期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 10, 期 15, 页码 8334-8343出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d2ta00451h
关键词
-
资金
- Key Research Program of Frontier Sciences, Chinese Academy of Sciences [QYZDB-SSW-JSC040]
- National Natural Science Foundation of China [21991090, 21991091]
- Sino-French International Laboratory (LIA) Zeolites
This study designed a series of bulky gemini-type bis(methylpyrrolidinium) dications as efficient OSDAs for MOR zeolite, improving the distribution of acid sites in the side pockets of MOR and enhancing the catalytic activity in the DME carbonylation reaction.
Mordenite (MOR) zeolite is an efficient catalyst for dimethyl ether (DME) carbonylation and syngas to ethylene conversion due to the unique confinement effect and catalytic activity in 8-membered ring (8-MR) side pockets. Herein, aiming at enhancing the distribution of acid sites in the side pockets of MOR and developing high-performance catalysts, a series of bulky gemini-type bis(methylpyrrolidinium) dications with varying methylene chain lengths (nBMPr) were designed and proved to be efficient OSDAs for MOR zeolite. The synthesis efficacy of nBMPr was revealed to be closely related with the methylene chain lengths. Compared with conventional MOR templated by tetraethylammonium hydroxide (TEAOH), nBMPr-MOR possessed an obviously enhanced Bronsted acid distribution and amounts in the side pockets, likely due to the higher charge compensation ability of nBMPr for the framework [AlO4](-) of 12-MR, promoting the preferential location of Na+ in the side pockets. Consequently, the resultant MOR zeolites showed remarkable catalytic activity in the DME carbonylation reaction. The space-time yield of methyl acetate can reach as high as 12.5 mmol g(-1) h(-1), which is the highest value ever reported for DME carbonylation using zeolitic catalysts.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据