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Surface-structure sensitivity of CeO<sub>2</sub> nanocrystals in photocatalysis and enhancing the reactivity with nanogold [electronic resource].

Published:
Washington, D.C. : United States. Dept. of Energy. Office of Basic Energy Sciences, 2015.
Oak Ridge, Tenn. : Distributed by the Office of Scientific and Technical Information, U.S. Dept. of Energy
Physical Description:
pages 4,385-4,393 : digital, PDF file
Additional Creators:
Brookhaven National Laboratory, United States. Department of Energy. Office of Basic Energy Sciences, and United States. Department of Energy. Office of Scientific and Technical Information
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Summary:
Structure–function correlations are a central theme in heterogeneous (photo)catalysis. In this research, using aberration-corrected scanning transmission electron microscopy (STEM), the atomic surface structures of well-defined one-dimensional (1D) CeO2 nanorods (NRs) and 3D nanocubes (NCs) are directly visualized at subangstrom resolution. CeO2 NCs predominantly expose the {100} facet, with {110} and {111} as minor cutoff facets at the respective edges and corners. Notably, the outermost surface layer of the {100} facet is nearly O-terminated. Neither surface relaxations nor reconstructions on {100} are observed, indicating unusual polarity compensation, which is primarily mediated by near-surface oxygen vacancies. The surface of CeO2 NRs is highly stepped, with the enclosed {110} facet exposing Ce cations and O anions on terraces. On the basis of STEM profile-view imaging and electronic structure analysis, the photoreactivity of CeO2 nanocrystals toward aqueous methyl orange degradation under UV is revealed to be surface-structure-sensitive, following the order: {110} >> {100}. The underlying surface-structure sensitivity can be attributed to the variation in low-coordinate surface cerium cations between {110} and {100} facets. To further enhance light absorption, Au nanoparticles (NPs) are deposited on CeO2 NRs to form Au/CeO2 plasmonic nanocomposites, which dramatically promotes the photoreactivity that is Au particle size- and excitation light wavelength-dependent. The mechanisms responsible for the enhancement of photocatalytic activity are discussed, highlighting the crucial role of photoexcited charge carrier transfer.
Report Numbers:
E 1.99:bnl--108402-2015-ja
bnl--108402-2015-ja
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Other Subject(s):
Note:
Published through SciTech Connect.
06/19/2015.
"bnl--108402-2015-ja"
"KC0302010"
ACS Catalysis 5 7 ISSN 2155-5435 AM
Lei, Wanying; Zhang, Tingting; Gu, Lin; Liu, Ping; Rodriguez, José; Liu, Gang; Liu, Minghua.
Funding Information:
51272048
CO009
View MARC record | catkey: 24046738