Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 116, Issue 8, Pages 2849-2853Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1813368116
Keywords
renewable fuel; hydrogen storage; electrocatalysis; nitrogen chemistry; sustainability
Categories
Funding
- US Department of Energy [DE-SC0016604]
- Camille Dreyfus Teacher-Scholar Awards Program
- U.S. Department of Energy (DOE) [DE-SC0016604] Funding Source: U.S. Department of Energy (DOE)
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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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