Catalytic combustion of chlorinated aromatics over WOx/CeO2 catalysts at low temperature

被引:134
|
作者
Gu, Yufeng [1 ]
Cai, Ting [2 ]
Gao, Xiaohui [1 ]
Xia, Hangqi [1 ]
Sun, Wei [1 ]
Zhao, Jian [1 ]
Dai, Qiguang [1 ]
Wang, Xingyi [1 ]
机构
[1] East China Univ Sci & Technol, Res Inst Ind Catalysis, Lab Adv Mat, Shanghai 200237, Peoples R China
[2] Shanghai Jiao Tong Univ, Sch Mat Sci & Engn, Shanghai 200240, Peoples R China
基金
中国国家自然科学基金;
关键词
Chlorobenzene; 1,2-Dichlorobenzene; Ceria; Tungsten; Catalytic combustion; TOTAL OXIDATION; TUNGSTEN-OXIDE; SITE DENSITIES; TURNOVER RATES; CERIUM OXIDE; IN-SITU; CHLOROBENZENE; REDUCTION; NO; ADSORPTION;
D O I
10.1016/j.apcatb.2018.12.055
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
WOx/CeO2 catalysts prepared by wet impregnation with (NH4)(6)H2W12O40 and (COOH)(2) aqueous solution were used in the catalytic combustion of chlorobenzene (CB) and 1,2-dichloro- benzene (1,2-DCB). Characterization by XRD, N-2 isothermal adsorption and desorption, Raman, XPS, H-2-TPR, O-2-TPD and NH3-TPD shows that CeO2 exists as a form of face-centered cubic fluorite structure, while WOx is identified as the forms of monoxo and dioxo monotungstate, polytungstate and nano-particle, depending on W content. W-O-Ce is formed as a result of interaction between WOx and CeO2, which increases oxygen vacancy and promotes the reducibility and acidity of WOx/CeO2 catalysts. In CB or 1,2-DCB oxidation, WOx/CeO2 catalysts with monotungstate WOx present excellent stable activity with TOF at 250 degrees C based on W-O-Ce in a range of 4.7-7.2 x 10(-4) s(-1). 90% conversion is obtained below 350 degrees C, at which chlorination is almost completely inhibited. The activity in feed containing 5% H2O or 5% CO2 is depending on their effects on the availability of surface oxygen. In situ FT-IR shows that the adsorbed CB species can be oxidized by surface lattice oxygen into phenolate, carboxylates and carbonate, while the formation of acetaldehyde on Bronsted acid sites is promoted by gas oxygen. Partial oxidation products are oxidized to COx by surface oxygen.
引用
收藏
页码:264 / 276
页数:13
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