Lewis Acid Catalysis Confined in Zeolite Cages as a Strategy for Sustainable Heterogeneous Hydration of Epoxides

被引：99

作者：

Dai, Weili ^{[1
,2
,3
]}

Wang, Chuanming ^{[4
]}

Tang, Bo ^{[1
,2
]}

Wu, Guangjun ^{[1
,2
,3
]}

Guan, Naijia ^{[1
,2
,3
]}

Xie, Zaiku ^{[4
]}

Hunger, Michael ^{[5
]}

Li, Landong ^{[1
,2
,3
]}

机构：

[1] Nankai Univ, Sch Mat Sci & Engn, Tianjin 300071, Peoples R China

[2] Nankai Univ, Natl Inst Adv Mat, Tianjin 300071, Peoples R China

[3] Nankai Univ, Collaborat Innovat Ctr Chem Sci & Engn, Minist Educ, Key Lab Adv Energy Mat Chem, Tianjin 300071, Peoples R China

[4] SINOPEC Shanghai Res Inst Petrochem Technol, Shanghai 201208, Peoples R China

[5] Univ Stuttgart, Inst Chem Technol, D-70550 Stuttgart, Germany

来源：

ACS CATALYSIS | 2016年 / 6卷 / 05期

基金：

中国国家自然科学基金;

关键词：

Lewis acid catalysis; Sn-H-SSZ-13; shape-selective; epoxide hydration; partially hydroxylated Sn species; SN-BETA ZEOLITES; SOLID-STATE NMR; ETHYLENE-OXIDE; LACTIC-ACID; TIN; ISOMERIZATION; CONVERSION; SITES; GLUCOSE; SUGARS;

D O I：

10.1021/acscatal.5b02823

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：

We report a heterogeneous catalysis strategy to the sustainable hydration of epoxides by designing robust Lewis acid catalysts confined in zeolite cages as natural shape-selective nanoreactors. In the case of ethylene oxide hydration, Sn-H-SSZ-13 zeolite exhibits remarkable catalytic performance, with an ethylene oxide conversion above 99% and a monoethylene glycol selectivity above 99%, at approaching stoichiometric water/ethylene oxide ratios and near-ambient reaction temperatures. It is revealed by theoretical studies that partially hydroxylated Sn species are the preferred Lewis acid sites for the hydration of ethylene oxide. The concept of Lewis acid catalysis confined in zeolite cages may be applied in the future in the chemical industry to develop energy-saving and environmentally benign processes.

引用

页码：2955 / 2964

页数：10

共 57 条

[1] Theoretical and experimental study of the 13C chemical shift tensors of acetone complexed with Bronsted and Lewis acids [J].

Barich, DH ;

Nicholas, JB ;

Xu, T ;

Haw, JF .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1998, 120 (47) :12342-12350

[2] Metalloenzyme-like catalyzed isomerizations of sugars by Lewis acid zeolites [J].

Bermejo-Deval, Ricardo ;

Assary, Rajeev S. ;

Nikolla, Eranda ;

Moliner, Manuel ;

Roman-Leshkov, Yuriy ;

Hwang, Son-Jong ;

Palsdottir, Arna ;

Silverman, Dorothy ;

Lobo, Raul F. ;

Curtiss, Larry A. ;

Davis, Mark E. .

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2012, 109 (25) :9727-9732

[3] Determination of the catalytically active oxidation Lewis acid sites in Sn-beta zeolites, and their optimisation by the combination of theoretical and experimental studies [J].

Boronat, M ;

Concepción, P ;

Corma, A ;

Renz, M ;

Valencia, S .

JOURNAL OF CATALYSIS, 2005, 234 (01) :111-118

[4] Production of p-Xylene from Biomass by Catalytic Fast Pyrolysis Using ZSM-5 Catalysts with Reduced Pore Openings [J].

Cheng, Yu-Ting ;

Wang, Zhuopeng ;

Gilbert, Christopher J. ;

Fan, Wei ;

Huber, George W. .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2012, 51 (44) :11097-11100

[5] Synthesis of Hierarchical Sn-MFI as Lewis Acid Catalysts for Isomerization of Cellulosic Sugars [J].

Cho, Hong Je ;

Dornath, Paul ;

Fan, Wei .

ACS CATALYSIS, 2014, 4 (06) :2029-2037

[6]

CHRISTEN JD, 1985, Patent No. 4521548

[7] AI-free Sn-beta zeolite as a catalyst for the selective reduction of carbonyl compounds (Meerwein-Ponndorf-Verley reaction) [J].

Corma, A ;

Domine, ME ;

Nemeth, L ;

Valencia, S .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2002, 124 (13) :3194-3195

[8] Sn-zeolite beta as a heterogeneous chemoselective catalyst for Baeyer-Villiger oxidations [J].

Corma, A ;

Nemeth, LT ;

Renz, M ;

Valencia, S .

NATURE, 2001, 412 (6845) :423-425

[9] Verifying the mechanism of the ethene-to-propene conversion on zeolite H-SSZ-13 [J].

Dai, Weili ;

Sun, Xiaoming ;

Tang, Bo ;

Wu, Guangjun ;

Li, Landong ;

Guan, Naijia ;

Hunger, Michael .

JOURNAL OF CATALYSIS, 2014, 314 :10-20

[10] Methanol-to-Olefin Conversion Catalyzed by Low-Silica AlPO-34 with Traces of Bronsted Acid Sites: Combined Catalytic and Spectroscopic Investigations [J].

Dai, Weili ;

Wang, Xin ;

Wu, Guanjun ;

Li, Landong ;

Guan, Naijia ;

Hunger, Michael .

CHEMCATCHEM, 2012, 4 (09) :1428-1435

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