstrates H2 evolution rate of 908 mmol·gPt-1·min-1 and low deactivation rate of 0.0043 h-1. Remarkably, the catalyst displays outstanding stability and regeneration performance, maintaining its activity without significant loss during a 60-hour dehydrogenation reaction and retaining a cyclohexane conversion of 77.2% after 10 consecutive cycles. Comprehensive characterization techniques, including XPS, CO-FTIR, NH3-TPD, H2-TPD, Benzene-TPD, and Py-IR, reveals that boron modification reduces the electron density of Pt, generating abundant electron-deficient Pt atoms. These electron-deficient Pt atoms enhances H2 adsorption and accelerated benzene desorption, effectively preventing coke formation from deep benzene dehydrogenation, which is responsible for the high catalytic performance of the Pt/0.5B-ZrO2 catalyst. These findings offer a valuable strategy for optimizing dehydrogenation catalysts in liquid organic hydrogen carrier (LOHC) technologies, addressing a critical bottleneck in the development of this essential energy storage solution.
Synergistic Brønsted and Lewis Acid Sites for Selective Catalytic Valorization of Isopropanol from VOC Streams
Honghong Zhang, Zhiwei Wang, Lu Wei, Zhiquan Hou, Yuxi Liu, Hongxing Dai, Zhenxia Zhao, Jiguang Deng
, Available online  , doi: 10.1016/j.gee.2025.09.003
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Directional catalytic transformation of volatile organic compounds (VOCs) into value-added chemicals represents a more sustainable strategy than complete mineralization, as it simultaneously mitigates environmental pollution and reduces carbon emissions. The primary challenge in achieving multifunctional olefin production from alcohol-type VOCs is the lack of mechanistic clarity, which hinders the targeted synthesis of selective catalysts. Herein, we developed W-Ti hybrid metal oxide catalysts (WTiOx) with active Ti-O-W interfaces via a one-step hydrothermal synthesis and demonstrated their effectiveness for isopropanol conversion processes. Remarkably, WTiOx-500 achieved 99.8% isopropanol conversion and 99.3% propylene yield at 140 °C, significantly outperforming TiO2 (98.4% yield at 180 °C) and WO3 (90.5% yield at 240 °C). WTiOx-500 also displayed higher thermal stability, with isopropanol conversion and propylene yield decreasing by 1.0% and 1.6% after 35 h on-stream reaction. Although impurities (e.g., CO2, HCl, SO2) caused partial deactivation of WTiOx-500, oxygen treatment regenerated the catalyst. A series of characterization techniques indicated that the controlled calcination temperature promoted the formation of an optimal Ti-O-W interface in WTiOx-500 through W substitution into the TiO2 lattice and WO3-TiO2 surface interaction, where W species effectively tuned the electronic structure. This configuration endowed WTiOx-500 with moderate acidity of Brønsted (-OH) and Lewis (Ti4+/W6+) acid sites, which synergistically facilitated charge transfer between isopropanol and catalyst, accelerated C-O bond cleavage during dehydration. This work provides mechanistic insights into isopropanol dehydration and demonstrates a potential approach for VOC valorization.
Efficient construction of SiC membranes to filtrate high-temperature dust-laden gas for environmental sustainability
Shiying Ni, Yuqi Song, Dong Zou, Zhaoxiang Zhong, Weihong Xing
, Available online  , doi: 10.1016/j.gee.2025.08.003
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During the production processes of energy, metallurgy, chemical engineering, and other process industries, substantial high-temperature dust-laden flue gas is generated. Asymmetric silicon carbide (SiC) membranes exhibit significant potential in flue gas filtration since they enable direct filtration of high-temperature gas and facilitate thermal energy recovery. However, membrane particle penetration is a prevalent issue when constructing membrane layer directly on macroporous support, which contributes to a considerable mass transfer resistance. Herein, a novel hydrophobic modification strategy was developed to avoid the slurry penetration, thereby fabricating the asymmetric SiC membrane without the necessity of any intermediate or sacrificial layer. Firstly, the modifier concentration was adjusted to guarantee that the support was hydrophobic enough to prevent the slurry from penetrating. Subsequently, the slurry surface tension was fine-tuned by introducing ethanol to enhance the integrity of the SiC membrane. Furthermore, the effect of solid content was systematically investigated. It was demonstrated that the optimized SiC membranes obtained excellent gas permeance from 100.8 to 199.8 m3·m−2·h−1·kPa−1 with the pore size ranging from 1.93 to 3.89 μm. Also, the SiC membrane exhibited excellent stability for 24 h and achieved an excellent dust removal efficiency (99.99%) when filtering ultrafine dust particles (∼300 nm) under high temperatures. This method effectively bridges the membrane particle penetration issue caused by the particle size disparity among different layers of the asymmetric membrane, establishing an efficient strategy to fabricate high-permeance SiC membranes applied in high-temperature dust-laden gas filtration.
High-valent cobalt-oxo species mediated selective oxidation of glucose to chemicals in photocatalytic Fenton-like system
Tianliang Xia, Chengxu Wang, Xinyu Bai, Meiting Ju, Hengli Qian, Ruite Lai, Chao Xie, Guanjie Yu, Yao Tang, Fei Qu, Chaojie Zhang, Shuwen Zhou, Haijiao Xie, Shaolan Song, Qidong Hou
, Available online  , doi: 10.1016/j.gee.2025.08.001
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Peroxymonosulfate (PMS)-based Fenton-like technologies have been increasingly employed in the upgrading of biomass, but they are commonly limited by the trade-off between conversion and selectivity due to the short lifetime of reactive oxygen species (ROS) and uncontrollable oxidation pathways. Herein, we show that single-atom Co supported on carbon nitride enables the high-valent-oxo cobalt species (Co(IV)=O) mediated oxidation of glucose into value-added products in acetonitrile. This photocatalytic Fenton-like system achieved an overall selectivity of gluconic acid, glucaric acid, arabinose, and formic acid up to 90.3% at glucose conversion of 69.6%, outperforming most of previously reported catalytic systems. The small amount (0.72 wt%) of single-atom Co could not only elevate the optical absorption and the efficiency of photo-generated carriers separation but also induce the efficient generation of Co(IV)=O with reduced ROS to enable efficient and selective oxidation. These findings prove the great promise of high-valent metal-oxo species in biomass conversions.
The Need to Consider Regional Supply Chains and Water Usage in H2-Steel Transition
Peng Peng, Tae Lim, Fabian Rosner, Hanna Breunig, Prakash Rao, Arman Shehabi
, Available online  , doi: 10.1016/j.gee.2025.08.002
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The iron and steel industry is one of the largest contributors to U.S. and global greenhouse gas emissions. Hydrogen can act as a promising reducing agent and clean energy carrier to decarbonize this sector, and has received significant attention in terms of process modelling, techno-economic analysis, and life cycle assessment in recent years. Policy incentives, hydrogen storage and transportation, and water stress levels are key factors that require significantly more consideration in order to realize hydrogen’s potential to decarbonize this industry. This review demonstrates the need for a systematic understanding and critical assessment of these areas, and their profound impacts on the decarbonization of the iron and steel sector. Furthermore, hydrogen and water supply face competition from other hard-to-decarbonize sectors, which should be considered on national and regional levels. Lastly, future research should also consider the impact of other environmental factors and hydrogen leak when deploying hydrogen at scale for industrial decarbonization.
Selective oxidation of high-concentration 5-hydroxymethylfurfural to 2,5-furan dicarboxylic acid at room temperature in water by synergic electronic effect of bimetallic RuCo/NC catalyst
Lihua Du, Conghao Ku, Mengmeng Feng, Junjie Lan, Jeunghee Park, Ik Seon Kwon, Lingzhao Kong, Weiran Yang
, Available online  , doi: 10.1016/j.gee.2025.07.008
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Bio-based 2,5-furandicarboxylic acid (FDCA) has the potential to replace petroleum-based terephthalic acid for the synthesis of high-performance polyester materials, demonstrating broad application prospects. Its primary preparation method involves the selective oxidation of 5-hydroxymethylfurfural (HMF). However, the industrial process is limited by low HMF concentration during the reaction due to the formation of humus resulting from HMF instability especially in high concentration. In this study, a RuCo/NC bimetallic catalyst was fabricated, which can effectively catalyze the selective oxidation of HMF to obtain FDCA at room temperature (25 °C). Side reactions caused by HMF instability were significantly reduced at room temperature, allowing for the application of high-concentration HMF (10 wt%) to achieve an excellent FDCA yield of 91.92% in water. Mechanism studies reveal that a synergistic electronic effect exists between two metals that electrons transfer from Co to Ru to increase the electron density on the surface of Ru nanoparticles, improving oxygen activation ability. Meanwhile, the electron-deficient Co further enhances the adsorption of HMF on the catalyst surface for better reactivity. This study realized the high-concentration HMF aerobic oxidation to FDCA at room temperature in water, paving the way for FDCA to serve as a sustainable substitute for terephthalic acid in polyester production.
CdS-Enzyme Composite Promotes Photobiocatalytic Conversion of Plastic-derived Lactate to Chiral Chemicals
Willy W.L. See, Phuc T.T. Nguyen, Heng Yih Tan, Jie Fu Jeff Zhou, Sie Shing Wong, Kang Zhou, Ning Yan
, Available online  , doi: 10.1016/j.gee.2025.07.018
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The combination of photo- and bio-catalysis in one-pot enables sustainable, visible-light driven cascade reactions for the synthesis of value-added chiral chemicals under mild conditions. Despite the attractiveness of merging the redox capability of heterogeneous photocatalysts with the excellent enantioselectivity of enzymes, developing such reaction under one-pot conditions poses a challenge due to catalyst incompatibility. In this study, a cadmium sulfide (CdS)-enzyme composite was engineered for one-pot conversion of plastic-derived lactate into chiral compounds. By coating CdS onto alginate beads, its redox capability for the oxidation of lactate in water under visible light was preserved. The generated pyruvate subsequently underwent enantioselective transformation catalyzed by encapsulated enzymes within the beads, producing (R)-acetoin, L-alanine, or (R)-phenylacetylcarbinol. The core-shell structure of the CdS-enzyme composite protects the enzymes against radical attacks and also facilitates recycling, with 81% yield of (R)-acetoin achieved after four reaction cycles. Additionally, we demonstrated an upcycling process converting post-consumer polylactic acid cups into (R)-acetoin. This work introduces a novel approach for integrating photocatalysts and enzymes to synthesize chiral chemicals from end-of-life plastics.
Mechanistic insights into the role of N/O-doped biochar in enhanced phenolics production during biomass pyrolysis
Zihang Zhang, Honghui Li, Jinlong Liu, Jusheng Hu, Shurong Wang
, Available online  , doi: 10.1016/j.gee.2025.07.017
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Phenolic compounds are vital chemicals that can be converted into high-density jet fuel components, such as aromatic hydrocarbons or cycloalkanes. Pyrolysis of biomass waste for producing high-value phenolic compounds offers a sustainable approach to waste management and energy conversion. While N/O-doped biochar has demonstrated potential in enhancing phenolics production, its application faces challenges such as complex preparation, high activation temperatures, and unclear catalytic mechanisms. This study addresses these issues by developing a single-step sodium amide (NaNH2) activation method at mild temperatures (<500℃) to produce N/O-doped biochar with optimized catalytic properties. Characterization identified graphitic-N (-GN) and oxidized-N (-ON) configurations, along with aldehyde-O (-CHO) and carboxyl-O (-COOH) groups, as key active sites that enhance catalytic performance. Experimentally, the N/O-doped biochar achieved a phenolics yield of 57.87% at an activation temperature of 400℃, representing a 19.18% increase over non-catalytic conditions. Density functional theory (DFT) calculations further elucidated the role of N and O groups, showing that -GN and -ON in N groups and -CHO and -COOH in O groups lower energy barriers in radical-induced demethoxylation which promotes phenolic product formation. Machine learning analysis identified nucleophilicity and local softness as critical descriptors, indicating that these configurations effectively modulate electron density at active sites. These findings provide a comprehensive mechanistic understanding of how specific N and O functional groups in biochar enhance catalytic efficiency in targeted phenolic production.
Manipulating and unveiling contributions of the reactive oxygen species dramatically promote selective photo-oxidation of 5-hydroxymethylfurfural into 2,5-furandicarboxylic acid in aqueous solution
Runqing Xiao, Qingmao Yang, Yanjie Li, Wei Zhang, Gang Xiao, Chun Shen
, Available online  , doi: 10.1016/j.gee.2025.07.014
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Achieving high selectivity to 2,5-furandicarboxylic acid (FDCA) in the photocatalytic oxidation of 5-hydroxymethylfurfural (HMF) in aqueous solution advocates the principle of green and sustainable chemistry, but still remains a significant challenge. Herein, manipulating the reactive oxygen species (ROS) has been realized and dramatically promotes the selective photocatalytic oxidation of HMF in aqueous solution. High FDCA yield of 98.6% has been achieved after 3 hours of visible light irradiation over the as-prepared FeOx-Au/TiO2 catalyst, being one of the leading photocatalytic performances. Furthermore, satisfactory FDCA yields of higher than 80% could be realized even in the outdoor environment under natural sunlight irradiation, regardless of sunny or cloudy weather. A combination study including physical characterization, kinetic analysis, radical trapping experiments and density functional theory calculations unveils the rate-determining step (oxidation of hydroxyl group) and respective contributions of the generated ROS (1O2 and·O2-) in each step of the entire reaction network. The present work would push ahead the understanding of HMF photocatalytic oxidation and contribute to the rational design of high-performance photocatalysts.
Enhancing Carbonization of Microcrystalline Cellulose through Ball Milling under Decoupled Temperature and Pressure Hydrothermal Conditions
Kaile Li, Jiahui Hu, Zhiqiang Xu, Shijie Yu, Qinghai Li, Yanguo Zhang, Hui Zhou
, Available online  , doi: 10.1016/j.gee.2025.07.016
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Hydrothermal treatment of cellulose is a promising green route for bioenergy and biochemical production, yet requiring investigations of the mechanisms. In this study, the effects of cellulose crystallinity and decoupled temperature and pressure conditions on cellulose conversion and product distribution were investigated. Microcrystalline cellulose was ball-milled for varying durations, leading to a reduction in crystallinity, with 4 h of milling sufficient to achieve near-complete amorphization. Unlike concurrent recrystallization and hydrolysis observed under autogenous pressure, decoupled conditions significantly accelerated hydrolysis of cellulose. Notably, lower crystallinity cellulose exhibited significant improvements in glucose and 5-HMF yields, with 4-hour ball milling showing optimal performance among all samples. Furthermore, carbon sub-micron spheres were largely produced, which were confirmed via PTFE encapsulation experiments to primarily consist of secondary char deriving from re- polymerization and condensation reactions of the liquid phase. Overall, this study demonstrates that lower crystallinity not only facilitates hydrolysis but also accelerates the carbonization processes under decoupled pressure conditions, highlighting its potential for efficient biomass conversion into valuable products.
Advanced Batteries for Sustainable Energy Storage
Wenbin Li, Changtai Zhao, Chang Yu, Yan Yu, Jiaqi Huang, Yingying Lu, Hao Jiang, Shuai Gu, Zhouguang Lu, Xue Yang, Le Yu, Yuan Ren, Siqi Shi, Weihua Chen
, Available online  , doi: 10.1016/j.gee.2025.07.009
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The increasingly severe energy crisis and environmental issues have raised higher requirements for grid-scale energy storage system. Rechargeable batteries have enormous development prospects for their flexibility and environmental protection. However, the traditional organic liquid-based batteries cannot meet our needs for future advanced batteries in terms of safety, energy density, and stability under extreme working conditions. In this case, we comprehensively summarize various advanced battery technologies to overcome the above problems. Firstly, we highlight the advantage of solid-state batteries compared to liquid electrolytes. Specifically, we focus on the advantages and challenges of solid-state lithium/sodium batteries and other types of solid-state batteries associated with the electrodes, solid electrolytes and the electrode/electrolyte interphase. Secondly, we discuss the environmentally friendly and safe liquid-state battery and their application prospect. Thirdly, the battery improvement strategy has been proposed to enhance the application of batteries under extreme conditions. Subsequently, we emphasized the importance of theoretical calculations and AI technology in promoting the development of battery technology. Finally, the current challenges and future directions of battery technology are summarized. The combination of in-depth failure mechanism analysis, advanced characterization techniques, economic commercialization and machine learning enables the rapid development of advanced battery technology for sustainable energy storage.
Insights into degradation mechanisms and engineering strategies of layered manganese-based oxide cathodes for sodium-ion battery
Jun-Wei Yin, Yi-Meng Wu, Xin-Yu Liu, Jing Li, Peng-Fei Wang, Zong-Lin Liu, Lin-Lin Wang, Jie Shu, Ting-Feng Yi
, Available online  , doi: 10.1016/j.gee.2025.07.013
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Manganese-based oxides are widely regarded as highly promising cathode materials for sodium-ion batteries due to their abundant resources, low cost and high specific capacity. Especially in the P2 and O3-type structures, excellent electrochemical performance and structural stability are expected to be achieved by modulating the ratio of Mn to other transition metals. However, these materials are susceptible to phase transitions, Jahn-Teller distortions and manganese dissolution during cycling, which limits their structural stability and electrochemical performance. To solve these critical issues, researchers have proposed various material design and modulation strategies and achieved remarkable progress. This review provides a systematic summary of the current state of research on manganese-based oxides in sodium-ion batteries and offers a detailed analysis of the root causes of performance degradation in terms of material structural features, defect types and formation mechanisms. Meanwhile, the current research progress in ion doping, high entropy strategy, surface modification, and interfacial engineering is reviewed in order to explore the synergistic regulation on structural stability and electrochemical behavior. The unique advantages of these materials in terms of phase stability, rate capability and cycle life are demonstrated. Finally, this paper looks forward to the future research directions and development trends for manganese-based oxides, providing a theoretical foundation and technical support for the construction of high-performance and scalable cathode materials for sodium-ion batteries.
Acetone-Mediated Glucose Isomerization over a ZrO2-NC Composite Catalyst
Mi Gao, Hongquan Fu, Wenhua Zhang, Zhicheng Jiang, Bi Shi
, Available online  , doi: 10.1016/j.gee.2025.07.012
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The agglomeration-prone properties of metal oxide catalysts limit their catalytic efficiency in the isomerization of glucose to fructose. Herein, the hierarchical structure and abundant coordination groups of collagen fibers were used to anchor Zr4+, and a highly dispersed ZrO2-nitrogen-doped carbon (ZrO2-NC) composite catalyst was subsequently fabricated by calcination. For the catalytic glucose-to-fructose isomerization over ZrO2-NC, fructose was obtained in 41.3% yield and 85.3% selectivity in a water-acetone solvent at 120 ℃ for 10 min. The electron-deficient environment of ZrO2 surface during charge transfer from ZrO2-to-NC layer benefited to preferentially adsorb glucose, which accelerated glucose isomerization and fructose desorption. The amphoteric catalyst triggered both proton transfer on the Bronsted base sites and the intramolecular hydride shift of glucose on the Lewis acid sites of ZrO2-NC in the mixed solvent. The latter isomerization mechanism depended on the presence of acetone, which lowered the energy barrier and increased fructose yield.
Boosting redox kinetics in CoS/Ti3C2 heterostructure via interfacial charge redistribution for high-energy-density supercapacitors
Yu Liu, Mengjie Pan, Mengqin Gong, Huachen Lin, Yulong Ying, Longhua Li, Hong Jia
, Available online  , doi: 10.1016/j.gee.2025.07.015
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Supercapacitors are indispensable for next-generation energy storage, achieving high energy density and long-term durability remains a formidable challenge. Conventional CoS suffers from poor conductivity, while Ti3C2 faces severe restacking. Herein, we report a novel synthesis strategy that integrates metal-organic framework (MOF) growth with electrostatic self-assembly to construct heterojunction of CoS nanotubes coated with ultrathin Ti3C2 nanofilms. Material characterization via SEM, TEM, XRD, and XPS systematically confirms the heterostructure formation, and chemical composition. This rational design synergistically leverages CoS high pseudocapacitance and Ti3C2 metallic conductivity while the heterostructure mitigates restacking, enhances charge transfer, and stabilizes interfacial interactions. Density functional theory (DFT) calculations reveal strengthened OH- adsorption at the Co-Ti interface (Ead = 1.106 eV). Consequently, the CoS/Ti3C2@CC delivers a remarkable specific capacitance of 1034.21 F g-1 at 1 A g-1. Assembled into a supercapacitor, CoS/Ti3C2@CC//AC achieves a high energy density of 74.22 Wh kg-1 at 800 W kg-1, maintaining 89.13% initial capacitance after 10,000 cycles. Significantly, it exhibits a remarkably low leakage current (0.23 μA) and ultra-prolonged voltage retention (47.14% after 120 h), underscoring exceptional durability. This work pioneers a rational heterostructure engineering strategy by integrating MOF-derived architectures with conductive MXene nanofilms, offering critical insights for the development of ultradurable supercapacitor.
Harnessing tunable lignin-based carbon quantum dots for sustainable water purification
Xinyan Hou, Pengfei Zhou, Jun Guo, Shenao Yuan, Shiman Chen, Heyu Chen, Xiao Xiao, Jikun Xu, Feng Peng
, Available online  , doi: 10.1016/j.gee.2025.07.011
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Developing on-demand biomass valorization represents an ideal path to alleviate the double burden of sustainable energy-environment future, yet exploring tunable lignin-first chemistry to accomplish multifunctional water purification remains elusive. Herein, we report a versatile solvent-fractionation to construct heteroatom-doped multicolor lignin carbon quantum dots (CQDs) with the functions of bimodule pollutant sensing, metaL-ionic visualization, and photocatalytic antibiotic dissociation. With the aid of oxidation cleavage and biphasic extraction, the underlying lignin features of molecular weight and functional linkages influence the quantum size and core-surface state of CQDs conferring the unique opticaL-structure-performance. The N, S co-doped blue-emitting CQDs via light-quenching offers the selective identification of Fe3+-ions in a broad response range with acceptable limit of detection. The addition of L-cysteine can efficiently restore the fluorescence of CQDs by forming a stable Fe3+-L-cys complex. The green-emissive CQDs is facilely embedded into cellulose hydrogel to directly visualize the presence of metaL-ions. A red-CQDs modified ternary ZnIn2S4 (ZIS) composite is fabricated to achieve photocatalytic antibiotic removal with an efficiency of ~85%. The excellent photo-generated electron and storage capabilities of CQDs improve the light-capturing, electron conduction, and charge carriers separation of ZIS. The reactive species are of importance to photocatalytic tetracycline oxidation, wherein the electron holes (h+) function as the main contributor followed by ·O2-, 1O2 and ·OH. The directly interfacial electron escaping-shuttling with the help of optimized electronic and energy-band structures is confirmed via electrochemical test and theoretical computation. We anticipate that the present work not only sheds a substantial light to manipulate polychromatic lignin-based CQDs via a tailored solvent-engineering, but also presents an emerging green route of emphasizing biomass-water nexus.
Lattice sulfur-induced disordered and electron-deficient Pd-based nanosheets enabling selective electrocatalytic semi-hydrogenation of alkynes
Hongyao Luo, Haochuan Jing, Bing Zhang, Nailiang Yang, Tao Sun, Chuntian Qiu, Yangsen Xu, Peng Yang, Xiang Ling
, Available online  , doi: 10.1016/j.gee.2025.07.003
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The semi-hydrogenation of alkynes to alkenes is of great significance in industrial production of pharmaceutical and fine chemicals. Electrochemical semi-hydrogenation (ECSH) has emerged as a promising alternative to conventional thermochemical hydrogenation. However, its practical application is hindered by low reaction rate and competing hydrogen evolution reaction (HER). In this work, the controllable incorporation of sulfur into the lattice of Pd nanostructures is proposed to develop disordered and electron-deficient Pd-based nanosheets on Ni foam and enhance their ECSH performance of alkynes. Mechanistic investigations demonstrate that the electronic and geometric structures of Pd sites are optimized by lattice sulfur, which tunes the competitive adsorption of H* and alkynes, inherently inhibits the H* coupling and weakens alkene adsorption, thereby promotes the semi-hydrogenation of alkynes and prevents the over-hydrogenation of alkenes. The optimized Pd-based nanosheets exhibit efficient electrocatalytic semi-hydrogenation performance in an H-cell, achieving 97% alkene selectivity and 94% Faradaic efficiency, and a reaction rate of 303.7 μmol mg-1 catal. h-1 using 4-methoxyphenylacetylene as the model substrate. Even in a membrane electrode assembly (MEA) configuration, the optimized Pd-based nanosheets achieves a single-cycle alkyne conversion of 96% and an alkene selectivity of 97%, with continuous production of alkene at a rate of 1901.1 μmol mgcatal.-1 h-1. The potential- and time-independent selectivity, good substrate universality with excellent tolerance to active groups (C-Br/Cl/C=O, etc.) further highlight the potential of this strategy for advanced catalysts design and green chemistry.
Ultrasonic-enhanced Cu(I)/Cu(II) nanointerfaces for sustainable ozone activation in green aluminum production:atomic-level catalysis of organic waste degradation
Jianfeng Ran, Xu Sun, Jiaping Zhao, Shaoshuai Wei, Haisheng Duan, Ying Chen, Libo Zhang, Shaohua Yin
, Available online  , doi: 10.1016/j.gee.2025.07.007
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The accumulation of refractory organics in Bayer liquor (pH 14.4) critically compromises aluminum production efficiency and product quality, necessitating sustainable remediation strategies. Herein, we develop an ultrasonic-driven catalytic ozonation system with dynamically reconstructed CuO/Cu2O heterointerfaces, achieving unprecedented efficiency in extreme alkaline wastewater treatment. Atomic-scale interface engineering endows the catalyst with hydrophilicity (contact angle:6.1°) and 3.8-4.3 times higher oxygen vacancy density compared to single-phase catalysts. These properties facilitate efficient interfacial interactions with Bayer liquor and enable superior ozone activation through synergistic Cu(I)/Cu(II) redox cycling across the heterointerface. This interfacial synergy reduces ozone adsorption energy from 5.46 eV (Cu2O) to 1.48 eV, driving reactive oxygen species (ROS) generation via low-energy pathways. Under optimized conditions, the system achieves 57.82% TOC removal within 1.5 h with 2.3-fold faster kinetics than ozone- alone processes, while improving energy efficiency by 1.82-3.22 times per kWh over conventional thermal oxidation. Remarkable stability is demonstrated through 80.21% activity retention after 6 cycles, attributed to surface energy minimization (0.61 J/m2), alongside 67.91% hydroxyl radical (·OH)-mediated degradation confirmed by quenching tests. In XPS, EEMs analysis, and ECOSAR modeling further elucidate the surface reconstruction mechanism and intermediate toxicity reduction. This work establishes an atomic interface design paradigm that bridges catalytic innovation with green metallurgy applications, offering a sustainable solution for industrial wastewater remediation aligned with circular economy principles.
Grafting Sulfonated Triptycene-Based Hypercrosslinked Polymers onto Bi2WO6 for Enhanced Adsorption and Photoelimination of Antibiotics
Yingxue Zhang, Wanjun Xu, Xiao Yang, Shihong Dong, Najun Li, Qingfeng Xu, Hua Li, Jianmei Lu, Dongyun Chen
, Available online  , doi: 10.1016/j.gee.2025.07.004
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Antibiotics, as an emerging pollutant due to their extensive use and difficulty in biodegradation, can cause harm to health through bioaccumulation. To address this, various photocatalysts have been developed for rapid antibiotic removal. However, their low concentrations limit mass transfer efficiency, resulting in suboptimal performance. Adsorption is crucial for enhancing photocatalytic efficiency. In this study, a series of binary heterojunction catalysts (x% BWO@STHP) were synthesized, consisting of Bi2WO6 (BWO) grafted with sulfonated triptycene-based hypercrosslinked polymer (STHP). The high specific surface area of STHP, combined with π-π conjugation and ionic interactions with antibiotics, significantly enhances adsorption capacity. This facilitates effective contact between low-concentration pollutants in aqueous solutions and the active sites of the catalyst. The formation of a Z-scheme heterojunction between BWO and STHP facilitates photogenerated charge separation, and further significantly improves photocatalytic degradation performance. Specifically, the 20% BWO@STHP catalyst achieved rapid adsorption equilibrium for oxytetracycline (OTC), doxycycline (DOX), and tetracycline (TC) within 2 min and completely degraded them after 15 min of irradiation, compared to pristine BWO, the photocatalytic reaction rate constants are significantly increased, being 9.69 times higher for OTC and 13.45 times higher for DOX. The catalyst exhibits excellent reusability and holds promising potential for practical applications.
Cu doping induced lattice distortion and oxygen vacancy formation in PbBiO2Br:Band structure modulation enhances photocatalytic nitrogen fixation and pollutant degradation performance
Shude Yuan, Yekang Zheng, Yuxin Chu, Chuanqi Xia, Ruoyu Dong, Jiating Xu, Botao Teng, Ying Wu, Yiming He
, Available online  , doi: 10.1016/j.gee.2025.07.005
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Photocatalytic nitrogen fixation has emerged as a sustainable alternative for ammonia synthesis, playing a crucial role in alleviating energy shortages and environmental pollution. In this study, PbBiO2Br was applied to photocatalytic nitrogen fixation for the first time, and its photocatalytic performance was effectively enhanced through Cu doping. The catalyst was synthesized via a simple reduction method, and its morphology, structure, and physicochemical properties were systematically investigated using various characterization techniques and density functional theory calculations. The results revealed that the incorporation of Cu2+ partially replaced Pb2+, inducing lattice distortion in PbBiO2Br, promoting the formation of oxygen vacancies, and modifying its electronic band structure. Specifically, Cu doping led to a slight bandgap narrowing, a reduction in work function, and a significant upward shift in the conduction band position. These changes enhanced light absorption, facilitated charge carrier migration and separation, and improved the reduction ability of photogenerated electrons. Moreover, Cu doping promoted N2 adsorption and activation. Consequently, the photocatalytic nitrogen fixation performance of Cu- doped PbBiO2Br was significantly enhanced, achieving an optimal nitrogen fixation rate of 293 μmol L-1 g-1 h-1, which is 3.6 times higher than that of pristine PbBiO2Br. Additionally, Cu- PbBiO2Br also showed good activity in the photocatalytic degradation of RhB, with a degradation rate 4.6 times higher than that of PbBiO2Br. This work offers new insights into the application of PbBiO2Br in photocatalytic nitrogen fixation and offers valuable guidance for the development of highly efficient nitrogen fixation materials in the future.
Interpretable machine learning analysis on CO2 adsorption and separation capacity of biochar under multi-scenario conditions
Jialiang Dong, Ruikun Wang, Yulong Xie, Fuyan Gao, ShiTeng Tan, Zhenghui Zhao, Qianqian Yin, Eric J. Hu
, Available online  , doi: 10.1016/j.gee.2025.07.001
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Biochar has been widely recognized as a promising solid CO2 adsorbent with economic and ecological benefits. Industrial CO2 emissions originate from diverse sources, while the pore structure and chemical functional groups of biochar exhibit varying degrees of influence on CO2 adsorption and separation performance under different adsorption conditions. Therefore, exploring the matching relationship between the physicochemical properties of biochar and its adsorption and separation performance at different adsorption conditions is essential for the development and optimization of carbon-based adsorbents. This study selected the high-performance extreme gradient boosting (XGB) algorithm from various algorithms and utilized it to develop CO2, N2, CH4 adsorption prediction models. Based on this, coupled prediction models were developed for CO2/N2 and CO2/CH4 adsorption selectivity. Furthermore, feature importance and partial dependence analysis were performed using SHAP values. The results indicate that during CO2 adsorption, the influence of the pore structure of biochar outweighs that of its chemical composition. Specifically, the pore structure of 0.4-0.6 nm is the most important property influencing CO2 adsorption at low and medium pressure (0-0.6 bar), and the pore structure of 0.6-0.8 nm, as well as the specific surface area contribute the most at high pressure (0.6-1 bar). During CO2 selective separation, the CO2/N2 mixture is primarily separated through the selective adsorption of CO2 by nitrogen functional groups. In contrast, for CO2/CH4 mixtures, pore structure <1 nm plays a more critical role in determining adsorption selectivity. In addition, molecular simulation studies further revealed the adsorption filling mechanisms of CO2 molecules within different pore sizes and functional groups. Finally, nitrogen-doped biochar was synthesized using de-alkalize lignin as the precursor, KOH as the activating agent, and urea as the nitrogen dopant. CO2, N2, and CH4 isothermal adsorption experiments were conducted, and the experimental results confirmed that the developed prediction models exhibit high accuracy (R2>0.9).
Efficient Electro-Catalytic Desulfurization by In-Situ Oxidant Generation
Yang Cao, Shilong Zhou, Linlin Chen, Yan Huang, Hui Liu, Yiru Zou, Peiwen Wu, Haiyan Ji, Wenshuai Zhu, Chunming Xu
, Available online  , doi: 10.1016/j.gee.2025.07.002
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In this study, we present an extraction-coupled electro-catalytic oxidative desulfurization (EC-EODS) system that achieves efficient sulfur removal from fuel oils without external oxidants. The system utilizes an electrolyte composed of ionic liquids (ILs), NaCl, and H2SO4, integrating extraction and electrochemical oxidation to effectively remove different aromatic sulfur compounds with sulfur removals of 100%. Additionally, H2 is co-produced at the cathode, supporting refinery processes and reducing H2 storage and transportation costs, thereby improving economic viability. Detailed mechanism analysis shows that IL selectively extracts and concentrates sulfur compounds, while NaCl and H2SO4 facilitate ClO- generation, serving as the in-situ oxidant. The EC-EODS system operates without external catalysts, relying on graphite electrodes that generate superoxide radicals from ClO-. Moreover, a strategy for the separation of desulfurization products as well as the electrolyte is proposed as well. The EC-EODS system offers a sustainable, high-efficiency strategy for desulfurization, with economic benefits through sulfur oxidation and H2 co-generation.
Recent progress in biochar-based photocatalysts for environmental remediation
Ke Zhu, Yuheng Yao, Xiaoying Liang, Yi Yang, Hector F. Garces, Kai Yan
, Available online  , doi: 10.1016/j.gee.2025.07.006
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With the accelerating industrialization, environmental pollution has become increasingly severe. Photocatalysis, as a solar-driven advanced oxidation process, has emerged as a promising solution for environmental remediation. Biochar, with its unique surface properties, tunable functional groups, excellent conductivity, and chemical stability, serves as an ideal support for photocatalysts. The integration of photocatalysts with biochar forms biochar-based photocatalysts (Bio-BPs), which synergistically enhance functional groups, porosity, surface active sites, and catalytic performance. This review systematically summarizes the synthesis methods of Bio-BPs to guide optimal preparation strategies, enumerates the advanced characterization techniques, explores modification mechanisms and their effects on photocatalytic activity, examines applications in removing both aqueous pollutants and atmospheric pollutants and discusses sustainable prospects for the future development of Bio-BPs to provide guidelines for designing high-performance biochar-based materials for practical environmental applications.
Advances in Cathode's Microstructure Modification to Boost Performance of Lithium-Sulfur Batteries
Modeste Venin Mendieev Nitou, Wu Yu, Waqas Muhammad, Ziheng Zhang, Daiqian Chen, Hesheng Yu, Mengjun Tang, Xiaodong Fang, Rui Liu, Yashuai Pang, Aadheeshwaran Samynathan, Benammar Djenet Sondra, Yinghua Niu, Weiqiang Lv, Yuanfu Chen
, Available online  , doi: 10.1016/j.gee.2025.06.006
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Lithium-sulfur (Li-S) battery becomes one of the most promising next-generation energy storage devices due to its ultrahigh energy density of 2600 Wh/kg. However, their commercialization is impeded by several critical challenges, including the polysulfide shuttle effect, low electrical conductivity of sulfur, and significant volume expansion during cycling. This review addresses recent developments in the microstructural innovations aimed at improving lithium-sulfur (Li-S) battery performance, with a particular focus on the modification of cathode materials. The strategies discussed primarily revolve around enhancing the conductivity of sulfur and effectively confining polysulfides to reduce the dissolution of lithium polysulfides in organic electrolytes. Key findings highlight the effectiveness of porous carbon structures, and metal compounds in stabilizing polysulfides and enhancing electrochemical performances. Additionally, the roles of advanced synthesis techniques that facilitate the creation of hybrid cathodes with superior mechanical properties and cycling stability are summarized. By addressing the inherent limitations of traditional Li-S battery designs, these innovations pave the way for more efficient and reliable energy storage systems, positioning Li-S technology as a viable alternative to conventional lithium-ion batteries in future applications.
Highly selective electrocatalytic CO2 reduction to liquid C2 products by means of a tandem catalytic system
Nan Wang, Yuan Zhang, Xiaoxin Tian, Mingming Sun, Lei Yuan, Huiyong Wang, Jianji Wang
, Available online  , doi: 10.1016/j.gee.2025.06.007
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Electrocatalytic CO2 reduction for the synthesis of high value-added multi-carbon (C2+) products is a promising strategy to achieve energy storage and carbon neutrality, However, to acquire high selectivity of C2+ products remains a challenge. Herein, Ag NCs@Ag-MOF with highly dispersed Ag nanoclusters (NCs) and Cu-O2N2-COF with Cu-O2N2 active sites were designed, synthesized and then coupled for the conversion of CO2 to liquid C2 products (ethanol and acetate). Faradaic efficiency (FE) of the liquid C2 products was 90.9% at -0.98 V (vs. RHE), which is 1.9 times that of Cu-O2N2-COF in direct CO2 electroreduction and the highest liquid C2 products selectivity reported so far. The current density reached 324.8 mA cm-2 at -1.2 V (vs. RHE). In situ infrared spectroscopy and density functional theory calculations showed that the tandem catalytic system significantly enhanced the accumulation of *CO on the catalyst and promoted *CO-*CO coupling, thus significantly improving the selectivity of liquid C2 products.
Cutting-edge aminated conjugated microporous poly(aniline)s enabled highperformance membrane for seawater uranium extraction
Xiaoxia Ye, Bingqing Huang, Xueying Chen, Yaping Wang, Zhihong Zheng, Yifan Liu, Yuancai Lv, Chunxiang Lin, Jian Huang, Jie Chen
, Available online  , doi: 10.1016/j.gee.2025.06.005
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The extraction of uranium from seawater via membrane adsorption is a promising strategy for ensuring a long-term supply of uranium and the sustainability of nuclear energy. However, this approach has been hindered by the longstanding challenge of identifying sustainable membrane materials. In response, we propose a prototypal hybridization strategy to design a novel series of conjugated microporous polymer (CMPO)@collagen fiber membrane (COLM), as decorated with multiple functional groups through an amination. These sustainable and low-cost membrane materials allow a rapid and high-affinity kinetic to capture 90% of the uranium in just 30 min from 50 ppm with a high selectivity of Kd > 105 mL·g-1. They also afford a robustly reusable adsorption capacity as high as 345 mg·g-1 that could harvest 1.61 mg·g-1 of uranium in a short 7-day real marine engineering in Fujian Province, even though suffered from very low uranium concentration of 3.29 µg·L-1 and tough influence of salts such as 10.77 g·L-1 of Na+, 1.75 µg·L-1of VO3-etc in the rough seas. The structural evidence from both experimental and theoretical studies confirmed the formation of favorable chelating motifs from the amino group on CMPN, and the intensification by the synergistic effect from the size-sieving action of CMPN and the capillary inflow effect of COLM.
Enhanced hydroxide conductivity in zwitterionic polyacrylate-based anion exchange membranes via side-chain length optimization
Lu Cai, Naibing Li, Bingbing Li, Tianchi Zhou, Zhengyuan Zhou, Yongnan Zhou, Xi Luo, Kaiying Zhao, Yuekun Lai, Jinli Qiao
, Available online  , doi: 10.1016/j.gee.2025.06.003
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Developing advanced ion-conductive networks is crucial for anion exchange membranes (AEMs). A flexible molecular structure facilitates the formation of ion clusters and results in enhanced ionic conductivity. Polyacrylates, known for their outstanding flexibility and chemical stability, hold significant potential as polymer electrolyte membranes. In this work, we innovatively constructed a series of polyacrylate-based AEMs decorated with pendant zwitterions (designated as PSBPA-X, BSBPA-X, where X=20, 30, 40). Specifically, the spacer length between the zwitterions is strategically optimized to enhance the ionic conductivity. Atomic force microscopy reveals that a longer spacer length between the zwitterions promotes the microphase separation and the formation of advanced water channels, which facilitates the OH- transport in the BSBPA-40 membrane. Moreover, the stronger electrostatic potential and lower interaction energy between the BSBPA-40 and OH- further contributes to efficient OH- hopping transmission. Consequently, the BSBPA-40 membrane demonstrates the highest OH- conductivity, achieving 102.1 mS/cm at 80 °C and 90% relative humidity, significantly surpassing that of the PSBPA-40 membrane (75.2 mS/cm). Additionally, the BSBPA-40 membrane exhibits remarkable flexibility with an improved breaking elongation of 480.5% due to the ionic cross-linking between the zwitterions. Notably, the BSBPA-40 membrane-based zinc-air battery achieves an outstanding power density of 156.7 mW/cm2 at room temperature, while its water electrolysis performance reaches 2.1 A/cm2 at 2.0 V. These results indicate that the developed membranes hold great promise for applications in sustainable and clean energy technologies.
Single-atom Mn-modified Biomimetic Phthalocyanine Covalent Organic Frameworks with Tunable Pendant Groups for High-efficiency Sodium Chloride Batteries
Jiajun Cui, Zhenzhen Wang, Yongqiang Gu, Ting Xu, Tairan Pang, Chuanling Si, Weiwei Huan, Jie Li
, Available online  , doi: 10.1016/j.gee.2025.06.002
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Rechargeable chlorine-based battery recently emerged as a promising substitute for energy storage systems due to their high average operating voltage (∼3.7 V) and large theoretical capacity of ∼754.9 mAh g-1. However, insufficient supply of chlorine (Cl2) and sluggish oxidation of NaCl to Cl2 limit its practical application. Covalent Organic Frameworks (COFs) have the potential to be ideal Cl2 host materials as Cl2 adsorbents for their abundant porosity and easily modifiable nature. In this work, the single atom Mn coordinated biomimetic phthalocyanine COFs is used for Cl2 capture and catalyst. The DFT reveals that ASMn and -NH2 significantly change the microenvironment around the active site, effectively promote the oxidation of NaCl. When applied as the cathode material for Na-Cl2 batteries, the SAMn-COFs-NH2 electrode exhibits large reversible capacities and excellent high-rate cycling performances throughout 200 cycles based on the mechanism of highly reversible NaCl/Cl2 redox reactions. Even at the temperature as low as -40 oC, the SAMn-COFs-NH2 cathode showed stable discharge capacities at ∼1000 mAh g-1 over 50 cycles with a voltage plateau of ∼3.3 V. This work may provide new insights for the investigation of chlorine-based electrochemical redox mechanisms and the design of green nanoscaled electrodes for high-property chlorine-based batteries.
Converting waste polyimide into porous carbon nanofiber for all-weather freshwater and hydroelectricity generation
Lijie Liu, Huajian Liu, Huiyue Wang, Kuankuan Liu, Guixin Hu, Yan She, Xueying Wen, Hangyuan Du, Lingling Feng, Jiang Gong
, Available online  , doi: 10.1016/j.gee.2025.06.004
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The dual system capable of solar-driven interfacial steam production and all-weather hydropower generation is emerging as a potential way to alleviate freshwater shortage and energy crisis. However, the intrinsic mechanism of hydroelectric electricity generation powered by the interaction between seawater and material structure is vague, and it remains challenging to develop dual-functional evaporators with high photothermal conversion efficiency and ionic selectivity. Herein, an all-weather dual-function evaporator based on porous carbon fiber-like (PCF) is acquired through the pyrolysis of barium-based metal-organic framework (Ba-BTEC), which is originated from waste polyimide. The PCF-based evaporator/device exhibits a high steam generation rate of 2.93 kg m-2 h-1 in seawater under 1 kW m-2 irradiation, along with the notable open-circuit voltage of 0.32 V, owing to the good light absorption ability, optimal wettability, and suitable aperture size. Moreover, molecular dynamics simulation result reveals that Na+ tends to migrate rapidly within the nanoporous channels of PCF, owing to a strong affinity between oxygen-containing functional group and water molecule. This work not only proposes an eco-friendly strategy for constructing low-cost full-time freshwater-hydroelectric co-generation device, but also contributes to the understanding of evaporation-driven energy harvesting technology.
Enhancing C-N bond formation in amine carbonylation through dual hydrogen bonding catalysis under mild reaction conditions
Xiang Hui, Jianhui Shi, Jiajun Zhang, Yan Cao, Huiquan Li, Peng He, Liguo Wang
, Available online  , doi: 10.1016/j.gee.2025.05.010
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The carbonylation of amines offers a promising route for synthesizing N-substituted carbamates with high atom economy. However, conventional catalysts exhibit limited catalytic efficiency, and the underlying proton transfer mechanism remains elusive. Herein, we reported a metal-free, roomtemperature strategy utilizing 1,5,7-triazabicyclo[4.4.0]dec-5-ene (TBD) as a dual hydrogen bond catalyst to synergistically activate propylamine (PA) and dimethyl carbonate (DMC). This green catalytic system achieves a 10-fold acceleration in reaction rate compared to other hydrogen bonding catalysts under mild conditions. This is enabled by dual hydrogen bonding of TBD with PA and DMC, which facilitates rapid proton transfer and stabilizes tetrahedral intermediates. Theoretical calculations confirm that the dual hydrogen bond system significantly lowers activation energy compared to single hydrogen bond analogs. Furthermore, it was revealed that the hydrogen bonding network within the product is the primary factor responsible for the sluggish reaction rate. This study demonstrates the effectiveness of a dual hydrogen bond system in accelerating the carbonylation of amines and provides a green route to access carbamates.
Advancing Battery Safety System: Introducing Eutectic Hydrated Salt Composite Phase Change Materials with Two Stage Thermal Storage Properties
Wensheng Yang, Zhubin Yao, Xiaoyu Zhou, Xinxi Li, Ya Mao, Wei Jia, Yuhang Wu, Weifu Xu, Rui Liang, Xiaozhou Liu, Lifan Yuan, Zhizhou Tan, Canbing Li
, Available online  , doi: 10.1016/j.gee.2025.05.011
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To address the challenge of balancing thermal management and thermal runaway mitigation, it is crucial to explore effective methods for enhancing the safety of lithiumion battery systems. Herein, an innovative hydrated salt composite phase change material (HSCPCM) with dual phase transition temperature zones has been proposed. This HSCPCM, denoted as SDMA10, combines hydrophilic modified expanded graphite, an acrylic emulsion coating, and eutectic hydrated salts to achieve leakage prevention, enhanced thermal stability, cycling stability, and superior phase change behavior. Battery modules incorporating SDMA10 demonstrate significant thermal control capabilities. Specifically, the cylindrical battery modules with SDMA10 can maintain maximum operating temperatures below 55 °C at 4 C discharge rate, while prismatic battery modules can keep maximum operating temperatures below 65 °C at 2 C discharge rate. In extreme battery overheating conditions simulated using heating plates, SDMA10 effectively suppresses thermal propagation. Even when the central heating plate reaches 300 °C, the maximum temperature at the module edge heating plates remains below 85 °C. Further, compared to organic composite phase change materials (CPCMs), the battery module with SDMA10 can further reduce the peak thermal runaway temperature by 93 °C and delay the thermal runaway trigger time by 689 s, thereby significantly decreasing heat diffusion. Therefore, the designed HSCPCM integrates excellent latent heat storage and thermochemical storage capabilities, providing high thermal energy storage density within the thermal management and thermal runaway threshold temperature range. This research will offer a promising pathway for improving the thermal safety performance of battery packs in electric vehicle and other energy storage systems.
Bio-Inspired Amino Acid Promoted Nanofluidic Ion Transport and Energy Conversion in Free-Standing Layered Vermiculite-based Membranes
Ruohan Feng, Chaoran Zhang, Di Zhang, Fang Song
, Available online  , doi: 10.1016/j.gee.2025.05.009
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Two-dimensional nanofluidic membranes have garnered considerable interest due to their potential for cost-effective osmotic energy harvesting. One promising approach to enhancing ion conductivity and selectivity is the incorporation of guest additives. However, the traditional host-guest configuration can undermine the structural integrity of nanochannels owing to the inconsistent size and shape of these additives. Drawing inspiration from the intricate design of biological protein channels, which utilize small amino acid molecules as guests, we have addressed this issue by incorporating glycine, a common amino acid, into a vermiculite membrane using a simple vacuum-assisted infiltration method. The resulting vermiculite-glycine membrane demonstrates 1.8 times greater ionic conductivity and twice the power density compared to pure vermiculite membranes. Analysis based on glycine content, coupled with spectroscopic examination, reveals that ion conductivity is linked to the distribution of glycine molecules across three specific sites within the membrane. This suggests that glycine molecules—whether confined in voids, adsorbed onto nanochannel surfaces, or intercalated within multilayered vermiculite nanoparticles—enhance nanofluidic ion transport by modulating surface and space charge density, as well as strengthening hydrogen bonding, electrostatic interactions, and steric effects. This work reveals the specific interactions between amino acids and vermiculite, offering a novel path for advancing nanofluidic composite membranes and highlighting critical considerations for the proposed strategy.
Multi-scale Nanofiber Filter-based TENG for Sustainable Enhanced PM0.3 Filtration and Self-powered Respiratory Monitoring
Mengtong Yi, Nan Lu, Yukui Gou, Pinmei Yan, Hong Liu, Xiaoqing Gao, Jianying Huang, Weilong Cai, Yuekun Lai
, Available online  , doi: 10.1016/j.gee.2025.05.001
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Advanced healthcare monitors for air pollution applications pose a significant challenge in achieving a balance between high-performance filtration and multifunctional smart integration. Electrospinning triboelectric nanogenerators (TENG) provide a significant potential for use under such difficult circumstances. We have successfully constructed a high-performance TENG utilizing a novel multi-scale nanofiber architecture. Nylon 66 (PA66) and chitosan quaternary ammonium salt (HACC) composites were prepared by electrospinning, and PA66/H multiscale nanofiber membranes composed of nanofibers (≈ 73 nm) and submicron-fibers (≈ 123 nm) were formed. PA66/H multi-scale nanofiber membrane as the positive electrode and negative electrode-spun PVDF-HFP nanofiber membrane composed of respiration- driven PVDF-HFP@PA66/H TENG. The resulting PVDF-HFP@PA66/H TENG based air filter utilizes electrostatic adsorption and physical interception mechanisms, achieving PM0.3 filtration efficiency over 99% with a pressure drop of only 48 Pa.Besides PVDF-HFP@PA66/H TENG exhibits excellent stability in high-humidity environments, with filtration efficiency reduced by less than 1%. At the same time, the TENG achieves periodic contact separation through breathing drive to achieve self- power, which can ensure the long-term stability of the filtration efficiency. In addition to the air filtration function, TENG can also monitor health in real time by capturing human breathing signals without external power supply. This integrated system combines high-efficiency air filtration, self-powered operation, and health monitoring, presenting an innovative solution for air purification, smart protective equipment, and portable health monitoring. These findings highlight the potential of this technology for diverse applications, offering a promising direction for advancing multifunctional air filtration systems.
Optimizing CO production in electrocatalytic CO2 Reduction via electron accumulation at Ni Sites in Ni3ZnC0.7/Ni on N-doped carbon nanofibers
Ge Bai, Min Wang, Luwei Peng, Lulu Li, Yadan Yu, Wenyi Li, Nianjun Yang, Daniil I. Kolokolove, Jinli Qiao
, Available online  , doi: 10.1016/j.gee.2025.04.010
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The electrocatalytic reduction of carbon dioxide (CO2RR) to valuable products presents a promising solution for addressing global warming and enhancing renewable energy storage. Herein, we construct a novel Ni3ZnC0.7/Ni heterostructure electrocatalyst, using an electrospinning strategy to prepare metal particles uniformly loaded on nitrogen-doped carbon nanofibers (CNFs). The incorporation of zinc (Zn) into nickel (Ni) catalysts optimizes the adsorption of CO2 intermediates, balancing the strong binding affinity of Ni with the comparatively weaker affinity of Zn, which mitigates over-activation. The electron transfer within the Ni3ZnC0.7/Ni@CNFs system facilitates rapid electron transfer to CO2, resulting in great performance with a faradaic efficiency for CO (FECO) of nearly 90% at -0.86 V vs. the reversible hydrogen electrode (RHE) and a current density of 17.51 mA cm-2 at -1.16 V vs. RHE in an H-cell. Furthermore, the catalyst exhibits remarkable stability, maintaining its crystal structure and morphology after 50 hours of electrolysis. Moreover, the Ni3ZnC0.7/Ni@CNFs is used in the membrane electrode assembly reactor (MEA), which can achieve a FECO of 91.7% at a cell voltage of -3 V and a current density of 200 mA cm-2 at -3.9 V, demonstrating its potential for practical applications in CO2 reduction.
Robust Ambient-Stable 2D Heterostructure of Copper Oxides Intercalating Black Phosphorus for Flame Retardancy and Catalytic Removal of Carbon Monoxide
Xiaoyang Yu, Huan Li, Xuyang Miao, Ning Kang, Wenbin Yao, Mingjun Xu
, Available online  , doi: 10.1016/j.gee.2025.04.009
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Two-dimensional black phosphorus (2D BP) utilized in flame retardant applications frequently encounters significant challenges, including inadequate ambient stability and elevated carbon monoxide (CO) release rates. To mitigate these issues, an effective approach was proposed for the fabrication of 2D heterostructures comprising copper oxide intercalated with BP in this work. This methodology takes into account both thermodynamic and kinetic factors, resulting in substantial enhancements in the ambient stability of BP and the catalytic performance for CO elimination, achieved through the synergistic interactions between 2D BP and copper oxide, all while preserving the structural integrity of 2D BP. The incorporation of gelatin and kosmotropic anions facilitated the efficient adhesion of the multifunctional heterostructures to the flammable flexible polyurethane foam (FPUF), which not only scavenged free radicals in the gas phase but also catalyzed the formation of a dense carbon layer in the condensed phase. Kosmotropic anions induce a salting-out effect that fosters the development of a chain bundle, a hydrophobic interaction domain, and a potential microphase separation region within the gelatin chains, leading to a marked improvement in the mechanical strength of the heterostructure coatings. The modified FPUF exhibited a high limiting oxygen index (LOI) value of 34%, alongside significantly improved flame resistance: the peak CO release rate was reduced by 78%, the peak heat release rate decreased by 57%, and the fire performance index (FPI) was increased by 40 times compared to untreated FPUF. The 2D heterostructure coatings demonstrated better CO catalytic removal performance relative to previously reported flame retardant products. This research offers a promising design principle for the development of next-generation high-performance flame retardant coatings aimed at enhancing fire protection.
Construction of Hollow Porous Lychee-structured Ni/C/ZnFe2O4 MicrowaveResponsive Catalysts with Rapid Efficiently Reduction of Cr(VI) ions
Gaoqian Yuan, Ling Zhang, Jingzhe Zhang, Long Dong, Xuefeng Liu, Yage Li, Liang Huang, Faliang Li, Haijun Zhang
, Available online  , doi: 10.1016/j.gee.2025.04.008
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Designing catalyst with high reactive efficiency is essential for the reduction of heavy metal Cr(VI) ions in wastewater via microwave induction. In this paper, a unique microwave-responsive lychee-like Ni/C/ZnFe2O4 composite catalyst with double-shell hollow porous heterojunction structure was constructed for the efficient reduction of Cr(VI). Benefiting from the novel hollow porous structure and "carbon nanocage" structure of the Ni/C/ZnFe2O4, coupled with excellent electromagnetic wave absorption ability, the prepared lychee-like Ni/C/ZnFe2O4 composite catalyst could remove up to 98% of Cr(VI) (50 mg/L, 50 mL) after 40 mins of microwave irradiation, even in nearly neutral water conditions. Additionally, density functional theory calculations indicated that the heterojunction interface between Ni/C and ZnFe2O4 enhances electron transfer from ZnFe2O4 to Ni/C, ultimately facilitating the removal of Cr(VI). Furthermore, the incorporation of Ni/C facilitated the acceleration of H ion transfer to *Cr2O72-, thereby expediting the conversion kinetics of the atter. This research aims to establish a theoretical and experimental foundation for the effective and stable microwave-assisted catalytic reduction of heavy metal Cr(VI) ions, presenting new insights and methods to combat heavy metal contamination.
Constructing S-scheme 3D Zn3In2S6/ReS2 heterojunction photocatalyst for simultaneous organic pollutants degradation and hydrogen production
Qi Gao, Tiantian Wang, Liangmeng Ni, Zhenrui Li, Xia Du, Shaowen Rong, Hui Wang, Liquan Jing, Zhijia Liu, Jinguang Hu
, Available online  , doi: 10.1016/j.gee.2025.04.007
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Controlling efficient interfacial charge transfer is crucial for developing advanced photocatalysts. This study successfully developed a bifunctional photocatalyst with an S-scheme heterojunction by incorporating ReS2 into the Zn3In2S6 (ZIS) nanoflower structure, enabling the organic pollutants degradation and synergistic hydrogen production. The optimized ZIS/ReS2-1% exhibited exceptional photocatalytic efficiency, reaching a 97.7% degradation rate of ibuprofen (IBP) within 2 h, along with a hydrogen generation rate of 1.84 mmol/g/h. The degradation efficiency and hydrogen generation rate were 1.78 and 5.75 times greater than that of Zn3In2S6, respectively. Moreover, ZIS/ReS2-1% demonstrated excellent catalytic degradation abilities for various organic pollutants such as ciprofloxacin, amoxicillin, norfloxacin, levofloxacin, ofloxacin, sulfamethoxazole, and tetracycline, while also showing good synergistic hydrogen production efficiency. Electron spin resonance and radical scavenging experiments verified that h+, ·O2-, and ·OH were the primary reactive species responsible for IBP degradation. The superior photocatalytic performance of the ZIS/ReS2-1% was mainly attributed to its broad and intense absorption of visible light, effective separation of charge carriers, and enhanced redox capabilities. The degradation pathway of IBP was unveiled through Fukui function and liquid chromatography-mass spectrometry, and the toxicity of the degradation intermediates was also examined. In-situ XPS and density functional theory (DFT) calculations confirmed the existence of S-scheme heterojunction. This study provided a new pathway for simultaneously achieving organic pollutant treatment and energy conversion.
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.
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.
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.
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.
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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