JOURNAL OF MEMBRANE SCIENCE
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2025
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IF 9
Xiaoqing Wang,Jinyun Xu,Shijie Shang,Ming Li,Sijia He,Xiaoyan Wang,Bingyu Yang,Yirang He,Xiaolu Ru,Yanyan Ji,Wenju Zhu,Chunming Zheng,Xiaohong Sun
Bipolar membranes (BPMs), composed of anion exchange membrane (AEM) and cation exchange membrane (CEM), hold promise for energy and environmental applications due to their ability to dissociate water into H + and OH − under reverse bias. However, their practical voltage requirements often exceed theoretical potentials, necessitating efficiency optimization. This study introduces an innovative BPM design integrating alginate (SA)-based CEM with chitosan AEM, enhanced by polydopamine-coated halloysite nanotubes (DHNTs) loaded with phosphotungstic acid (HPW). The tubular structure of the DHNTs, modified via dopamine polymerization, improved mechanical stability and proton conductivity, while HPW coating (optimized at 10 wt %) facilitated acid-base interactions, reducing proton hopping distances. Comprehensive characterization (SEM, FTIR, XPS, TGA) confirmed successful HPW coating and structural modification. The optimized BPM exhibited enhanced tensile strength than unmodified BPM with proton conductivity of 36.56 mS/cm and low water dissociation overpotential of 1.188 V at 70 mA/cm 2 . Electrodialysis tests revealed reduced interfacial resistance (IR drop) and increased stability over 48 h, attributed to HPW's catalytic role in accelerating ion transport and minimizing energy loss. The synergy between DHNTs and HPW significantly improved hydrophilicity, mechanical robustness, and energy efficiency, demonstrating the potential of this design for sustainable electrochemical systems. These findings provide critical insights into advanced BPM development for scalable energy and environmental technologies.
研究领域:
材料科学
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能源技术
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环境科学
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产品关联
DOI
高影响因子
Energy & Environmental Materials
·
2021
·Vol. 6
·期 1
·e12292
·
IF 15.122
Ruofan Shen,Yanyan Liu,Hao Wen,Xianli Wu,Zhikun Peng,Sehrish Mehdi,Tao Liu,Huanhuan Zhang,Shuyan Guan,Erjun Liang,Baojun Li
The dissociation of water is the rate-determining step of several energy-relating reactions due to high energy barrier in homolysis of H-O bond. Herein, engineering vacancy-atom ensembles via injecting oxygen vacancy (V O ) into single facet-exposed TiO 2 -Pd catalyst to form V O -Pd ensemble is proposed and implemented. The outstanding activity of as-prepared catalyst, 1.5-PdTV O , toward water dissociation is established with a turnover frequency of 240 min −1 in ammonia borane hydrolysis at 298 K. Density functional theory simulation suggests that the V O -Pd ensemble is responsible for the high intrinsic catalytic activity. Water molecules tend to be dissociated on V O sites and ammonia borane molecules on Pd atoms. Those H atoms from water dissociation on V O combine with H atoms from ammonia borane on Pd atoms to generate H 2 . This insights into engineering vacancy-atom ensembles catalysis provide a new avenue to design catalytic materials for important energy chemical reactions.
研究领域:
材料科学
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催化化学
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能源化学
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
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2019
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IF 7.723
Hongye Qin,Biao Zhang,Yaping Pan,Xixi Wang,Lechen Diao,Jiao Chen,Jinli Wu,Enzuo Liu,Junwei Sha,Liying Ma,Naiqin Zhao
Developing efficient and low-cost electrocatalysts for hydrogen evolution reaction (HER) is important in clean energy systems. Non-noble transition metals are the most promising candidates for the replacement of conventional Pt group catalysts of HER . However, most non-noble metals show poor HER activity due to the intrinsic electronic structures. Herein, P atoms doped Ni 3 S 2 (P-doped Ni 3 S 2 ) nanosheets array grown on Ni foam has been successfully synthesized and further applied as the efficient electrocatalysts for HER in alkaline media. P-doped Ni 3 S 2 shows higher catalytic activity for HER compared with pristine Ni 3 S 2 , which affords the current densities of 10 mA cm −2 at an overpotential of 139 mV and long-term stability over 110 h. Density functional theory (DFT) calculations reveal that the introduction of P atoms modify the electronic structure of Ni 3 S 2 , enhance the electrical conductivity, optimize the HER Gibbs free-energy (Δ G H* ) and the change of water adsorption energy (Δ G H2O* ), and reduce the barrier of water dissociation optimize the HER Gibbs free-energy (Δ G H* ), change water adsorption energy (Δ G H2O * ) and reduce the barrier of water dissociation. Remarkably, energy integral of a crystal orbital Hamilton population (ICOHP) gives access to the contribution of an atom or a chemical bond to the distribution of one-particle bonding within the transistion state of water dissociation and reveals the reduced essence of water dissociation barrier.
研究领域:
材料科学
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电催化
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理论计算
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DOI
高影响因子
Nature Communications
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2022
·Vol. 13
·期 1
·1-13
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IF 17.694
Hao Jiace,Zhuang Zechao,Cao Kecheng,Gao Guohua,Wang Chan,Lai Feili,Lu Shuanglong,Ma Piming,Dong Weifu,Liu Tianxi,Du Mingliang,Zhu Han
High-entropy alloys have received considerable attention in the field of catalysis due to their exceptional properties. However, few studies hitherto focus on the origin of their outstanding performance and the accurate identification of active centers. Herein, we report a conceptual and experimental approach to overcome the limitations of single-element catalysts by designing a FeCoNiXRu (X: Cu, Cr, and Mn) High-entropy alloys system with various active sites that have different adsorption capacities for multiple intermediates. The electronegativity differences between mixed elements in HEA induce significant charge redistribution and create highly active Co and Ru sites with optimized energy barriers for simultaneously stabilizing OH * and H * intermediates, which greatly enhances the efficiency of water dissociation in alkaline conditions. This work provides an in-depth understanding of the interactions between specific active sites and intermediates, which opens up a fascinating direction for breaking scaling relation issues for multistep reactions.
研究领域:
材料科学
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电化学
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催化反应
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Yong Li,Weining Song,Teng Gai,Lipeng Wang,Zhen Li,Peng He,Qi Liu,Lawrence Yoon Suk Lee
Molybdenum carbides are promising alternatives to Pt-based catalysts for the hydrogen evolution reaction (HER) due to their similar d -band electronic configuration. Notably, Mo x C exhibits superior HER kinetics in alkaline media compared to acidic conditions, contrasting with Pt-based catalysts. Herein, we present 3D porous β-Mo 2 C nanosheets, achieving an overpotential of 111 mV at 10 mA cm −2 in 1 M KOH, significantly lower than in acidic environments. Simulations on pristine Mo 2 C surface reveal that water dissociation poses a higher energy barrier in alkaline media, suggesting that crystal structure alone does not dictate kinetics. Operando attenuated total reflection surface-enhanced infrared absorption spectroscopy shows that Mo 2 C activates interfacial water, generating liquid-like and free water, and facilitates hydroxyl species adsorption, reducing activation energy to below 38.43 ± 0.19 kJ/mol. Our findings on the self-activation effect offer insights into the HER mechanism of Mo-based electrocatalysts and guide the design of highly active HER catalysts.
研究领域:
材料科学
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电化学
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催化科学
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产品关联
DOI
PubMed
高影响因子
INORGANIC CHEMISTRY
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2024
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IF 4.3
Huijiao Wang,Gening Du,Jinzhi Jia,Junfeng Huang,Mudong Tu,Jinhua Zhang,Yong Peng,Hua Li,Cailing Xu
The Electrochemical reduction of nitrate to ammonia (NH3) is a process of great significance to energy utilization and environmental protection. However, it suffers from sluggish multielectron/proton-involved steps involving coupling reactions between different reaction intermediates and active hydrogen species (Hads) produced by water decomposition. In this study, a Ru-doped NiFe-MIL-53 (NiFeRu-MIL-53) supported on Ni foam (NF) has been designed for the nitrate reduction reaction (NO3RR). The NiFeRu-MIL-53 exhibits excellent NO3RR activity with a maximum Faradaic efficiency (FE) of 100% at −0.4 V vs. RHE for NH3 and a maximum NH3 yield of 62.39 mg h–1 cm–2 at −0.7 V vs. RHE in alkaline media. This excellent performance for the NO3RR is attributed to a strong synergistic effect between Ru and reconstructed NiFe(OH)2. Additionally, the doped Ru facilitates water dissociation, leading to an appropriate supply of Hads required for N species hydrogenation during NO3RR, thereby further enhancing its performance. Furthermore, in situ Raman analysis reveals that incorporating Ru facilitates the reconstruction of MOFs and promotes the formation of hydroxide active species during the NO3RR process. This work provides a valuable strategy for designing electrocatalysts to improve the efficiency of the reduction of electrochemical nitrate to ammonia.
研究领域:
环境科学
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电化学
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材料科学
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产品关联
DOI
PubMed
高影响因子
ACS Applied Energy Materials
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2020
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IF 4.473
Zijuan Ge,Muhammad Aamir Shehzad,Liang Ge,Yuan Zhu,Huijuan Wang,Geng Li,Jianjun Zhang,Xiaolin Ge,Liang Wu,Tongwen Xu
Bipolar membrane (BPM) has been used commercially in electrodialysis separation processes for the generation of acid and base from aqueous salt solutions and electrochemical water splitting processes for hydrogen generation. Research advances have demonstrated that, upon a sufficient applied reverse bias, water molecules at the junction zone of the BPM can dissociate into protons (H+) and hydroxide anions (OH–). Therefore, a stable and catalytic active junction for rapid water dissociation is highly desired, but it still remains a challenge for current bipolar membrane designs. Here, we demonstrate a versatile strategy for fabricating a thin metal–polymer coordination complex junction-based bipolar membrane. The complex used consists of polyethylenimine (PEI) that coordinate to Fe(III) centers through the amine–iron interaction (Fe(III)@PEI). The unique coordination interaction enables to promote water dissociation and suppress catalyst leakage issue. In addition, to prevent junction layer dehydration from highly efficient water dissociation, the cation-exchange membrane containing porous water channels is utilized to sufficiently replenish the water molecules consumed at the junction zone. Notably, under a current density of 320 mA cm–2, Fe(III)@PEI-based BPM exhibits a voltage of 1.88 V, which is 56 and 36% lower than PEI-based BPM and FeCl3-based BPM, respectively. Moreover, during a constant current density operation at 60 mA cm–2, Fe(III)@PEI-based BPM exhibits a much lower voltage increasing speed (5.93 mV h–1) than the FeCl3-based BPM (32.64 mV h–1), indicating the improved durability of the metal–polymer coordination complex junction.
研究领域:
化学工程
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电化学
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材料科学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
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2019
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IF 8.456
Jianpo Chen,Qiuyan Jin,Yinwei Li,Yan Li,Hao Cui,Chengxin Wang
In alkaline media, the water-dissociation-related Volmer process always suppresses the hydrogen formation/desorption process, which makes it challenging to develop non-noble-metal alkaline electrocatalysts with excellent catalytic activity. Here, we proposed a two-pronged strategy to simultaneously promote the kinetic process of both water dissociation and hydrogen desorption with the Co-doped WO2/amorphous CoxW hybrid electrocatalyst. Impressively, the optimized hybrid exhibits an outstanding hydrogen evolution reaction (HER) activity with the quite small Tafel slope of 19.77 mV dec–1 and ultralow overpotential of just 25 mV to reach a current density of 10 mA cm–2 in alkaline media. Both experiments and density functional theory calculations reveal that the top-level HER performance can be attributed to the cooperation of two different active components, in which the water molecule can easily be activated on the amorphous CoxW with low energy barrier (ΔGw = 0.46 eV), while hydrogen atoms can rapidly desorb from the Co-doped WO2 with an optimal Gibbs free energy of hydrogen adsorption (ΔGH* = −0.06 eV). Also, the density functional theory calculation further confirms that the H* tends to combine with another H* via Tafel step rather than Heyrovsky step. The findings provide unique insights for the development of the state-of-the-art non-noble-metal HER electrocatalyst with a Pt-like kinetic behavior in alkaline media.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
WATER RESEARCH
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2025
·
IF 12.4
Hao Zhang,Xupeng Liu,Biao Zhou,Ziyue Chen,Jundi Cheng,Kehang Zeng,Lizhi Zhang,Hongwei Sun,Zhihui Ai
Mercury (Hg) is a toxic metal of great concern, and its reduction from Hg(II) to Hg(0) is crucial to prevent its mobilization and transformation to even more hazardous methylmercury. Fe° could reduce Hg(II), but the role of active hydrogen species (*H) remains unexplored. Herein, we prepared the phosphate-modified zero-valent iron by ball milling (P-ZVI bm ) and investigated its Hg(II) reduction and immobilization capacity compared with the ZVI bm counterpart. P-ZVI bm rapidly adsorbed and reduced Hg(II) from water at a rate 22 times faster than ZVI bm , with *H accounting for 36% of Hg(II) reduction. A greatly higher proportion of negative surface electrostatic potential on P-ZVI bm (50.38%) than ZVI bm (37.61%) facilitated the adsorption of Hg(II) cation. H 2 O adsorption on P-ZVI bm was more favorable, as demonstrated by the in situ ATR-FTIR spectra, H 2 O TPD-mass spectra, and the substantially lower adsorption energy (-0.78 eV) than ZVI bm (-0.17 eV). The energy span of H 2 O dissociation to *H also decreased from 2.80 eV on ZVI bm to 1.99 eV on P-ZVI bm . Moreover, *H adsorption energy on P-ZVI bm (1.70 eV) was lower than on ZVI bm (-1.20 eV), thereby inhibiting consumption of *H by H 2 evolution. P-ZVI bm demonstrated remarkable efficacy in removing Hg(II), Cu(II), Ni(II), Cd(II), and Pb(II) from electroplating and mining wastewater. These results highlight P-ZVI bm as a promising material for Hg(II) and other heavy metal remediation and underscore the essential role of *H in the enhanced Hg(II) reduction.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
Advanced Powder Materials
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2024
·
IF 28.6
Jingjing Yan,Rundong Wu,Guoqiang Jin,Litao Jia,Gang Feng,Xili Tong
Water electrolysis via alkaline hydrogen evolution reaction (HER) is a promising approach for large-scale production of high-purity hydrogen at a low cost, utilizing renewable and clean energy. However, the sluggish kinetics derived from the high energy barrier of water dissociation impedes seriously its practical application. Herein, a series of hybrid Pt nanoclusters/Ru nanowires (Pt/Ru NWs) catalysts are demonstrated to accelerate alkaline HER. And the optimized Pt/Ru NWs (10 % wt Pt) exhibits exceptional performance with an ultralow overpotential (24 mV at 10 mA cm −2 ), a small Tafel slope (26.3 mV dec −1 ), and long-term stability, outperforming the benchmark commercial Pt/C-JM-20 % wt catalyst. This amazing performance also occurred in the alkaline anion-exchange membrane water electrolysis devices, where it delivered a cell voltage of about 1.9 V at 1 A cm −2 and an outstanding stability (more than 100 h). The calculations have revealed such a superior performance exhibited by Pt/Ru NWs stems from the formed heterointerfaces, which significantly reduce the energy barrier of the decisive rate step of water dissociation via cooperative-action between Pt cluster and Ru substance. This work provides valuable perspectives for designing advanced materials toward alkaline HER and beyond.
研究领域:
材料科学
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催化化学
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可再生能源
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产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2022
·Vol. 32
·期 16
·2109439
·
IF 19.924
Jiachen Li,Yang Li,Jiaao Wang,Chi Zhang,Huijun Ma,Chenhui Zhu,Daidi Fan,Zhaoqi Guo,Ming Xu,Yaoyu Wang,Haixia Ma
Hydrazine oxidation (HzOR)-assisted overall water splitting (OWS) provides a unique approach to energy-efficient hydrogen production (HER). However, there are still major challenges in the design of bifunctional catalysts and gain deep insight into the mechanism of both water dissociation and dehydrogenation kinetics triggered by the same active species during HzOR-assisted OWS. Here, ruthenium single atoms (Ru SAs) anchored onto sulphur-vacancies of tungsten disulphide (WS 2 ) are prepared by a sulfidation and facile galvanostatic deposition strategy. The WS 2 /Ru SAs act as a bifunctional catalyst and outperforms commercial platinum (Pt) catalysts for both HzOR and HER. Ultralow potentials of −74 and −32.1 mV at 10 mA cm −2 are achieved for HzOR and HER, respectively. Two-electrode electrolyzer using WS 2 /Ru SAs as both anode and cathode reaches 10 mA cm −2 with cell voltage of only 15.4 mV, which is far below that of most electrocatalysts including commercial Pt. Density functional theory calculations unravel the critical role of Ru SAs in WS 2 , where the sluggish dissociation of water in HER can be promoted on Ru sites, and the sulfur sites of WS 2 exhibit a more thermoneutral behavior for hydrogen intermediate adsorption. Moreover, Ru sites are also active centers for stepwise hydrazine dehydrogenation during HzOR.
研究领域:
材料科学
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催化化学
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理论计算
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Weisheng Yu,Fen Luo,Xiaojiang Li,Jingjing Tu,Xian Liang,Yan Xu,Zhiru Liu,Wenfeng Li,Jihao Zhang,Luxin Xiong,Huijuan Wang,Liang Wu,Tongwen Xu
Water dissociation (WD, H2O → H+ + OH–) occurring at the bipolar membrane (BPM) junction can be leveraged in water electrolyzers for green hydrogen production, enabling the anode and cathode reactions to operate in kinetically favorable pH environments. However, practical application of BPM-integrated membrane electrode assemblies (BPMEAs) in electrolyzers faces formidable challenges due to the sluggish WD efficiency and insufficient stability at the bipolar junction. Here, we develop a convenient serial spraying approach to fabricate an all-in-one BPMEA. This approach endows the BPMEA with a wrinkled bipolar junction and integrated membrane/electrode interfaces, expanding the active interfaces and thereby enhancing WD efficiency and mass transport within BPMEA. As a result, the BPMEA exhibits competitive pure water and asymmetric acid/alkali electrolyzer voltages of 3.25 and 2.69 V at a high current density of 3000 mA cm–2, achieving 32% and 23% savings in energy consumption. Moreover, the wrinkled architecture imparts physical reinforcement to the bipolar junction and membrane/electrode interfaces, leading to an appropriate durability at current densities of 500–1000 mA cm–2. This work provides insights into the performance degradation mechanisms of BPM electrolyzers, and the proposed all-in-one approach is applicable to a broader range of electrochemical applications beyond water electrolysis.
研究领域:
电化学
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能源材料
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膜科学
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氢能源
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催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）