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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.

SUBMITTER: Habibzadeh F 

PROVIDER: S-EPMC6386726 | biostudies-literature | 2019 Feb

REPOSITORIES: biostudies-literature

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Homogeneous electrocatalytic oxidation of ammonia to N<sub>2</sub> under mild conditions.

Habibzadeh Faezeh F   Miller Susanne L SL   Hamann Thomas W TW   Smith Milton R MR  

Proceedings of the National Academy of Sciences of the United States of America 20190117 8


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 expe  ...[more]

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