Conversion of CO2 on a highly active and stable Cu/FeOx/CeO2 catalyst: tuning catalytic performance by oxide-oxide interactions

被引:33
作者
Lin, Lili [1 ]
Yao, Siyu [1 ]
Rui, Ning [1 ]
Han, Lili [2 ]
Zhang, Feng [3 ]
Gerlak, Clifford A. [1 ]
Liu, Zongyuan [1 ]
Cen, Jiajie [3 ]
Song, Liang [3 ]
Senanayake, Sanjaya D. [1 ]
Xin, Huolin L. [2 ]
Chen, Jingguang G. [1 ]
Rodriguez, Jose A. [1 ,3 ,4 ]
机构
[1] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA
[2] Univ Calif Irvine, Dept Phys & Astron, Irvine, CA 92697 USA
[3] SUNY Stony Brook, Dept Mat Sci & Chem Engn, Stony Brook, NY 11794 USA
[4] SUNY Stony Brook, Dept Chem, Stony Brook, NY 11794 USA
关键词
RAY-ABSORPTION SPECTROSCOPY; IN-SITU CHARACTERIZATION; GAS-SHIFT REACTION; CERIA; HYDROGENATION; DEHYDROGENATION; DEACTIVATION; REDUCTION; OXIDATION; SUPPORT;
D O I
10.1039/c9cy00722a
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
Nanoparticles of FeOx dispersed on ceria exhibit unique chemical and textural properties. They undergo a dynamic FeOx <-> Fe transformation depending on the reaction conditions. The high density Fe oxide clusters dispersed over CeO2 are effective texture promoters that enhance the stability of Cu/CeO2 catalyst in the high temperature reverse water gas shift reaction. At the optimal Fe loading, the deactivation rate constant of a 5Cu1.6Fe/CeO2 catalyst is only 0.003 h(-1), five times smaller than that of the monometallic 5Cu/CeO2 catalyst. In situ XRD, AP-XPS and XAFS characterizations reveal that the partially reduced Fe nanoparticles would be oxidized by CO2 in the reductive atmosphere and re-disperse into high density FeOx clusters under the high temperature CO2 hydrogenation process. The wetting phenomenon, maximizing the density of FeOx particles on the CeO2 support, benefits from strong oxide-oxide (Fe-O-Ce) interactions.
引用
收藏
页码:3735 / 3742
页数:8
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