Promoting the activity of Ce-incorporated MOR in dimethyl ether carbonylation through tailoring the distribution of Bronsted acids

被引：66

作者：

Li, Ying ^{[1
]}

Huang, Shouying ^{[1
]}

Cheng, Zaizhe ^{[1
]}

Cai, Kai ^{[1
]}

Li, Landong ^{[2
,3
]}

Milan, Emile ^{[4
]}

Lv, Jing ^{[1
]}

Wang, Yue ^{[1
]}

Sun, Qi ^{[1
]}

Ma, Xinbin ^{[1
]}

机构：

[1] Tianjin Univ, Sch Chem Engn & Technol, Collaborat Innovat Ctr Chem Sci & Engn, Key Lab Green Chem Technol,Minist Educ, Tianjin 300350, Peoples R China

[2] Nankai Univ, Sch Mat Sci & Engn, Tianjin 300350, Peoples R China

[3] Nankai Univ, Natl Inst Adv Mat, Tianjin 300350, Peoples R China

[4] Univ Ottawa, Sch Informat Technol & Engn, 800 King Edward Ave, Ottawa, ON, Canada

来源：

APPLIED CATALYSIS B-ENVIRONMENTAL | 2019年 / 256卷

基金：

中国国家自然科学基金;

关键词：

H-MOR; Heteroatom substitution; Al sitting; Bronsted acid site distribution; Carbonylation reaction; CATALYTIC CARBONYLATION; SELECTIVE CARBONYLATION; MORDENITE ZEOLITE; ETHANOL SYNTHESIS; METHYL ACETATE; MCM-22; ZEOLITE; MFI ZEOLITES; H-MORDENITE; IRMS-TPD; SYNGAS;

D O I：

10.1016/j.apcatb.2019.117777

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

As Bronsted acid site (BAS) located in 8-membered ring (8-MR) of zeolite is accepted as the exclusive active site for dimethyl ether carbonylation to methyl acetate, tailoring the distribution of tetrahedral Al in zeolite channels is important to improve catalytic performance. In this work, a series of Ce-containing mordenite were synthesized by one-step hydrothermal method. By a combination of mutually complementary characterization techniques (e.g. XPS, UV-vis, Raman, acidity characterizations etc.), it is confirmed that Ce atoms incorporated into the zeolite framework as Ce3+ species, resulting in an enrichment of BAS in the 8-MR. Acid strength, apparent activation energy and DFT calculations revealed that the incorporation of Ce resulted in an increase of Si-OH-Al in the 8-MR, which was responsible for the improved activity. This work provides a facile way to tailor the acidic concentration and distribution of zeolites, which is able to guide rational design of zeolites for the shape-selective catalysis.

引用

页数：12

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