Homogeneous electrocatalytic oxidation of ammonia to N2 under mild conditions

Habibzadeh, Faezeh; Miller, Susanne L.; Hamann, Thomas W.; Smith, III, Milton R.

doi:10.1073/pnas.1813368116

Homogeneous electrocatalytic oxidation of ammonia to N₂ under mild conditions

Journal Article · Wed Jan 16 23:00:00 EST 2019 · Proceedings of the National Academy of Sciences of the United States of America

DOI:https://doi.org/10.1073/pnas.1813368116· OSTI ID:1491265

Habibzadeh, Faezeh; Miller, Susanne L.; Hamann, Thomas W.;

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. This work establishes a platform for answering mechanistic questions relevant to using ammonia to store and distribute renewable energy.

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Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: SC0016604

OSTI ID:: 1491265

Alternate ID(s):: OSTI ID: 1612672

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 8 Vol. 116; ISSN 0027-8424

Publisher:: National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: English

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