Synergic Effect of Active Sites in Zinc-Modified ZSM-5 Zeolites as Revealed by High-Field Solid-State NMR Spectroscopy

被引：58
|
作者：
Qi, Guodong [1 ]
Wang, Qiang [1 ]
Xu, Jun [1 ]
Trebosc, Julien [2 ]
Lafon, Olivier [2 ]
Wang, Chao [1 ]
Amoureux, Jean-Paul [2 ,3 ]
Deng, Feng [1 ]
机构：
[1] Chinese Acad Sci, State Key Lab Magnet Resonance & Atom & Mol Phys, CAS Key Lab Magnet Resonance Biol Syst, Natl Ctr Magnet Resonance Wuhan,Wuhan Inst Phys &, Wuhan 430071, Peoples R China
[2] Univ Lille, CNRS, Unite Catalyse & Chim Solide, ENSCL,UMR 8181, F-59000 Lille, France
[3] East China Normal Univ, Shanghai 200062, Peoples R China
来源：
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2016年 / 55卷 / 51期
基金：
中国国家自然科学基金;
关键词：
active sites; C-H bond activation; solid-state NMR spectroscopy; synergic effects; zinc-modified zeolite; QUADRUPOLAR NUCLEI; HYDROXYL-GROUPS; ACID STRENGTH; ACETIC-ACID; METHANE; ZN; ACTIVATION; CATALYST; ALKANES; AROMATIZATION;
D O I：
10.1002/anie.201608322
中图分类号：
O6 [化学];
学科分类号：
0703 ;
摘要：
Understanding the nature of active sites in metal-supported catalysts is of great importance towards establishing their structure-property relationships. The outstanding catalytic performance of metal-supported catalysts is frequently ascribed to the synergic effect of different active sites, which is however not well spectroscopically characterized. Herein, we report the direct detection of surface Zn species and H-1-Zn-67 internuclear interaction between Zn2+ ions and BrOnsted acid sites on Zn-modified ZSM-5 zeolites by high-field solid-state NMR spectroscopy. The observed promotion of C-H bond activation of methane is rationalized by the enhanced BrOnsted acidity generated by synergic effects arising from the spatial proximity/interaction between Zn2+ ions and BrOnsted acidic protons. The concentration of synergic active sites is determined by H-1-Zn-67 double-resonance solid-state NMR spectroscopy.
引用
收藏
页码：15826 / 15830
页数：5
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