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Vacancy-cluster-mediated surface activation for boosting CO(2) chemical fixation

The cycloaddition of CO(2) with epoxides towards cyclic carbonates provides a promising pathway for CO(2) utilization. Given the crucial role of epoxide ring opening in determining the reaction rate, designing catalysts with rich active sites for boosting epoxide adsorption and C–O bond cleavage is...

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Autores principales: Liu, Wenxiu, Li, Lei, Shao, Wei, Wang, Hui, Dong, Yun, Zuo, Ming, Liu, Jiandang, Zhang, Hongjun, Ye, Bangjiao, Zhang, Xiaodong, Xie, Yi
Formato: Online Artículo Texto
Lenguaje:English
Publicado: The Royal Society of Chemistry 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9906647/
https://www.ncbi.nlm.nih.gov/pubmed/36794176
http://dx.doi.org/10.1039/d2sc05596a
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author Liu, Wenxiu
Li, Lei
Shao, Wei
Wang, Hui
Dong, Yun
Zuo, Ming
Liu, Jiandang
Zhang, Hongjun
Ye, Bangjiao
Zhang, Xiaodong
Xie, Yi
author_facet Liu, Wenxiu
Li, Lei
Shao, Wei
Wang, Hui
Dong, Yun
Zuo, Ming
Liu, Jiandang
Zhang, Hongjun
Ye, Bangjiao
Zhang, Xiaodong
Xie, Yi
author_sort Liu, Wenxiu
collection PubMed
description The cycloaddition of CO(2) with epoxides towards cyclic carbonates provides a promising pathway for CO(2) utilization. Given the crucial role of epoxide ring opening in determining the reaction rate, designing catalysts with rich active sites for boosting epoxide adsorption and C–O bond cleavage is necessary for gaining efficient cyclic carbonate generation. Herein, by taking two-dimensional FeOCl as a model, we propose the construction of electron-donor and -acceptor units within a confined region via vacancy-cluster engineering to boost epoxide ring opening. By combing theoretical simulations and in situ diffuse reflectance infrared Fourier-transform spectroscopy, we show that the introduction of Fe–Cl vacancy clusters can activate the inert halogen-terminated surface and provide reactive sites containing electron-donor and -acceptor units, leading to strengthened epoxide adsorption and promoted C–O bond cleavage. Benefiting from these, FeOCl nanosheets with Fe–Cl vacancy clusters exhibit enhanced cyclic carbonate generation from CO(2) cycloaddition with epoxides.
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spelling pubmed-99066472023-02-14 Vacancy-cluster-mediated surface activation for boosting CO(2) chemical fixation Liu, Wenxiu Li, Lei Shao, Wei Wang, Hui Dong, Yun Zuo, Ming Liu, Jiandang Zhang, Hongjun Ye, Bangjiao Zhang, Xiaodong Xie, Yi Chem Sci Chemistry The cycloaddition of CO(2) with epoxides towards cyclic carbonates provides a promising pathway for CO(2) utilization. Given the crucial role of epoxide ring opening in determining the reaction rate, designing catalysts with rich active sites for boosting epoxide adsorption and C–O bond cleavage is necessary for gaining efficient cyclic carbonate generation. Herein, by taking two-dimensional FeOCl as a model, we propose the construction of electron-donor and -acceptor units within a confined region via vacancy-cluster engineering to boost epoxide ring opening. By combing theoretical simulations and in situ diffuse reflectance infrared Fourier-transform spectroscopy, we show that the introduction of Fe–Cl vacancy clusters can activate the inert halogen-terminated surface and provide reactive sites containing electron-donor and -acceptor units, leading to strengthened epoxide adsorption and promoted C–O bond cleavage. Benefiting from these, FeOCl nanosheets with Fe–Cl vacancy clusters exhibit enhanced cyclic carbonate generation from CO(2) cycloaddition with epoxides. The Royal Society of Chemistry 2022-12-13 /pmc/articles/PMC9906647/ /pubmed/36794176 http://dx.doi.org/10.1039/d2sc05596a Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by-nc/3.0/
spellingShingle Chemistry
Liu, Wenxiu
Li, Lei
Shao, Wei
Wang, Hui
Dong, Yun
Zuo, Ming
Liu, Jiandang
Zhang, Hongjun
Ye, Bangjiao
Zhang, Xiaodong
Xie, Yi
Vacancy-cluster-mediated surface activation for boosting CO(2) chemical fixation
title Vacancy-cluster-mediated surface activation for boosting CO(2) chemical fixation
title_full Vacancy-cluster-mediated surface activation for boosting CO(2) chemical fixation
title_fullStr Vacancy-cluster-mediated surface activation for boosting CO(2) chemical fixation
title_full_unstemmed Vacancy-cluster-mediated surface activation for boosting CO(2) chemical fixation
title_short Vacancy-cluster-mediated surface activation for boosting CO(2) chemical fixation
title_sort vacancy-cluster-mediated surface activation for boosting co(2) chemical fixation
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9906647/
https://www.ncbi.nlm.nih.gov/pubmed/36794176
http://dx.doi.org/10.1039/d2sc05596a
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