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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...
Autores principales: | , , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
The Royal Society of Chemistry
2020
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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. |
format | Online Article Text |
id | pubmed-8179658 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2020 |
publisher | The Royal Society of Chemistry |
record_format | MEDLINE/PubMed |
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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