Frustrated Lewis Pair in Zeolite Cages for Alkane Activations

被引：34

作者：

Chen, Wei ^{[1
]}

Han, Jingfeng ^{[2
]}

Wei, Yingxu ^{[2
]}

Zheng, Anmin ^{[1
,3
]}

机构：

[1] Chinese Acad Sci, Innovat Acad Precis Measurement Sci & Technol, Natl Ctr Magnet Resonance Wuhan,Key Lab Magnet Re, Wuhan Inst Phys & Math,State Key Lab Magnet Reson, Wuhan 430071, Peoples R China

[2] Chinese Acad Sci, iChEM Collaborat Innovat Ctr Chem Energy Mat, Dalian Inst Chem Phys, Natl Engn Lab Methanol Olefins,Dalian Natl Lab Cl, Dalian 116023, Peoples R China

[3] Univ Chinese Acad Sci, Beijing 100049, Peoples R China

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2022年 / 61卷 / 15期

基金：

中国国家自然科学基金;

关键词：

Alkane Dehydrogenation; Carbocations; Frustrated Lewis Pair; Heterolysis; Zeolites; REACTION TEMPERATURE; OLEFINS CONVERSION; BOND FORMATION; METHANOL; CATALYSIS; REACTIVITY; LIFETIME; HYDROGEN; ACIDITY; CO;

D O I：

10.1002/anie.202116269

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The frustrated Lewis pair (FLP) concept in homogeneous catalysis was extended to heterogeneous catalysis via the supramolecular system of FLP between deprotonated zeolite framework oxygens and confined carbocations in methanol-to-olefin (MTO) reactions. In this FLP, the polymethylbenzenium (PMB+) functioned as the Lewis acid to accept an electron pair, and the deprotonated framework oxygen site acted as the Lewis base to donate an electron pair. This FLP theoretically demonstrated the ability to undergo H-2 heterolysis and alkanes dehydrogenation, and this was further confirmed by gas chromatography-mass spectrometer (GC-MS) catalytic experiments inside FLP-containing chabazite zeolites. All these findings not only bring new recognition to the carbocation chemistry in zeolite cages but also put forward a new reaction pathway as one part of MTO reactions.

引用

页数：7

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