2024 Vol. 9, No. 8

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Accelerating the practical application of MOFs for hydrogen storage—from performance-driven to application-oriented
Yifan Wang, Jinghui Wu, Yidi Gao, Keqing Li, Chi Wang, Xiaochun Cui, Mingxin Huo, Xianze Wang
2024, 9(8): 1193-1198. doi: 10.1016/j.gee.2024.03.007
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Metal–organic frameworks (MOFs) are highly promising porous materials known for their exceptional porosity, extensive surface area, and customizable pore structures, making them an ideal solution for hydrogen storage. However, most MOFs research remains confined to the laboratory, lacking practical applications. To address this, the author proposes a shift towards practical applications, the creation of a comprehensive MOFs database, alignment of synthesis with practical considerations, and diversification of MOFs applications. These steps are crucial for harnessing the full potential of MOFs in real-world energy challenges.
Review articles
Micro-nano-fabrication of green functional materials by multiphase microfluidics for environmental and energy applications
Cheng Qi, Tao Zhou, Xingjiang Wu, Kailang Liu, Lei Li, Zhou Liu, Zhuo Chen, Jianhong Xu, Tiantian Kong
2024, 9(8): 1199-1219. doi: 10.1016/j.gee.2023.05.012
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Multiphase microfluidic has emerged as a powerful platform to produce novel materials with tailor-designed functionalities, as microfluidic fabrication provides precise controls over the size, component, and structure of resultant materials. Recently, functional materials with well-defined micro-/nanostructures fabricated by microfluidics find important applications as environmental and energy materials. This review first illustrated in detail how different structures or shapes of droplet and jet templates are formed by typical configurations of microfluidic channel networks and multiphase flow systems. Subsequently, recent progresses on several representative energy and environmental applications, such as water purification, water collecting and energy storage, were overviewed. Finally, it is envisioned that integrating microfluidics and other novel materials will play increasing important role in contributing environmental remediation and energy storage in near future.
Indispensable gutter layers in thin-film composite membranes for carbon capture
Gengyi Zhang, Haiqing Lin
2024, 9(8): 1220-1238. doi: 10.1016/j.gee.2023.08.001
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Industrial thin-film composite (TFC) membranes achieve superior gas separation properties from high-performance selective layer materials, while the success of membrane technology relies on high-performance gutter layers to achieve production scalability and low-cost manufacturing. However, the current literature predominantly focuses on the design of polymer architectures to obtain high permeability and selectivity, while the art of fabricating gutter layers is usually safeguarded by industrial manufacturers and appears lackluster to academic researchers. This is the first report aiming to provide a comprehensive and critical review of state-of-the-art gutter layer materials and their design and modification to enable TFC membranes with superior separation performance. We first elucidate the importance of the gutter layer on membrane performance through modeling and experimental results. Then various gutter layer materials used to obtain high-performance composite membranes are critically reviewed, and the strategies to improve their compatibility with the selective layer are highlighted, such as oxygen plasma treatment, polydopamine deposition, and surface grafting. Finally, we present the opportunities of the gutter layer design for practical applications.
Ordered mesoporous materials for water pollution treatment: Adsorption and catalysis
Peng Zhang, Mingming He, Wei Teng, Fukuan Li, Xinyuan Qiu, Kexun Li, Hao Wang
2024, 9(8): 1239-1256. doi: 10.1016/j.gee.2023.11.001
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To meet the growing emission of water contaminants, the development of new materials that enhance the efficiency of the water treatment system is urgent. Ordered mesoporous materials provide opportunities in environmental processing applications due to their exceptionally high surface areas, large pore sizes, and enough pore volumes. These properties might enhance the performance of materials concerning adsorption/catalysis capability, durability, and stability. In this review, we enumerate the ordered mesoporous materials as adsorbents/catalysts and their modifications in water pollution treatment from the past decade, including heavy metals (Hg2+, Pb2+, Cd2+, Cr6+, etc.), toxic anions (nitrate, phosphate, fluoride, etc.), and organic contaminants (organic dyes, antibiotics, etc.). These contributions demonstrate a deep understanding of the synergistic effect between the incorporated framework and homogeneous active centers. Besides, the challenges and perspectives of the future developments of ordered mesoporous materials in wastewater treatment are proposed. This work provides a theoretical basis and complete summary for the application of ordered mesoporous materials in the removal of contaminants from aqueous solutions.
Research papers
Homovalent doping: An efficient strategy of the enhanced TiNb2O7 anode for lithium-ion batteries
Xiaohe Jin, Yirui Deng, Han Tian, Miaomiao Zhou, Wenhao Tang, Huiyou Dong, Xinquan Zhang, Ruiping Liu
2024, 9(8): 1257-1266. doi: 10.1016/j.gee.2023.01.007
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The low energy density, unsatisfied cycling performance, potential safety issue and slow charging kinetics of the commercial lithium-ion batteries restrained their further application in the fields of fast charging and long-haul electric vehicles. Monoclinic TiNb2O7 (TNO) with the theoretical capacity of 387 mAh g-1 has been proposed as a high-capacity anode materials to replace Li4Ti5O12. In this work, homovalent doping strategy was used to enhance the electrochemical performance of TiNb2O7 (TNO) by employing Zr to partial substitute Ti through solvothermal method. The doping of Zr4+ ions can enlarge the lattice structure without changing the chemical valence of the original elements, refine and homogenize the grains, improve the electrical conductivity, and accelerate the ion diffusion kinetics, and finally enhance the cycle and rate performance. Specifically, Z0.05-TNO shows initial discharge capacity of as high as 312.2 mAh g-1 at 1 C and 244.8 mAh g-1 at 10 C, and still maintains a high specific capacity of 171.3 mAh g-1 after 800 cycles at 10 C. This study provides a new strategy for high-performance fast-charging energy storage electrodes.
Biomass-based production of trimellitic and trimesic acids
Lin Yuan, Yancheng Hu, Guangyi Li, Fengan Han, Aiqin Wang, Yu Cong, Tao Zhang, Feng Wang, Ning Li
2024, 9(8): 1267-1278. doi: 10.1016/j.gee.2023.02.004
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The production of industrial chemicals with renewable biomass feedstock holds potential to aid the world in pursuing a carbon-neutral society. Trimellitic and trimesic acids are important commodity chemicals in industry that are prepared by the oxidation of petroleum-derived trimethylbenzene. To reduce the dependence on the limited oil source, we develop a potential sustainable alternative towards trimellitic and trimesic acids using biomass-based 2-methyl-2,4-pentandiol (MPD), acrylate and crotonaldehyde as starting materials. The process for trimellitic acid includes dehydration/D-A reaction of MPD and acrylate, flow aromatization over Pd/C catalyst, hydrolysis and catalytic aerobic oxidation (60% overall yield). The challenging regioselectivity issue of D-A reaction is tackled by a matched combination of temperature and deep eutectic solvent ChCl/HCO2H. Crotonaldehyde can also participate in the reaction, followed by Pd/C-catalyzed decarbonylation/dehydrogenation and oxidation to provide trimesic acid in 54% overall yield. Life cycle assessment implies that compared to conventional fossil process, our biomass-based routes present a potential in reducing carbon emissions.
Armoring lithium metal anode with soft–rigid gradient interphase toward high-capacity and long-life all-solid-state battery
Rui Zhang, Biao Chen, Yuhan Ma, Yue Li, Junwei Sha, Liying Ma, Chunsheng Shi, Naiqin Zhao
2024, 9(8): 1279-1289. doi: 10.1016/j.gee.2023.02.006
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Solid polymer electrolytes (SPEs) are highly promising for realizing high-capacity, low-cost, and safe Li metal batteries. However, the Li dendritic growth and side reactions between Li and SPEs also plague these systems. Herein, a fluorinated lithium salt coating (FC) with organic-inorganic gradient and soft–rigid feature is introduced on Li surface as an artificial protective layer by the in-situ reaction between Li metal and fluorinated carboxylic acid. The FC layer can improve the interface stability and wettability between Li and SPEs, assist the transport of Li ions, and guide Li nucleation, contributing to a dendrite-free Li deposition and long-lifespan Li metal batteries. The symmetric cell with FC-Li anodes exhibits a high areal capacity of 1 mAh cm-2 at 0.5 mA cm-2, and an ultra-long lifespan of 2000 h at a current density of 0.1 mA cm-2. Moreover, the full cell paired with the LiFePO4 cathode exhibits improved cycling stability, remaining 83.7% capacity after 500 cycles at 1 C. When matching with the S cathode, the FC layer can prevent the shuttle effect, contributing to stable and high-capacity Li–S battery. This work provided a promising way for the construction of stable all-solid-state lithium metal batteries with prolonged lifespan.
Rapid and stable calcium-looping solar thermochemical energy storage via co-doping binary sulfate and Al–Mn–Fe oxides
Changjian Yuan, Xianglei Liu, Xinrui Wang, Chao Song, Hangbin Zheng, Cheng Tian, Ke Gao, Nan Sun, Zhixing Jiang, Yimin Xuan, Yulong Ding
2024, 9(8): 1290-1305. doi: 10.1016/j.gee.2023.02.009
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Solar thermochemical energy storage based on calcium looping (CaL) process is a promising technology for next-generation concentrated solar power (CSP) systems. However, conventional calcium carbonate (CaCO3) pellets suffer from slow reaction kinetics, poor stability, and low solar absorptance. Here, we successfully realized high power density and highly stable solar thermochemical energy storage/release by synergistically accelerating energy storage/release via binary sulfate and promoting cycle stability, mechanical strength, and solar absorptance via Al–Mn–Fe oxides. The energy storage density of proposed CaCO3 pellets is still as high as 1455 kJ kg-1 with only a slight decay rate of 4.91% over 100 cycles, which is higher than that of state-of-the-art pellets in the literature, in stark contrast to 69.9% of pure CaCO3 pellets over 35 cycles. Compared with pure CaCO3, the energy storage power density or decomposition rate is improved by 120% due to lower activation energy and promotion of Ca2+ diffusion by binary sulfate. The energy release or carbonation rate rises by 10% because of high O2- transport ability of molten binary sulfate. Benefiting from fast energy storage/release rate and high solar absorptance, thermochemical energy storage efficiency is enhanced by more than 50% under direct solar irradiation. This work paves the way for application of direct solar thermochemical energy storage techniques via achieving fast energy storage/release rate, high energy density, good cyclic stability, and high solar absorptance simultaneously.
Current collectors’ effects on the electrochemical performance of LiNi0.6Co0.2Mn0.2O2 suspension electrodes for lithium slurry battery
Linshan Peng, Yufei Ren, Zhaoqiang Yin, Zhitong Wang, Xiangkun Wu, Lan Zhang
2024, 9(8): 1306-1313. doi: 10.1016/j.gee.2023.03.002
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Take after the advantages of lithium-ion battery (LIB) and redox flow battery (RFB), semi-solid flow battery (SSFB) is a promising electrochemical energy storage device in renewable energy utilization. The flowable slurry electrode realizes decouple of energy and power density, while it also brings about new challenge to SSFBs, electron transport between active material and the out circuit. In this consideration, three types of current collectors (CCs) are applied to study the resistance and electrochemical performances of slurry cathodes within pouch cells for the first time. It proves that the electronic resistance (Re) between slurry electrode and the CC plays a decisive role in SSFB operation, and it is so large when Al foil is adopted that the cell cannot even work. Contact angle between Ketjen black (KB) slurry without active material (AM) and the CC is a preliminarily sign for the Re, the smaller the angle, the lower the resistance, and the better electrochemical performance of the cell.
Facet effects on bimetallic ZnSn hydroxide microcrystals for selective electrochemical CO2 reduction
Liu Han, Cheng-wei Wang, Shan-shan Luo, Ying-tang Zhou, Bing Li, Ming Liu
2024, 9(8): 1314-1320. doi: 10.1016/j.gee.2023.04.004
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Employing crystal facets to regulate the catalytic properties in electrocatalytic carbon dioxide reduction reaction (eCO2RR) has been well demonstrated on electrocatalysts containing single metals but rarely explored for bimetallic systems. Here, we synthesize ZnSn(OH)6 (ZSO) microcrystals (MCs) with distinct facets and investigate the facet effects in eCO2RR. Electrochemical studies and in situ Fourier Transform Infrared Spectroscopy (in situ-FTIR) reveal that ZSO MCs produce mainly C1 products of HCOOH and CO. The {111} facet of the ZSO MCS exhibits higher selectivity and faradaic efficiency (FE) than that of the {100} facet over a wide range of potentials (-0.9 V ∼ -1.3 V versus RHE). Density Functional Theory (DFT) calculations elucidate that the {111} facet is favorable to the adsorption/activation of CO2 molecules, the formation of intermediate in the rate-determining step, and the desorption of C1 products of CO and HCOOH molecules.
Tailoring Ni based catalysts by indium for the dehydrogenative coupling of ethanol into ethyl acetate
Ming Yin, Jifeng Pang, Jin Guo, Xianquan Li, Yujia Zhao, Pengfei Wu, Mingyuan Zheng
2024, 9(8): 1321-1331. doi: 10.1016/j.gee.2023.10.001
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Exploring stable and robust catalysts to replace the current toxic CuCr based catalysts for dehydrogenative coupling of ethanol to ethyl acetate is a challenging but promising task. Herein, novel NiIn based catalysts were developed by tailoring Ni catalysts with Indium (In) for this reaction. Over the optimal Ni0.1Zn0.7Al0.3InOx catalyst, the ethyl acetate selectivity reached 90.1% at 46.2% ethanol conversion under the conditions of 548 K and a weight hourly space velocity of 1.9 h-1 in the 370 h time on stream. Moreover, the ethyl acetate productivity surpassed 1.1 gethyl acetate gcatalyst-1 h-1, one of the best performance in current works. According to catalyst characterizations and conditional experiments, the active sites for dehydrogenative coupling of ethanol to ethyl acetate were proved to be Ni4In alloys. The presence of In tailored the chemical properties of Ni, and subsequently inhibited the C–C cracking and/or condensation reactions during ethanol conversions. Over Ni4In alloy sites, ethanol was dehydrogenated into acetaldehyde, and then transformed into acetyl species with the removal of H atoms. Finally, the coupling between acetyl species and surface-abundant ethoxyde species into ethyl acetate was achieved, affording a high ethyl acetate selectivity and catalyst stability.

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