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单原子钨负载在 MOF 衍生的 N 掺杂碳上用于稳定电化学析氢。

Single Tungsten Atoms Supported on MOF-Derived N-Doped Carbon for Robust Electrochemical Hydrogen Evolution.

机构信息

Department of Chemistry, Tsinghua University, Beijing, 100084, China.

Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081, China.

出版信息

Adv Mater. 2018 Jul;30(30):e1800396. doi: 10.1002/adma.201800396. Epub 2018 Jun 10.

Abstract

Tungsten-based catalysts are promising candidates to generate hydrogen effectively. In this work, a single-W-atom catalyst supported on metal-organic framework (MOF)-derived N-doped carbon (W-SAC) for efficient electrochemical hydrogen evolution reaction (HER), with high activity and excellent stability is reported. High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and X-ray absorption fine structure (XAFS) spectroscopy analysis indicate the atomic dispersion of the W species, and reveal that the W N C moiety may be the favored local structure for the W species. The W-SAC exhibits a low overpotential of 85 mV at a current density of 10 mA cm and a small Tafel slope of 53 mV dec , in 0.1 m KOH solution. The HER activity of the W-SAC is almost equal to that of commercial Pt/C. Density functional theory (DFT) calculation suggests that the unique structure of the W N C moiety plays an important role in enhancing the HER performance. This work gives new insights into the investigation of efficient and practical W-based HER catalysts.

摘要

基于钨的催化剂是有效产生氢气的有前途的候选物。在这项工作中,报道了一种负载在金属有机骨架(MOF)衍生的 N 掺杂碳(W-SAC)上的单 W 原子催化剂,用于高效电催化析氢反应(HER),具有高活性和优异的稳定性。高角度环形暗场扫描透射电子显微镜(HAADF-STEM)和 X 射线吸收精细结构(XAFS)光谱分析表明 W 物种的原子分散性,并揭示出 W-N-C 部分可能是 W 物种的优选局部结构。在 0.1 m KOH 溶液中,W-SAC 在电流密度为 10 mA cm 时表现出 85 mV 的低过电势和 53 mV dec 的小塔菲尔斜率。W-SAC 的 HER 活性几乎与商业 Pt/C 相当。密度泛函理论(DFT)计算表明,W-N-C 部分的独特结构在增强 HER 性能方面起着重要作用。这项工作为研究高效实用的 W 基 HER 催化剂提供了新的见解。

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