Atomically Dispersed Pd-O Species on Ceo2(111) as Highly Active Sites for Low-Temperature CO Oxidation

被引:253
作者
Spezzati, Giulia [1 ]
Su, Yaqiong [1 ]
Hofmann, Jan P. [1 ]
Benavidez, Angelica D. [2 ,3 ]
DeLaRiva, Andrew T. [2 ,3 ]
McCabe, Jay [2 ,3 ]
Datye, Abhaya K. [2 ,3 ]
Hensen, Emiel J. M. [1 ]
机构
[1] Eindhoven Univ Technol, Lab Inorgan Mat Chem, Dept Chem Engn & Chem, POB 513, NL-5600 MB Eindhoven, Netherlands
[2] Univ New Mexico, Dept Chem & Biol Engn, Albuquerque, NM 87131 USA
[3] Univ New Mexico, Ctr Microengn Mat, Albuquerque, NM 87131 USA
关键词
cerium oxide; palladium; single site; CO oxidation; FTIR; computational modeling mechanism; WATER-GAS SHIFT; METHANE COMBUSTION; CERIA CATALYSTS; SURFACE; PLATINUM; CEO2; NANOPARTICLES; REACTIVITY; DEPENDENCE; SUPPORTS;
D O I
10.1021/acscatal.7b02001
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
Ceria-supported Pd is a promising heterogeneous catalyst for CO oxidation relevant to environmental cleanup reactions. Pd loaded onto a nanorod form of ceria exposing predominantly (111) facets is already active at 50 degrees C. Here we report a combination of CO-FTIR spectroscopy and theoretical calculations that allows assigning different forms of Pd on the Ceo(2)(111) surface during reaction conditions. Single Pd atoms stabilized in the form of PdO and Pdo(2) in a CO/O-2 atmosphere participate in a catalytic cycle involving very low activation barriers for CO oxidation. The presence of single Pd atoms on the Pd/Ceo(2)-nanorod, corroborated by aberration-corrected TEM and CO-FTIR spectroscopy, is considered pivotal to its high CO oxidation activity.
引用
收藏
页码:6887 / 6891
页数:5
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