The catalytic combustion of CH2Cl2 over SO42--TixSn1-x modified with Ru

被引:31
作者
Zhao, Jian [1 ]
Tu, Chensheng [1 ]
Sun, Wei [1 ]
Xia, Hangqi [1 ]
Zhang, Hao [1 ]
Dai, Qiguang [1 ]
Wang, Xingyi [1 ]
机构
[1] East China Univ Sci & Technol, Sch Chem & Mol Engn, Res Inst Ind Catalysis, Shanghai 200237, Peoples R China
基金
中国国家自然科学基金; 上海市自然科学基金;
关键词
POLYOXYMETHYLENE DIMETHYL ETHERS; DICHLOROMETHANE OXIDATION; IRON-OXIDE; ACID SITES; CHLORINATED AROMATICS; SULFATED ZIRCONIA; METAL-OXIDES; MECHANISM; TEMPERATURE; TITANIA;
D O I
10.1039/c9cy01831j
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
Ru/SO42--TixSn1-x catalysts were prepared via impregnation with an aqueous solution of RuCl3 on SO42--TixSn1-x. For the samples with a Ti/Ti + Sn ratio higher or lower than 0.6, TiO2 or SnO2-rutile existed, and both contained the Ti-O-Sn structure. The residual SO42- species as chelating or bridged bidentate complexes with the Ti4+ and Sn4+ ions promoted the acidity significantly. Ru as Ru-0 and Ru4+ was highly dispersed on the matrices as a result of the interaction between the Ru and SO42- species. Ti-O-Sn increased the surface oxygen and SO42- complexes, while Ru promoted the redox activity. In CH2Cl2 oxidation, the Ru/SO42--TixSn1-x catalysts with the Ti-O-Sn structure presented high activity with TOFs at 225 degrees C of 0.18-0.63 x 10(-3) s(-1), which could be ascribed to the synergism between SO42--Ti4+ and the active surface oxygen. At 90% conversion, the selectivity for CO2 and HCl was 90% or higher. Furthermore, the Ru/SO42--TixSn1-x catalysts maintained stable activity for 50 h in wet or dry feed without significant changes. The in situ FT-IR spectra showed that the -O-CH2-O- organic sulfate was the main intermediate in CH2Cl2 oxidation. The hydroxyl activated by surface oxygen was responsible for high activity and Cl removal.
引用
收藏
页码:742 / 756
页数:15
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