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Title: Homogeneous electrocatalytic oxidation of ammonia to N 2 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.

Authors:
; ; ; ORCiD logo
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1491265
Grant/Contract Number:  
SC0016604
Resource Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 116 Journal Issue: 8; Journal ID: ISSN 0027-8424
Publisher:
Proceedings of the National Academy of Sciences
Country of Publication:
United States
Language:
English

Citation Formats

Habibzadeh, Faezeh, Miller, Susanne L., Hamann, Thomas W., and Smith, III, Milton R. Homogeneous electrocatalytic oxidation of ammonia to N 2 under mild conditions. United States: N. p., 2019. Web. doi:10.1073/pnas.1813368116.
Habibzadeh, Faezeh, Miller, Susanne L., Hamann, Thomas W., & Smith, III, Milton R. Homogeneous electrocatalytic oxidation of ammonia to N 2 under mild conditions. United States. doi:10.1073/pnas.1813368116.
Habibzadeh, Faezeh, Miller, Susanne L., Hamann, Thomas W., and Smith, III, Milton R. Tue . "Homogeneous electrocatalytic oxidation of ammonia to N 2 under mild conditions". United States. doi:10.1073/pnas.1813368116.
@article{osti_1491265,
title = {Homogeneous electrocatalytic oxidation of ammonia to N 2 under mild conditions},
author = {Habibzadeh, Faezeh and Miller, Susanne L. and Hamann, Thomas W. and Smith, III, Milton R.},
abstractNote = {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.},
doi = {10.1073/pnas.1813368116},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 8,
volume = 116,
place = {United States},
year = {2019},
month = {2}
}

Journal Article:
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This content will become publicly available on August 19, 2019
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