Homogeneous electrocatalytic oxidation of ammonia to N2 under mild conditions

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.