期刊名称：Proceedings of the National Academy of Sciences
印刷版ISSN：0027-8424
电子版ISSN：1091-6490
出版年度：2019
卷号：116
期号：8
页码：2849-2853
DOI：10.1073/pnas.1813368116
语种：English
出版社：The National Academy of Sciences of the United States of America
摘要：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.
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