The effect of reactants adsorption and products desorption for Au/TiO2 in catalyzing CO oxidation

被引:23
作者
Wei, Shuai [1 ]
Wang, Wei-Wei [1 ]
Fu, Xin-Pu [1 ]
Li, Shan-Qing [2 ]
Jia, Chun-Jiang [1 ]
机构
[1] Shandong Univ, Sch Chem & Chem Engn, Key Lab Colloid & Interface Chem, Key Lab Special Aggregated Mat, Jinan 250100, Shandong, Peoples R China
[2] Chizhou Univ, Dept Chem & Mat Engn, Chizhou 247000, Peoples R China
基金
中国国家自然科学基金;
关键词
Au/TiO2; In-situ characterization; Reactants adsorption; Products desorption; CO oxidation; METAL-SUPPORT INTERACTIONS; INITIO MOLECULAR-DYNAMICS; AU PARTICLE-SIZE; GOLD NANOPARTICLES; LOW-TEMPERATURE; CARBON-MONOXIDE; DEPOSITION-PRECIPITATION; RAMAN-SPECTROSCOPY; TIO2; NANOCRYSTALS; CATALYTIC SITES;
D O I
10.1016/j.jcat.2019.06.038
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
Supported gold catalysts exhibit very high activity for CO oxidation. However, there is lack of systematic study for supports effect on reactants adsorption and products desorption. Herein, we successfully prepared supported gold catalysts on TiO2 matrix exposing either {1 0 1} or {0 0 1} crystal plane (labeled as Au/TiO2-1 0 1 and Au/TiO2-0 0 1 respectively) by deposition-precipitation (DP) method. It is found that the reactivity of Au/TiO2-1 0 1 was much higher than Au/TiO2-0 0 1 in CO oxidation reaction (9.33 x 10(-3) mol(CO)g(Au)(-1) s(-1) vs. 6.23 x 10(-4) mol(CO)g(Au)(-1) s(-1) at 30 degrees C). The gold nanoparticles (similar to 2 nm) were detected as sole gold species in Au/TiO2-1 0 1, while not only gold nanoparticles (similar to 4 nm) but also clusters (similar to 1.3 nm) were present in Au/TiO2-0 0 1. The difference in gold status induced different CO adsorption situations that CO was more effectively adsorbed on gold nanoparticles in Au/TiO2-1 0 1 which existed more Au-0 site. Meanwhile, we revealed that the bidentate carbonate, which could either block active sites for the reaction or hinder access of reactants, were adsorbed much more strongly on TiO2-0 0 1. While on TiO2-1 0 1, bicarbonate was the main surface species which was easier decomposed to form CO2. Therefore, the differences between Au/TiO2-1 0 1 and Au/TiO2-0 0 1 in the efficiency of CO adsorption and the ability of CO2 desorption resulted in disparate reactivity. We reasonably gave the deep insight into the support effect that was intrinsically related to the adsorption and desorption behavior of surface species on the catalyst. (C) 2019 Elsevier Inc. All rights reserved.
引用
收藏
页码:134 / 145
页数:12
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