Spectromicroscopy of a Model Water鈥揋as Shift Catalyst: Gold Nanoparticles Supported on Ceria
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- 作者：David C. Grinter ; Chris Muryn ; Benito Santos ; Bobbie-Jean Shaw ; Tevfik O. Mente艧 ; Andrea Locatelli ; Geoff Thornton
- 刊名：Journal of Physical Chemistry C
- 出版年：2014
- 出版时间：August 21, 2014
- 年：2014
- 卷：118
- 期：33
- 页码：19194-19204
- 全文大小：734K
- ISSN：1932-7455
文摘
Nanometer-sized gold particles supported on ceria are an important catalyst for the low-temperature water鈥揼as shift reaction. In this work, we prepared a model system of epitaxial, ultrathin (1鈥? nm thick) CeO2鈥?i>x(111) crystallites on a Rh(111) substrate. Low-energy electron microscopy (LEEM) and X-ray photoemission electron microscopy (XPEEM) were employed to characterize the in situ growth and morphology of these films, employing Ce 4f resonant photoemission to probe the oxidation state of the ceria. The deposition of submonolayer amounts of gold at room temperature was studied with scanning tunneling microscopy (STM) and XPEEM. Spatially resolved, energy-selected XPEEM at the Au 4f core level after gold adsorption indicated small shifts to higher binding energy for the nanoparticles, with the magnitude of the shift inversely related to the particle size. Slight reduction of the ceria support was also observed upon increasing Au coverage. The initial oxidation state of the ceria film was shown to influence the Au 4f binding energy; more heavily reduced ceria promoted a larger shift to higher binding energy. Understanding the redox behavior of the gold/ceria system is an important step in elucidating the mechanisms behind its catalytic activity.