A DFT study of hydrogen-deuterium exchange over oxidized and reduced gallium species in Ga/HZSM-5 zeolite

被引：12
作者：
Kuzmin, IV
Zhidomirov, GM
Hensen, EJM
机构：
[1] Russian Acad Sci, ND Zelinskii Organ Chem Inst, Moscow 117913, Russia
[2] Russian Acad Sci, Boreskov Inst Catalysis, Siberian Branch, Novosibirsk 630090, Russia
[3] Eindhoven Univ Technol, Schuit Inst Catalysis, NL-5600 MB Eindhoven, Netherlands
来源：
CATALYSIS LETTERS | 2006年 / 108卷 / 3-4期
基金：
俄罗斯基础研究基金会;
关键词：
DFT; gallium; zeolite; Ga/ZSM-5; hydrogen activation; isotopes; exchange;
D O I：
10.1007/s10562-006-0043-9
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：
Quantum-chemical calculations give insight in the experimentally observed higher rate of hydrogen-deuterium exchange for oxidized Ga/HZSM-5 over reduced Ga/HZSM-5. The reaction is computed to be more facile over reduced (Ga+) than over oxidized (GaO+) cations. The difference lies in the difficult formation of active GaH2+ cations from Ga+ compared to facile hydrogen dissociation over GaO+ to give active GaHOH+ cations. Neutral gallium oxide clusters are shown to have a lower intrinsic activity than GaO+ cations.
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页码：187 / 191
页数：5
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