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Multi-heterointerfaces for selective and efficient urea production

A major impediment to industrial urea synthesis is the lack of catalysts with high selectivity and activity, which inhibits the efficient industrial production of urea. Here, we report a new catalyst system suitable for the highly selective synthesis of industrial urea by in situ growth of graphdiyn...

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Autores principales: Zhang, Danyan, Xue, Yurui, Zheng, Xuchen, Zhang, Chao, Li, Yuliang
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Oxford University Press 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9935990/
https://www.ncbi.nlm.nih.gov/pubmed/36817842
http://dx.doi.org/10.1093/nsr/nwac209
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author Zhang, Danyan
Xue, Yurui
Zheng, Xuchen
Zhang, Chao
Li, Yuliang
author_facet Zhang, Danyan
Xue, Yurui
Zheng, Xuchen
Zhang, Chao
Li, Yuliang
author_sort Zhang, Danyan
collection PubMed
description A major impediment to industrial urea synthesis is the lack of catalysts with high selectivity and activity, which inhibits the efficient industrial production of urea. Here, we report a new catalyst system suitable for the highly selective synthesis of industrial urea by in situ growth of graphdiyne on the surface of cobalt–nickel mixed oxides. Such a catalyst is a multi-heterojunction interfacial structure resulting in the obvious incomplete charge-transfer phenomenon between a graphdiyne and metal oxide interface and multiple intermolecular interactions. These intrinsic characteristics are the origin of the high performance of the catalyst. Studies on the mechanism reveal that the catalyst could effectively optimize the adsorption/desorption capacities of the intermediate and promote direct C–N coupling by significantly suppressing by-product reactions toward the formation of H(2), CO, N(2) and NH(3). The catalyst can selectively synthesize urea directly from nitrite and carbon dioxide in water at room temperature and pressure, and exhibits a record-high Faradaic efficiency of 64.3%, nitrogen selectivity (N(urea)-selectivity) of 86.0%, carbon selectivity (C(urea)-selectivity) of ∼100%, as well as urea yield rates of 913.2 μg h(−1) mg(cat)(−1) and remarkable long-term stability.
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spelling pubmed-99359902023-02-18 Multi-heterointerfaces for selective and efficient urea production Zhang, Danyan Xue, Yurui Zheng, Xuchen Zhang, Chao Li, Yuliang Natl Sci Rev Research Article A major impediment to industrial urea synthesis is the lack of catalysts with high selectivity and activity, which inhibits the efficient industrial production of urea. Here, we report a new catalyst system suitable for the highly selective synthesis of industrial urea by in situ growth of graphdiyne on the surface of cobalt–nickel mixed oxides. Such a catalyst is a multi-heterojunction interfacial structure resulting in the obvious incomplete charge-transfer phenomenon between a graphdiyne and metal oxide interface and multiple intermolecular interactions. These intrinsic characteristics are the origin of the high performance of the catalyst. Studies on the mechanism reveal that the catalyst could effectively optimize the adsorption/desorption capacities of the intermediate and promote direct C–N coupling by significantly suppressing by-product reactions toward the formation of H(2), CO, N(2) and NH(3). The catalyst can selectively synthesize urea directly from nitrite and carbon dioxide in water at room temperature and pressure, and exhibits a record-high Faradaic efficiency of 64.3%, nitrogen selectivity (N(urea)-selectivity) of 86.0%, carbon selectivity (C(urea)-selectivity) of ∼100%, as well as urea yield rates of 913.2 μg h(−1) mg(cat)(−1) and remarkable long-term stability. Oxford University Press 2022-10-04 /pmc/articles/PMC9935990/ /pubmed/36817842 http://dx.doi.org/10.1093/nsr/nwac209 Text en © The Author(s) 2022. Published by Oxford University Press on behalf of China Science Publishing & Media Ltd. https://creativecommons.org/licenses/by/4.0/This is an Open Access article distributed under the terms of the Creative Commons Attribution License (https://creativecommons.org/licenses/by/4.0/), which permits unrestricted reuse, distribution, and reproduction in any medium, provided the original work is properly cited.
spellingShingle Research Article
Zhang, Danyan
Xue, Yurui
Zheng, Xuchen
Zhang, Chao
Li, Yuliang
Multi-heterointerfaces for selective and efficient urea production
title Multi-heterointerfaces for selective and efficient urea production
title_full Multi-heterointerfaces for selective and efficient urea production
title_fullStr Multi-heterointerfaces for selective and efficient urea production
title_full_unstemmed Multi-heterointerfaces for selective and efficient urea production
title_short Multi-heterointerfaces for selective and efficient urea production
title_sort multi-heterointerfaces for selective and efficient urea production
topic Research Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9935990/
https://www.ncbi.nlm.nih.gov/pubmed/36817842
http://dx.doi.org/10.1093/nsr/nwac209
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