Solid acid catalysts based on H3PW12O40 heteropoly acid Acid and catalytic properties at a gas-solid interface

被引:137
|
作者
Alsalme, Ali M. [1 ]
Wiper, Paul V. [1 ]
Khimyak, Yaroslav Z. [1 ]
Kozhevnikova, Elena F. [1 ]
Kozhevnikov, Ivan V. [1 ]
机构
[1] Univ Liverpool, Dept Chem, Liverpool L69 7ZD, Merseyside, England
基金
英国工程与自然科学研究理事会;
关键词
Heterogeneous acid catalysis; Heteropoly acid; Interaction with support; Isopropanol dehydration; 12-TUNGSTOPHOSPHORIC ACID; DIFFERENT SUPPORTS; MIXED-OXIDE; ZIRCONIA; SILICA; TEMPERATURE; SURFACE; MCM-41;
D O I
10.1016/j.jcat.2010.09.014
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
Solid acid catalysts prepared by supporting 15 wt%H3PW12O40 heteropoly acid (HPA) on TiO2 ZrO2 and Nb2O5 with a sub-monolayer HPA coverage were characterised at a gas-solid interface regarding their acid properties and chemical structure of HPA on the catalyst surface and compared to standard HPA catalysts such as bulk and silica-supported H3PW12O40 and Cs-2 H-5(0) 5PW12O40. In contrast to the parent acid H3PW12O40 possessing strong Bronsted acid sites the catalysts supported on TiO2 ZrO2 and Nb2O5 have both Bronsted and Lewis acid sites with the latter mainly originating from the oxide support The strength of acid sites in these catalysts is weaker than that in H3PW12O40 and Cs-2 H-5(0) 5PW12O40 The catalytic activity (turnover frequency) in gas-phase isopropanol dehydration decreases in the order H3PW12O40 > Cs-2 H-5(0) 5PW12O40 > 15%H3PW12O40/SiO2 > 15%H3PW12O40/TiO2 > 15%H3PW12O40/Nb2O5 > 15%H3PW12O40/ZrO2 which is in line with the acid strength as determined by NH3 adsorption calorimetry Ammonia adsorption calorimetry P-31{H-1} MAS NMR and FTIR indicate increasing interaction between support and HPA in the following order of supports SiO2 < TiO2 < Nb2O5 < ZrO2 (C) 2010 Elsevier Inc All rights reserved
引用
收藏
页码:181 / 189
页数:9
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