Department of Chemistry, Yale University, 225 Prospect Street, New Haven, Connecticut 06520, United States.
Energy Sciences Institute, Yale University, 810 West Campus Drive, West Haven, Connecticut 06516, United States.
J Am Chem Soc. 2022 May 18;144(19):8449-8453. doi: 10.1021/jacs.2c01788. Epub 2022 May 10.
Electrocatalytic ammonia oxidation at room temperature and pressure allows energy-economical and environmentally friendly production of nitrites and nitrates. Few molecular catalysts, however, have been developed for this six- or eight-electron oxidation process. We now report [Cu(bipyalk)], a homogeneous electrocatalyst that realizes the title reaction in water at 94% Faradaic efficiency. The catalyst exhibits high selectivity against water oxidation in aqueous media, as [Cu(bipyalk)] is not competent for water oxidation.
室温常压下的电催化氨氧化反应可以经济有效地生产亚硝酸盐和硝酸盐，且对环境友好。然而，目前开发的用于该六电子或八电子氧化过程的分子催化剂很少。我们现在报告了一种均相电催化剂[Cu(bipyalk)]，它可以在水中以 94%的法拉第效率实现这一反应。该催化剂在水相介质中对水氧化具有高选择性，因为[Cu(bipyalk)]不能胜任水氧化。
