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Enhancement of the dimethyl ether carbonylation activation via regulating acid sites distribution in FER zeolite framework

The carbonylation of dimethyl ether (DME) with CO is a key step for ethanol synthesis from syngas, but traditional mordenite (MOR) zeolite shows low catalytic stability. Herein, various FER zeolite nanosheets were prepared with four types of organic templates. The catalytic performance of FER in DME...

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Detalles Bibliográficos
Autores principales: Guo, Yanxia, Wang, Sen, Geng, Rui, Wang, Pengfei, Li, Shiying, Dong, Mei, Qin, Zhangfeng, Wang, Jianguo, Fan, Weibin
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Elsevier 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10494173/
https://www.ncbi.nlm.nih.gov/pubmed/37701576
http://dx.doi.org/10.1016/j.isci.2023.107748
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author Guo, Yanxia
Wang, Sen
Geng, Rui
Wang, Pengfei
Li, Shiying
Dong, Mei
Qin, Zhangfeng
Wang, Jianguo
Fan, Weibin
author_facet Guo, Yanxia
Wang, Sen
Geng, Rui
Wang, Pengfei
Li, Shiying
Dong, Mei
Qin, Zhangfeng
Wang, Jianguo
Fan, Weibin
author_sort Guo, Yanxia
collection PubMed
description The carbonylation of dimethyl ether (DME) with CO is a key step for ethanol synthesis from syngas, but traditional mordenite (MOR) zeolite shows low catalytic stability. Herein, various FER zeolite nanosheets were prepared with four types of organic templates. The catalytic performance of FER in DME carbonylation is strongly dependent on the location of strong acid site in framework, which can be effectively regulated by altering organic template. FER-MORP sample synthesized with morpholine shows the highest DME conversion of 53%, thus, giving a methyl acetate space-time yield (STY(MA)) of 0.889 mmol g(–1) h(–1). DFT calculation, NH(3)-IR, (1)H/(27)Al/(29)Si MAS NMR, and in situ DRIFTS results indicate that morpholine directs more Al species, or strong Brønsted acid sites (BAS), to locate in 8-membered ring (8-MR) channels, which not only enhances carbonylation activity but also suppresses formation of coke species. The catalytic performance is well maintained within 4 repeated recycles (∼460 h).
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spelling pubmed-104941732023-09-12 Enhancement of the dimethyl ether carbonylation activation via regulating acid sites distribution in FER zeolite framework Guo, Yanxia Wang, Sen Geng, Rui Wang, Pengfei Li, Shiying Dong, Mei Qin, Zhangfeng Wang, Jianguo Fan, Weibin iScience Article The carbonylation of dimethyl ether (DME) with CO is a key step for ethanol synthesis from syngas, but traditional mordenite (MOR) zeolite shows low catalytic stability. Herein, various FER zeolite nanosheets were prepared with four types of organic templates. The catalytic performance of FER in DME carbonylation is strongly dependent on the location of strong acid site in framework, which can be effectively regulated by altering organic template. FER-MORP sample synthesized with morpholine shows the highest DME conversion of 53%, thus, giving a methyl acetate space-time yield (STY(MA)) of 0.889 mmol g(–1) h(–1). DFT calculation, NH(3)-IR, (1)H/(27)Al/(29)Si MAS NMR, and in situ DRIFTS results indicate that morpholine directs more Al species, or strong Brønsted acid sites (BAS), to locate in 8-membered ring (8-MR) channels, which not only enhances carbonylation activity but also suppresses formation of coke species. The catalytic performance is well maintained within 4 repeated recycles (∼460 h). Elsevier 2023-08-28 /pmc/articles/PMC10494173/ /pubmed/37701576 http://dx.doi.org/10.1016/j.isci.2023.107748 Text en © 2023 The Author(s) https://creativecommons.org/licenses/by-nc-nd/4.0/This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
spellingShingle Article
Guo, Yanxia
Wang, Sen
Geng, Rui
Wang, Pengfei
Li, Shiying
Dong, Mei
Qin, Zhangfeng
Wang, Jianguo
Fan, Weibin
Enhancement of the dimethyl ether carbonylation activation via regulating acid sites distribution in FER zeolite framework
title Enhancement of the dimethyl ether carbonylation activation via regulating acid sites distribution in FER zeolite framework
title_full Enhancement of the dimethyl ether carbonylation activation via regulating acid sites distribution in FER zeolite framework
title_fullStr Enhancement of the dimethyl ether carbonylation activation via regulating acid sites distribution in FER zeolite framework
title_full_unstemmed Enhancement of the dimethyl ether carbonylation activation via regulating acid sites distribution in FER zeolite framework
title_short Enhancement of the dimethyl ether carbonylation activation via regulating acid sites distribution in FER zeolite framework
title_sort enhancement of the dimethyl ether carbonylation activation via regulating acid sites distribution in fer zeolite framework
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10494173/
https://www.ncbi.nlm.nih.gov/pubmed/37701576
http://dx.doi.org/10.1016/j.isci.2023.107748
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