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Cooperative catalytically active sites for methanol activation by single metal ion-doped H-ZSM-5

Catalytic conversion of methanol to aromatics and hydrocarbons is regarded as a key alternative technology to oil processing. Although the inclusion of foreign metal species in H-ZSM-5 containing Brønsted acid site (BAS) is commonly found to enhance product yields, the nature of catalytically active...

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Autores principales: Lin, Wei-Che, Wu, Simson, Li, Guangchao, Ho, Ping-Luen, Ye, Yichen, Zhao, Pu, Day, Sarah, Tang, Chiu, Chen, Wei, Zheng, Anmin, Lo, Benedict T. W., Edman Tsang, Shik Chi
Formato: Online Artículo Texto
Lenguaje:English
Publicado: The Royal Society of Chemistry 2020
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8179658/
https://www.ncbi.nlm.nih.gov/pubmed/34168741
http://dx.doi.org/10.1039/d0sc04058d
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author Lin, Wei-Che
Wu, Simson
Li, Guangchao
Ho, Ping-Luen
Ye, Yichen
Zhao, Pu
Day, Sarah
Tang, Chiu
Chen, Wei
Zheng, Anmin
Lo, Benedict T. W.
Edman Tsang, Shik Chi
author_facet Lin, Wei-Che
Wu, Simson
Li, Guangchao
Ho, Ping-Luen
Ye, Yichen
Zhao, Pu
Day, Sarah
Tang, Chiu
Chen, Wei
Zheng, Anmin
Lo, Benedict T. W.
Edman Tsang, Shik Chi
author_sort Lin, Wei-Che
collection PubMed
description Catalytic conversion of methanol to aromatics and hydrocarbons is regarded as a key alternative technology to oil processing. Although the inclusion of foreign metal species in H-ZSM-5 containing Brønsted acid site (BAS) is commonly found to enhance product yields, the nature of catalytically active sites and the rationalization for catalytic performance still remain obscure. Herein, by acquiring comparable structural parameters by both X-ray and neutron powder diffractions over a number of metal-modified ZSM-5 zeolites, it is demonstrated for the first time that active pairs of metal site-BAS within molecular distance is created when single and isolated transition metal cation is ion-exchanged with the zeolites. According to our DFT model, this could lead to the initial heterolytic cleavage of small molecules such as water and methanol by the pair with subsequent reactions to form products at high selectivity as that observed experimentally. It may account for their active and selective catalytic routes of small molecule activations.
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spelling pubmed-81796582021-06-23 Cooperative catalytically active sites for methanol activation by single metal ion-doped H-ZSM-5 Lin, Wei-Che Wu, Simson Li, Guangchao Ho, Ping-Luen Ye, Yichen Zhao, Pu Day, Sarah Tang, Chiu Chen, Wei Zheng, Anmin Lo, Benedict T. W. Edman Tsang, Shik Chi Chem Sci Chemistry Catalytic conversion of methanol to aromatics and hydrocarbons is regarded as a key alternative technology to oil processing. Although the inclusion of foreign metal species in H-ZSM-5 containing Brønsted acid site (BAS) is commonly found to enhance product yields, the nature of catalytically active sites and the rationalization for catalytic performance still remain obscure. Herein, by acquiring comparable structural parameters by both X-ray and neutron powder diffractions over a number of metal-modified ZSM-5 zeolites, it is demonstrated for the first time that active pairs of metal site-BAS within molecular distance is created when single and isolated transition metal cation is ion-exchanged with the zeolites. According to our DFT model, this could lead to the initial heterolytic cleavage of small molecules such as water and methanol by the pair with subsequent reactions to form products at high selectivity as that observed experimentally. It may account for their active and selective catalytic routes of small molecule activations. The Royal Society of Chemistry 2020-10-21 /pmc/articles/PMC8179658/ /pubmed/34168741 http://dx.doi.org/10.1039/d0sc04058d Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by-nc/3.0/
spellingShingle Chemistry
Lin, Wei-Che
Wu, Simson
Li, Guangchao
Ho, Ping-Luen
Ye, Yichen
Zhao, Pu
Day, Sarah
Tang, Chiu
Chen, Wei
Zheng, Anmin
Lo, Benedict T. W.
Edman Tsang, Shik Chi
Cooperative catalytically active sites for methanol activation by single metal ion-doped H-ZSM-5
title Cooperative catalytically active sites for methanol activation by single metal ion-doped H-ZSM-5
title_full Cooperative catalytically active sites for methanol activation by single metal ion-doped H-ZSM-5
title_fullStr Cooperative catalytically active sites for methanol activation by single metal ion-doped H-ZSM-5
title_full_unstemmed Cooperative catalytically active sites for methanol activation by single metal ion-doped H-ZSM-5
title_short Cooperative catalytically active sites for methanol activation by single metal ion-doped H-ZSM-5
title_sort cooperative catalytically active sites for methanol activation by single metal ion-doped h-zsm-5
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8179658/
https://www.ncbi.nlm.nih.gov/pubmed/34168741
http://dx.doi.org/10.1039/d0sc04058d
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