Role of Lewis acid sites of ZSM-5 zeolite on gaseous ozone abatement

被引:103
|
作者
Brodu, Nicolas [1 ,2 ]
Manero, Marie-Helene [1 ,2 ]
Andriantsiferana, Caroline [1 ,2 ]
Pic, Jean-Stephane [3 ,4 ]
Valdes, Hector [5 ]
机构
[1] Univ Toulouse, INPT, UPS, Lab Genie Chim, F-31030 Toulouse, France
[2] CNRS, Lab Genie Chim, F-31030 Toulouse, France
[3] Univ Toulouse, LISBP, UMR INSA CNRS 5504, F-31077 Toulouse 4, France
[4] UMR INSA INRA 792, F-31077 Toulouse 4, France
[5] Univ Catolica Santisima Concepcion, Lab Tecnol Limpias F Ingn, Concepcion, Chile
关键词
Acidic sites; Chemical surface properties; Lewis acid sites; Ozone; Synthetic zeolites; ZSM-5; zeolite; NATURAL ZEOLITE; CATALYTIC OZONATION; REACTIVITY; DECOMPOSITION; REMOVAL; ALUMINA; SURFACES; CARBON; VOCS; BETA;
D O I
10.1016/j.cej.2013.07.002
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
In this work, chemical interactions between ozone and zeolite surface active sites are studied in order to propose a process for gaseous ozone removal. Synthetic ZSM-5 zeolites with three different Si/Al-2 ratios and similar specific surface areas and microporous volumes were used in this study. Zeolite samples were characterised using Fourier Transform InfraRed spectroscopy (FTIR) and pyridine sorption IR studies in order to determine acidic site concentrations and strength. Ozone removal experiments were conducted in a quartz fixed-bed flow reactor, at 20 degrees C and 101 kPa. Experiments using Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) were conducted in order to identify adsorbed ozone and/or adsorbed oxygen species on zeolite surface. Pyridine IR measurements evidence two kinds of Lewis acid sites induced by extra-framework aluminium species and electronic aluminium defaults inside zeolite structure. Results obtained here evidence the important role of acidic surface sites of ZSM-5 zeolite on gaseous ozone removal. The total amount of removed ozone is found to be directly proportional to the total content of Lewis acid sites. DRIFTS experiments exhibit two bands around 800 and 1400 cm(-1) that could correspond to adsorbed oxygen species linked to zeolite surface. DRIFTS experiments also exhibit a band around 1100 cm(-1) that correspond to adsorbed ozone on the zeolite surface. Gaseous ozone removal using ZSM-5 zeolite could be largely attributed to ozone decomposition on Lewis acid sites and also to ozone adsorption on the surface of the zeolites. (C) 2013 Elsevier B.V. All rights reserved.
引用
收藏
页码:281 / 286
页数:6
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