CO oxidation by Ti- and Al-doped ZnO: Oxygen activation by adsorption on the dopant

被引:61
作者
Pala, Rai Ganesh S. [1 ]
Tang, Wei [1 ]
Sushchikh, Michael M. [2 ]
Park, Jung-Nam [2 ]
Forman, Arnold J. [1 ]
Wu, Guang [1 ]
Kleiman-Shwarsctein, Alan [3 ]
Zhang, Jingping [3 ]
McFarland, Eric W. [2 ]
Metiu, Horia [1 ]
机构
[1] Univ Calif Santa Barbara, Dept Chem & Biochem, Santa Barbara, CA 93106 USA
[2] Univ Calif Santa Barbara, Dept Chem Engn, Santa Barbara, CA 93106 USA
[3] Univ Calif Santa Barbara, Dept Mat, Santa Barbara, CA 93106 USA
关键词
CO oxidation; Catalysis; Doped oxide; Ti; Al; ZnO; O-18(2); PROMOTED MAGNESIA CATALYST; TOTAL-ENERGY CALCULATIONS; NO REDUCTION; HYDROCARBON OXIDATION; PEROVSKITE CATALYSTS; INTELLIGENT CATALYST; RUTILE TIO2(110); SOLID-SOLUTIONS; HIGH-RATES; METHANE;
D O I
10.1016/j.jcat.2009.05.011
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
Using a combination of theory and experiments, we show that ZnO substitutionally doped with Ti or Al oxidizes CO by several parallel reaction pathways that differ from the traditional Mars-van Krevelen (MVK) mechanism. in one, the dopant atoms at the surface of the doped oxide adsorb and activate O-2 so that it reacts with CO. In the other, a surface oxygen atom from the lattice next to the dopant, D, moves onto the dopant and creates an O-D group and an oxygen vacancy. The O-D group is capable of oxidizing a reductant. To test these predictions made by theory, we have prepared Ti- and M-doped ZnO and have shown that these compounds oxidize CO at temperatures at which pure-phase ZnO, Al2O3, or TiO2 do not. The proposed mechanisms were made plausible by studying CO oxidation with O-18(2). (C) 2009 Elsevier Inc. All rights reserved.
引用
收藏
页码:50 / 58
页数:9
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