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Electrochemical ammonia synthesis by reduction of nitrate on Au doped Cu nanowires
Electrochemical nitrate reduction reaction (NO(3)(−)RR) to synthesize valuable ammonia (NH(3)) is considered as a green and appealing alternative to enable an artificial nitrogen cycle. However, as there are other NO(3)(−)RR pathways present, selectively guiding the reaction pathway towards NH(3) is...
Autores principales: | , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
The Royal Society of Chemistry
2023
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10043758/ https://www.ncbi.nlm.nih.gov/pubmed/36998524 http://dx.doi.org/10.1039/d3ra00679d |
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author | Zha, Yuankang Liu, Min Wang, Jinlu Feng, Jiyu Li, Daopeng Zhao, Dongnan Zhang, Shengbo Shi, Tongfei |
author_facet | Zha, Yuankang Liu, Min Wang, Jinlu Feng, Jiyu Li, Daopeng Zhao, Dongnan Zhang, Shengbo Shi, Tongfei |
author_sort | Zha, Yuankang |
collection | PubMed |
description | Electrochemical nitrate reduction reaction (NO(3)(−)RR) to synthesize valuable ammonia (NH(3)) is considered as a green and appealing alternative to enable an artificial nitrogen cycle. However, as there are other NO(3)(−)RR pathways present, selectively guiding the reaction pathway towards NH(3) is currently challenged by the lack of efficient catalyst. Here, we demonstrate a novel electrocatalyst for NO(3)(−)RR consisting of Au doped Cu nanowires on a copper foam (CF) electrode (Au–Cu NWs/CF), which delivers a remarkable NH(3) yield rate of 5336.0 ± 159.2 μg h(−1) cm(−2) and an exceptional faradaic efficiency (FE) of 84.1 ± 1.0% at −1.05 V (vs. RHE). The (15)N isotopic labelling experiments confirm that the yielded NH(3) is indeed from the Au–Cu NWs/CF catalyzed NO(3)(−)RR process. The XPS analysis and in situ infrared spectroscopy (IR) spectroscopy characterization results indicated that the electron transfer between the Cu and Au interface and oxygen vacancy synergistically decreased the reduction reaction barrier and inhibited the generation of hydrogen in the competitive reaction, resulting in a high conversion, selectivity and FE for NO(3)(−)RR. This work not only develops a powerful strategy for the rational design of robust and efficient catalysts by defect engineering, but also provides new insights for selective nitrate electroreduction to NH(3). |
format | Online Article Text |
id | pubmed-10043758 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | The Royal Society of Chemistry |
record_format | MEDLINE/PubMed |
spelling | pubmed-100437582023-03-29 Electrochemical ammonia synthesis by reduction of nitrate on Au doped Cu nanowires Zha, Yuankang Liu, Min Wang, Jinlu Feng, Jiyu Li, Daopeng Zhao, Dongnan Zhang, Shengbo Shi, Tongfei RSC Adv Chemistry Electrochemical nitrate reduction reaction (NO(3)(−)RR) to synthesize valuable ammonia (NH(3)) is considered as a green and appealing alternative to enable an artificial nitrogen cycle. However, as there are other NO(3)(−)RR pathways present, selectively guiding the reaction pathway towards NH(3) is currently challenged by the lack of efficient catalyst. Here, we demonstrate a novel electrocatalyst for NO(3)(−)RR consisting of Au doped Cu nanowires on a copper foam (CF) electrode (Au–Cu NWs/CF), which delivers a remarkable NH(3) yield rate of 5336.0 ± 159.2 μg h(−1) cm(−2) and an exceptional faradaic efficiency (FE) of 84.1 ± 1.0% at −1.05 V (vs. RHE). The (15)N isotopic labelling experiments confirm that the yielded NH(3) is indeed from the Au–Cu NWs/CF catalyzed NO(3)(−)RR process. The XPS analysis and in situ infrared spectroscopy (IR) spectroscopy characterization results indicated that the electron transfer between the Cu and Au interface and oxygen vacancy synergistically decreased the reduction reaction barrier and inhibited the generation of hydrogen in the competitive reaction, resulting in a high conversion, selectivity and FE for NO(3)(−)RR. This work not only develops a powerful strategy for the rational design of robust and efficient catalysts by defect engineering, but also provides new insights for selective nitrate electroreduction to NH(3). The Royal Society of Chemistry 2023-03-28 /pmc/articles/PMC10043758/ /pubmed/36998524 http://dx.doi.org/10.1039/d3ra00679d Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by/3.0/ |
spellingShingle | Chemistry Zha, Yuankang Liu, Min Wang, Jinlu Feng, Jiyu Li, Daopeng Zhao, Dongnan Zhang, Shengbo Shi, Tongfei Electrochemical ammonia synthesis by reduction of nitrate on Au doped Cu nanowires |
title | Electrochemical ammonia synthesis by reduction of nitrate on Au doped Cu nanowires |
title_full | Electrochemical ammonia synthesis by reduction of nitrate on Au doped Cu nanowires |
title_fullStr | Electrochemical ammonia synthesis by reduction of nitrate on Au doped Cu nanowires |
title_full_unstemmed | Electrochemical ammonia synthesis by reduction of nitrate on Au doped Cu nanowires |
title_short | Electrochemical ammonia synthesis by reduction of nitrate on Au doped Cu nanowires |
title_sort | electrochemical ammonia synthesis by reduction of nitrate on au doped cu nanowires |
topic | Chemistry |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10043758/ https://www.ncbi.nlm.nih.gov/pubmed/36998524 http://dx.doi.org/10.1039/d3ra00679d |
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