FORMATION OF SURFACE METHOXY GROUPS ON H-ZEOLITES FROM METHANOL - A QUANTUM-CHEMICAL STUDY

被引:82
作者
ZICOVICHWILSON, CM
VIRUELA, P
CORMA, A
机构
[1] UNIV POLITECN VALENCIA, CSIC, INST TECNOL QUIM, E-46022 VALENCIA, SPAIN
[2] UNIV VALENCIA, DEPT QUIM FIS, E-46100 BURJASSOT, SPAIN
关键词
D O I
10.1021/j100035a029
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
Methanol interaction with active sites on H-zeolites was studied by means of quantum chemical methods. Ab initio calculations at MP2/6-311+G(d)/6-31G(d,p)/31G level using the model cluster approximation were made for different possible conformations of chemisorbed methanol on H-zeolite. All structures were optimized and characterized as stationary points at the HF/3-21G level. Two model clusters with a different number of oxygen atoms able to interact with methanol were considered. We found three reaction paths for the interaction of methanol with the acid zeolite cluster. Our results also suggest that a population of the methoxy-zeolite complex, which has been proposed as an active electrophile in aromatic alkylations, can exist on SiOSi bridges, and such species are strongly activated for electrophilic attack.
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页码:13224 / 13231
页数:8
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