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首页> 外文期刊>ChemSusChem >Key Single-Atom Electrocatalysis in Metal-Organic Framework (MOF)-Derived Bifunctional Catalysts
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Key Single-Atom Electrocatalysis in Metal-Organic Framework (MOF)-Derived Bifunctional Catalysts

机译：金属有机框架（MOF）的关键单原子电催化（MOF）的双官能催化剂

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摘要

Metal-organic framework (MOF)-derived materials have attracted increasing interest and show promising catalytic performances in many fields. Intensive efforts have been focused on the structure design and metal-site integration in MOF-derived catalysts. However, the key catalytic processes related with the metal sites in MOF-derived catalysts that dominate the electrocatalytic performance still remain obscure. Herein, we show a neglected but critical issue in the pyrolytic synthesis of MOF-derived catalysts: the coupled evolution of dual sites, that is, metallic sites and single-atom metal sites. The identification of active sites of single-atom sites from the visible particles has been elucidated through the combined X-ray spectroscopic, electron microscopic, and electrochemical studies. Interestingly, after a total removal of metallic cobalt sites, catalysts with purified single-atom metal sites show no faltering activity for either the oxygen reduction reaction (ORR) or hydrogen evolution reaction (HER), while significantly enhanced ORR selectivity is achieved; this reveals the dominant activity and selectivity contribution from single-atom electrocatalysis. The insight of the coupled evolution of dual sites and the as-demonstrated dual-site decoupling strategies open up a new routine for the design and synthesis of MOF-derived catalysts with the optimized single-atom electrocatalysis towards various electrochemical reactions.
机译：金属有机框架（MOF）相移的材料吸引了越来越多的兴趣，并在许多领域中显示出有希望的催化性能。密集的努力集中在MOF衍生催化剂中的结构设计和金属现场集成上。然而，与MOF衍生催化剂中的金属位点有关的关键催化过程，其主导电催化性能仍然模糊不清。在此，我们在MOF衍生催化剂的热解合合成中显示出忽略但危重问题：双位点的偶联演变，即金属位点和单原子金属位点。通过组合的X射线光谱，电子显微镜和电化学研究，阐明了从可见颗粒的单原子位点的活性位点的鉴定。有趣的是，在总去除金属钴位点之后，具有纯化的单原子金属位点的催化剂表明，对于氧还原反应（ORR）或氢进化反应（她）而言，催化剂的活性不会达到富饶活性，同时实现显着增强的ORR选择性;这揭示了从单原子电催化的主导活动和选择性贡献。双部位耦合演化的洞察力和展示的双现场去耦策略开辟了一种新的常规，用于设计和合成MOF衍生的催化剂，其优化的单原子电常放朝各种电化学反应。

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  • 来源
    《ChemSusChem》 |2018年第19期|共7页
  • 作者

    Zhao Wanpeng; Wan Gang; Peng Chunlei; Sheng Huaping; Wen Jianguo; Chen Hangrong;

  • 作者单位

    Chinese Acad Sci Shanghai Inst Ceram State Key Lab High Performance Ceram &

    Superfine 1295 Dingxi Rd Shanghai 200050 Peoples R China;

    Chinese Acad Sci Shanghai Inst Ceram State Key Lab High Performance Ceram &

    Superfine 1295 Dingxi Rd Shanghai 200050 Peoples R China;

    Chinese Acad Sci Shanghai Inst Ceram State Key Lab High Performance Ceram &

    Superfine 1295 Dingxi Rd Shanghai 200050 Peoples R China;

    Argonne Natl Lab Ctr Nanoscale Mat 9700 S Cass Ave Lemont IL 60439 USA;

    Argonne Natl Lab Ctr Nanoscale Mat 9700 S Cass Ave Lemont IL 60439 USA;

    Chinese Acad Sci Shanghai Inst Ceram State Key Lab High Performance Ceram &

    Superfine 1295 Dingxi Rd Shanghai 200050 Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 化学;
  • 关键词

    electrocatalysis; hydrogen evolution reaction; oxygen reduction reaction; selectivity; transition-metal sites;

    机译：电殖分析;氢气进化反应;氧还原反应;选择性;过渡金属位点;

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