Deactivation mechanism of a Au/CeZrO4 catalyst during a low-temperature water gas shift reaction

被引:90
作者
Goguet, A.
Burch, R.
Chen, Y.
Hardacre, C. [1 ]
Hu, P.
Joyner, R. W.
Meunier, F. C.
Mun, B. S.
Thompsett, A.
Tibiletti, D.
机构
[1] Queens Univ Belfast, CenTACat Sch Chem & Chem Engn, Belfast BT9 5AG, Antrim, North Ireland
[2] Univ Calif Berkeley, Lawrence Berkeley Lab, Berkeley, CA 94720 USA
[3] Johnson Matthey Technol Ctr, Reading RG4 9NH, Berks, England
关键词
D O I
10.1021/jp0743976
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
On-stream deactivation during a water gas shift (WGS) reaction over gold supported on a ceria-zirconia catalyst was examined. Although the fresh catalyst has very high low temperature (< 200 degrees C) for WGS activity, a significant loss of CO conversion is found under steady-state operations over hours. This has been shown to be directly related to the concentration of water in the gas phase. The same catalyst also undergoes thermal deactivation above 250 degrees C, and using a combined experimental and theoretical approach, a common deactivation mechanism is proposed. In both cases, the gold nanoparticles, which are found under reaction conditions, are thought to detach from the oxide support either through hydrolysis, < 200 degrees C, or thermally, > 200 degrees C. This process reduces the metal-support interaction, which is considered to be critical in determining the high activity of the catalyst.
引用
收藏
页码:16927 / 16933
页数:7
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