在温和条件下，氨的均相电催化氧化生成 N。
Homogeneous electrocatalytic oxidation of ammonia to N under mild conditions.
机构信息
Department of Chemistry, Michigan State University, East Lansing, MI 48824.
Department of Chemistry, Michigan State University, East Lansing, MI 48824
出版信息
Proc Natl Acad Sci U S A. 2019 Feb 19;116(8):2849-2853. doi: 10.1073/pnas.1813368116. Epub 2019 Jan 17.
Abstract
We report that ruthenium polypyridyl complexes can catalyze ammonia oxidation to dinitrogen at room temperature and ambient pressure. During bulk electrolysis experiments, gas chromatography and mass spectrometry analysis of the headspace in the electrochemical cell showed that dinitrogen and dihydrogen are generated from ammonia with high faradaic efficiencies. A proposed mechanism where a hydrazine complex is the initial N-N bonded intermediate is supported by chemical and electrochemical experiments. This is a well-defined system for homogeneous electrocatalytic ammonia oxidation. It establishes a platform for answering mechanistic questions relevant to using ammonia to store and distribute renewable energy.
摘要
我们报告说，钌多吡啶配合物可以在室温常压下催化氨氧化为氮气。在批量电解实验中，对电化学电池中顶空的气相色谱和质谱分析表明，氮气和氢气是由氨以高法拉第效率生成的。化学和电化学实验支持一种假设的机制，即肼配合物是初始的 N-N 键合中间体。这是一个用于均相电催化氨氧化的明确定义的体系。它为回答使用氨来储存和分配可再生能源的相关机制问题提供了一个平台。
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