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Electrochemical C–N coupling with perovskite hybrids toward efficient urea synthesis
Electrocatalytic C–N coupling reaction by co-activation of both N(2) and CO(2) molecules under ambient conditions to synthesize valuable urea opens a new avenue for sustainable development, while the actual catalytic activity is limited by poor adsorption and coupling capability of gas molecules on...
Autores principales: | , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
The Royal Society of Chemistry
2021
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8098680/ https://www.ncbi.nlm.nih.gov/pubmed/33996000 http://dx.doi.org/10.1039/d1sc01467f |
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author | Yuan, Menglei Chen, Junwu Bai, Yiling Liu, Zhanjun Zhang, Jingxian Zhao, Tongkun Shi, Qiaona Li, Shuwei Wang, Xi Zhang, Guangjin |
author_facet | Yuan, Menglei Chen, Junwu Bai, Yiling Liu, Zhanjun Zhang, Jingxian Zhao, Tongkun Shi, Qiaona Li, Shuwei Wang, Xi Zhang, Guangjin |
author_sort | Yuan, Menglei |
collection | PubMed |
description | Electrocatalytic C–N coupling reaction by co-activation of both N(2) and CO(2) molecules under ambient conditions to synthesize valuable urea opens a new avenue for sustainable development, while the actual catalytic activity is limited by poor adsorption and coupling capability of gas molecules on the catalyst surface. Herein, theoretical calculation predicts that the well-developed built-in electric field in perovskite hetero-structured BiFeO(3)/BiVO(4) hybrids can accelerate the local charge redistribution and thus promote the targeted adsorption and activation of inert N(2) and CO(2) molecules on the generated local electrophilic and nucleophilic regions. Thus, a BiFeO(3)/BiVO(4) heterojunction is designed and synthesized, which delivers a urea yield rate of 4.94 mmol h(−1) g(−1) with a faradaic efficiency of 17.18% at −0.4 V vs. RHE in 0.1 M KHCO(3), outperforming the highest values reported as far. The comprehensive analysis further confirms that the local charge redistribution in the heterojunction effectively suppresses CO poisoning and the formation of the endothermic *NNH intermediate, which thus guarantees the exothermic coupling of *N[double bond, length as m-dash]N* intermediates with the generated CO via C–N coupling reactions to form the urea precursor *NCON* intermediate. This work opens a new avenue for effective electrocatalytic C–N coupling under ambient conditions. |
format | Online Article Text |
id | pubmed-8098680 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2021 |
publisher | The Royal Society of Chemistry |
record_format | MEDLINE/PubMed |
spelling | pubmed-80986802021-05-13 Electrochemical C–N coupling with perovskite hybrids toward efficient urea synthesis Yuan, Menglei Chen, Junwu Bai, Yiling Liu, Zhanjun Zhang, Jingxian Zhao, Tongkun Shi, Qiaona Li, Shuwei Wang, Xi Zhang, Guangjin Chem Sci Chemistry Electrocatalytic C–N coupling reaction by co-activation of both N(2) and CO(2) molecules under ambient conditions to synthesize valuable urea opens a new avenue for sustainable development, while the actual catalytic activity is limited by poor adsorption and coupling capability of gas molecules on the catalyst surface. Herein, theoretical calculation predicts that the well-developed built-in electric field in perovskite hetero-structured BiFeO(3)/BiVO(4) hybrids can accelerate the local charge redistribution and thus promote the targeted adsorption and activation of inert N(2) and CO(2) molecules on the generated local electrophilic and nucleophilic regions. Thus, a BiFeO(3)/BiVO(4) heterojunction is designed and synthesized, which delivers a urea yield rate of 4.94 mmol h(−1) g(−1) with a faradaic efficiency of 17.18% at −0.4 V vs. RHE in 0.1 M KHCO(3), outperforming the highest values reported as far. The comprehensive analysis further confirms that the local charge redistribution in the heterojunction effectively suppresses CO poisoning and the formation of the endothermic *NNH intermediate, which thus guarantees the exothermic coupling of *N[double bond, length as m-dash]N* intermediates with the generated CO via C–N coupling reactions to form the urea precursor *NCON* intermediate. This work opens a new avenue for effective electrocatalytic C–N coupling under ambient conditions. The Royal Society of Chemistry 2021-04-12 /pmc/articles/PMC8098680/ /pubmed/33996000 http://dx.doi.org/10.1039/d1sc01467f Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by/3.0/ |
spellingShingle | Chemistry Yuan, Menglei Chen, Junwu Bai, Yiling Liu, Zhanjun Zhang, Jingxian Zhao, Tongkun Shi, Qiaona Li, Shuwei Wang, Xi Zhang, Guangjin Electrochemical C–N coupling with perovskite hybrids toward efficient urea synthesis |
title | Electrochemical C–N coupling with perovskite hybrids toward efficient urea synthesis |
title_full | Electrochemical C–N coupling with perovskite hybrids toward efficient urea synthesis |
title_fullStr | Electrochemical C–N coupling with perovskite hybrids toward efficient urea synthesis |
title_full_unstemmed | Electrochemical C–N coupling with perovskite hybrids toward efficient urea synthesis |
title_short | Electrochemical C–N coupling with perovskite hybrids toward efficient urea synthesis |
title_sort | electrochemical c–n coupling with perovskite hybrids toward efficient urea synthesis |
topic | Chemistry |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8098680/ https://www.ncbi.nlm.nih.gov/pubmed/33996000 http://dx.doi.org/10.1039/d1sc01467f |
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