Tracking the formation, fate and consequence for catalytic activity of Pt single sites on CeO2

被引：279

作者：

Maurer, Florian ^{[1
]}

Jelic, Jelena ^{[2
]}

Wang, Junjun ^{[3
]}

Gaenzler, Andreas ^{[1
]}

Dolcet, Paolo ^{[1
]}

Woell, Christof ^{[3
]}

Wang, Yuemin ^{[3
]}

Studt, Felix ^{[1
,2
]}

Casapu, Maria ^{[1
]}

Grunwaldt, Jan-Dierk ^{[1
,2
]}

机构：

[1] Karlsruhe Inst Technol KIT, Inst Chem Technol & Polymer Chem ITCP, Karlsruhe, Germany

[2] Karlsruhe Inst Technol KIT, Inst Catalysis Res & Technol IKFT, Eggenstein Leopoldshafen, Germany

[3] Karlsruhe Inst Technol KIT, Inst Funct Interfaces IFG, Eggenstein Leopoldshafen, Germany

来源：

NATURE CATALYSIS | 2020年 / 3卷 / 10期

关键词：

RAY-ABSORPTION SPECTROSCOPY; TOTAL-ENERGY CALCULATIONS; WATER-GAS SHIFT; IN-SITU; CO OXIDATION; METAL-IONS; TEMPERATURE; IDENTIFICATION; PERFORMANCE; INTERFACE;

D O I：

10.1038/s41929-020-00508-7

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：

Platinum single sites are highly attractive due to their high atom economy and can be generated on CeO(2)by an oxidative high-temperature treatment. However, their location and activity are strongly debated. Furthermore, reaction-driven structural dynamics have not been addressed so far. In this study, we were able to evidence platinum-induced CeO(2)surface restructuring, locate platinum single sites on CeO(2)and track the variation of the active state under reaction conditions using a complementary approach of density functional theory calculations, in situ infrared spectroscopy, operando high-energy-resolution fluorescence detected X-ray absorption spectroscopy and catalytic CO (as well as C(3)H(6)and CH4) oxidation. We found that the onset of CO oxidation is linked to the migration of platinum single sites from four-fold hollow sites to form small clusters containing a few platinum atoms. This demonstrates that operando studies on single sites are essential to assess their fate and the resulting catalytic properties.

引用

页码：824 / 833

页数：10

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