ACS Sustainable Chemistry & Engineering
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2024
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IF 7.1
Yanyan Li,Haoran Guo,Jiayang Zhao,Kanglei Pang,Rui Song
Surface reconstruction generates genuine active phases under an electrochemical oxygen evolution reaction (OER); however, most OER catalysts exhibit slow self-reconstruction due to their relative stability in electrochemistry. Therefore, it is highly essential to rationally design precatalysts capable of rapidly generating more active OER species. Herein, a novel reconfigurable Te-doped NiFe layered double hydroxide (Te-NiFe LDH/NF) precatalyst is prepared, which exhibits ultrafast and in-depth self-reconstruction, significantly enhancing the activity for the OER step. By employing various in/ex situ techniques and theoretical calculations, the distinctive structure of Te-NiFe LDH/NF along with the alkaline electrolyte are identified as pivotal factors for facilitating the phase transition. The presence of Te cations can effectively reduce the energy barrier, thereby providing the feasibility of continuous reconstruction, while the alkaline electrolyte supplies a complement of OH– to form highly active oxyhydroxides. Besides, Te is doped in situ into the NiFeOxHy lattice (Te-NiFeOxHy/NF), leading to optimized binding energies of the OER intermediates and reduced energy barriers for the rate-determining step (RDS), ultimately enhancing the OER performance. As such, the self-restructured Te-NiFeOxHy/NF only required 208 and 310 mV to achieve 10 and 500 mA cm–2, respectively, together with high current stability for 300 h. This study provides a rational design strategy to develop highly efficient electrocatalysts for the OER through surface reconstruction.
研究领域:
材料科学
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电化学
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催化
✓ 已验证
产品关联
DOI
高影响因子
Surfaces and Interfaces
·
2024
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IF 5.7
Yichen Liu,Yaqi Liu,Guicheng Luo,Zuozheng Xu,Xuhao Sun,Yuan Zhu,Shuyi Wu,Lizhe Liu,Yun Shan
To efficiently control oxygen evolution reaction (OER) at electrocatalysts holds enormous promise for large-scale production of clean energy, but faces the scarcity of practical regulation strategies due to underexplored catalytic mechanism. Herein, a facile and feasible strategy is developed involving metal-metal super-exchange interaction to manipulate the electronic state configuration of catalysts, and the as-synthesized Ni-doped Co-1,3,5-benzenetricarboxylic acid Metal-Organic Frameworks (MOFs) only require an overpotential as low as 260 mV to reach a large current of 200 mA cm −2 , which is much lower than 400 mV for the commercial RuO 2 catalyst. The introduced Ni atoms lead to more broadly occupied states and d-band center close to the Fermi energy level for the spin-polarization of the electrons in Co atoms, thus decreasing the orbital occupancy to facilitate the adsorption/desorption of the reaction intermediates and lowering the rate-determining step barrier to accelerate OER. Our findings have an important paradigm role in the design of electrocatalysts with high performance for oxygen evolution reaction.
研究领域:
电化学
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催化
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材料科学
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能源存储与转换
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Changle Yue,Na Liu,Yaping Li,Yang Liu,Fengyue Sun,Wenjing Bao,Yongxiao Tuo,Yuan Pan,Ping Jiang,Yan Zhou,Yukun Lu
Herein, a novel in-situ “atomic binding to heterointerface” strategy is proposed to obtain Co 2 P/ [email protected] /CNTs catalyst with abundant heterointerface between cobalt phosphide and tungsten carbide (Co 2 P/WC) by the polyoxometalates (POMs)-based metal–organic frameworks (MOFs) precursor. The natural quasi interfaces in K 10 [Co 4 (H 2 O) 2 (PW 9 O 34 ) 2 ] molecule crucially guide the abundant Co 2 P/WC heterointerfaces down to atomic level. Meanwhile, MOFs cages can effectively encapsulate nanosized POMs at molecular level to control the size and dispersion of Co 2 P/WC nanoparticle , while carbon nanotubes (CNTs) enhance conductivity at nanoscale level. The interfacial electronic modulation between Co 2 P and WC lowering the energy barrier of the rate determining step , thus Co 2 P/ [email protected] /CNTs showed reasonable hydrogen evolution reaction (HER) activity and stability in all-pH media including sea water. This work provides a “bottom-up” synthetic strategy for confined heterostructures , thus offering the prospect for more efficient interfacial charge modulation.
研究领域:
材料科学
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电化学
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纳米技术
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催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
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2022
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IF 8.047
Leisheng Che,Jinqiu Guo,Zhiwei He,Hongbo Zhang
We report here that the reduction degree of the metal at the catalytic interface dominates the reactivity of acetylene hydrogenation, mainly in terms of turnover rates (TORs) and activation energies, which could certainly cause the switch of kinetically relevant steps (KRS) from “C 2 H 3 *+H*” over Ce(OH)SO 4 ·xH 2 O dispersed Pd catalyst to “C 2 H 4 *+H*” elementary step over Pd/CeO 2 . Besides, a compact kinetic model has been established to describe the reaction process and the dissociative mechanism was confirmed by H 2 /D 2 exchange experiment. Meanwhile, the rate-determining step (RDS) and the main adsorbed species of the reaction were confirmed by systematic kinetic studies as well as in-situ FTIR analysis. More importantly, with the aid of parity fitting and gas isothermic adsorption analysis, the energetic relationship among the steps along with the acetylene hydrogenation is quantitatively described, which provides a good support and complement for the previous research, and helps researchers build up advanced reaction systems.
研究领域:
化学动力学
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催化
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表面化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）