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Title: The impact of nitrogen oxides on electrochemical carbon dioxide reduction

Abstract

The electroreduction of carbon dioxide offers a promising avenue to produce valuable fuels and chemicals using greenhouse gas carbon dioxide as the carbon feedstock. Because industrial carbon dioxide point sources often contain numerous contaminants, such as nitrogen oxides, understanding the potential impact of contaminants on carbon dioxide electrolysis is crucial for practical applications. Herein, we investigate the impact of various nitrogen oxides, including nitric oxide, nitrogen dioxide, and nitrous oxide, on carbon dioxide electroreduction on three model electrocatalysts (i.e., copper, silver, and tin). We demonstrate that the presence of nitrogen oxides (up to 0.83%) in the carbon dioxide feed leads to a considerable Faradaic efficiency loss in carbon dioxide electroreduction, which is caused by the preferential electroreduction of nitrogen oxides over carbon dioxide. The primary products of nitrogen oxides electroreduction include nitrous oxide, nitrogen, hydroxylamine, and ammonia. Despite the loss in Faradaic efficiency, the electrocatalysts exhibit similar carbon dioxide reduction performances once a pure carbon dioxide feed is restored, indicating a negligible long-term impact of nitrogen oxides on the catalytic properties of the model catalysts.

Authors:
ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo
Publication Date:
Research Org.:
Univ. of Delaware, Newark, DE (United States); Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Sponsoring Org.:
USDOE Office of Fossil Energy (FE); National Science Foundation (NSF); USDOE Office of Science (SC)
OSTI Identifier:
1716536
Alternate Identifier(s):
OSTI ID: 1712672; OSTI ID: 1760530
Report Number(s):
BNL-220878-2021-JACI
Journal ID: ISSN 2041-1723; 5856; PII: 19731
Grant/Contract Number:  
FE0029868; SC0012704; CBET-1803200
Resource Type:
Published Article
Journal Name:
Nature Communications
Additional Journal Information:
Journal Name: Nature Communications Journal Volume: 11 Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United Kingdom
Language:
English
Subject:
carbon dioxide; electrocatalysts; electrochemical reduction; chemical engineering; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Ko, Byung Hee, Hasa, Bjorn, Shin, Haeun, Jeng, Emily, Overa, Sean, Chen, Wilson, and Jiao, Feng. The impact of nitrogen oxides on electrochemical carbon dioxide reduction. United Kingdom: N. p., 2020. Web. https://doi.org/10.1038/s41467-020-19731-8.
Ko, Byung Hee, Hasa, Bjorn, Shin, Haeun, Jeng, Emily, Overa, Sean, Chen, Wilson, & Jiao, Feng. The impact of nitrogen oxides on electrochemical carbon dioxide reduction. United Kingdom. https://doi.org/10.1038/s41467-020-19731-8
Ko, Byung Hee, Hasa, Bjorn, Shin, Haeun, Jeng, Emily, Overa, Sean, Chen, Wilson, and Jiao, Feng. Tue . "The impact of nitrogen oxides on electrochemical carbon dioxide reduction". United Kingdom. https://doi.org/10.1038/s41467-020-19731-8.
@article{osti_1716536,
title = {The impact of nitrogen oxides on electrochemical carbon dioxide reduction},
author = {Ko, Byung Hee and Hasa, Bjorn and Shin, Haeun and Jeng, Emily and Overa, Sean and Chen, Wilson and Jiao, Feng},
abstractNote = {The electroreduction of carbon dioxide offers a promising avenue to produce valuable fuels and chemicals using greenhouse gas carbon dioxide as the carbon feedstock. Because industrial carbon dioxide point sources often contain numerous contaminants, such as nitrogen oxides, understanding the potential impact of contaminants on carbon dioxide electrolysis is crucial for practical applications. Herein, we investigate the impact of various nitrogen oxides, including nitric oxide, nitrogen dioxide, and nitrous oxide, on carbon dioxide electroreduction on three model electrocatalysts (i.e., copper, silver, and tin). We demonstrate that the presence of nitrogen oxides (up to 0.83%) in the carbon dioxide feed leads to a considerable Faradaic efficiency loss in carbon dioxide electroreduction, which is caused by the preferential electroreduction of nitrogen oxides over carbon dioxide. The primary products of nitrogen oxides electroreduction include nitrous oxide, nitrogen, hydroxylamine, and ammonia. Despite the loss in Faradaic efficiency, the electrocatalysts exhibit similar carbon dioxide reduction performances once a pure carbon dioxide feed is restored, indicating a negligible long-term impact of nitrogen oxides on the catalytic properties of the model catalysts.},
doi = {10.1038/s41467-020-19731-8},
journal = {Nature Communications},
number = 1,
volume = 11,
place = {United Kingdom},
year = {2020},
month = {11}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1038/s41467-020-19731-8

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