期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 263, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2019.118237
关键词
Dichloromethane; Chlorobenzene; Titanium; Tin; Ruthenium; Catalytic combustion
资金
- National Key Research and Development Program of China [2016YFCO204300]
- National Natural Science Foundation of China [21976056and21777043]
Ru/TixSn1-x catalysts, prepared by incipient-wetness with aqueous solution of RuCl3 were applied in the catalytic oxidation of dichloromethane (DCM) and chlorobenzene (CB). In mixed oxides of TixSn1-x, Sn4+ entered into TiO2-rutile and Ti4+, into SnO2-rutile, forming Ti-O-Sn species, which disordered rutile lattice and increased strong Lewis acid. Ru was identified as Ru-O-Ti and Ru-O-Sn, as a result of the interaction between TiO2 or SnO2 and Ru. Ru-O-Sn increased surface oxygen, while Ru-O-Ti promoted the basicity of surface lattice oxygen. In oxidation of DCM at 240 degrees C and CB at 275 degrees C, Ru/TixSn1-x catalysts presented high activity with the rates of 0.084-0.201 and 0.046-0.719 umol min(-1)m(-2), respectively, which was ascribed to the synergism between Ru-OTi and Ru-O-Sn. At 90% conversion, CO2 was almost only the carbon-containing product. Ru/TixSn1-x catalysts maintained stable activity for at least 50 h without substantial changes. High activity for Deacon was responsible for quick removal of Cl species, which was a slow step in the reaction. In the presence of water, the temperature needed for 100% conversion maintained constant. In situ FT-IR showed that chloromethoxyl and phenolate were the adsorbed species of DCM and CB, respectively, which were sequentially converted by surface oxygen into carboxylates and CO2.
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