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首页> 外文期刊>Proceedings of the National Academy of Sciences of the United States of America >Cobalt and nickel diimine-dioxime complexes as molecular electrocatalysts for hydrogen evolution with low overvoltages
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Cobalt and nickel diimine-dioxime complexes as molecular electrocatalysts for hydrogen evolution with low overvoltages

机译：钴和二亚胺二肟-二肟肟镍配合物作为低过电压析氢的分子电催化剂

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摘要

Hydrogen production through the reduction of water appears to be a convenient solution for the long-run storage of renewable energies. However, economically viable hydrogen production requests platinum-free catalysts, because this expensive and scarce (only 37 ppb in the Earth's crust) metal is not a sustainable resource [Gordon RB, Bertram M, Graedel TE (2006) Proc Natl Acad Sci USA 103:1209-1214]. Here, we report on a new family of cobalt and nickel diimine-dioxime complexes as efficient and stable electro-catalysts for hydrogen evolution from acidic nonaqueous solutions with slightly lower overvoltages and much larger stabilities towards hydrolysis as compared to previously reported cobaloxime catalysts. A mechanistic study allowed us to determine that hydrogen evolution likely proceeds through a bimetallic homolytic pathway. The presence of a proton-exchanging site in the ligand, furthermore, provides an exquisite mechanism for tuning the electrocatalytic potential for hydrogen evolution of these compounds in response to variations of the acidity of the solution, a feature only reported for native hydrogenase enzymes so far.
机译：通过减少水分生产氢气似乎是长期存储可再生能源的便捷解决方案。但是，经济上可行的制氢需要无铂催化剂，因为这种昂贵且稀少的金属（地壳中只有37 ppb）不是可持续的资源[Gordon RB，Bertram M，Graedel TE（2006）Proc Natl Acad Sci USA 103 ：1209-1214]。在这里，我们报告了一个新的钴和亚胺二亚胺-二肟配合物家族，它是从酸性非水溶液中析氢的高效且稳定的电催化剂，与先前报道的钴肟催化剂相比，该过氧化物具有较低的过电压和更大的水解稳定性。一项机械研究使我们能够确定氢的逸出可能是通过双金属均解途径进行的。此外，配体中质子交换位点的存在还提供了一种精致的机制，可以根据溶液酸度的变化来调节这些化合物的氢析出电催化能力，这是迄今为止仅针对天然氢化酶的一项功能。

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  • 作者

    Pierre-Andre Jacques; Vincent Artero; Jacques Pecaut; Marc Fontecave;

  • 作者单位

    Laboratoire de Chimie et Biologie des Metaux, Universite Joseph Fourier, Grenoble, Centre National de la Recherche Scientifique, Unite Mixte de Recherche 5249, CEA, DSV/iRTSV, 17 rue des Martyrs, F-38054 Grenoble cedex 9, France;

    Laboratoire de Chimie et Biologie des Metaux, Universite Joseph Fourier, Grenoble, Centre National de la Recherche Scientifique, Unite Mixte de Recherche 5249, CEA, DSV/iRTSV, 17 rue des Martyrs, F-38054 Grenoble cedex 9, France;

    Laboratoire de Reconnaissance lonique et Chimie de Coordination Unite Mixte de Recherche Centre National de la Recherche Scientifique/Universite Joseph Fourier/CEA E3, 17 rue des Martyrs, F-38054 Grenoble cedex 9, France;

    Laboratoire de Chimie et Biologie des Metaux, Universite Joseph Fourier, Grenoble, Centre National de la Recherche Scientifique, Unite Mixte de Recherche 5249, CEA, DSV/iRTSV, 17 rue des Martyrs, F-38054 Grenoble cedex 9, France College de France, 11 place Marcelin-Berthelot, 75231 Paris cedex 05, France;

  • 收录信息 美国《科学引文索引》(SCI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    bio-inspired chemistry; cobaloxime; electrocatalysis; hydrogen evolution reaction; hydrogenase;

    机译：生物启发化学;钴肟电催化析氢反应氢化酶;

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