期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 58, 期 32, 页码 10932-10935出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201904680
关键词
atom-cluster catalysts; cluster compounds; metal-support interactions; silver; titanium-oxo clusters
资金
- National Key Research and Development Program of China [2018YFA0208600, 2017YFA0206801]
- National Natural Science Foundation of China [21673238, 91645116]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB20000000]
- Natural Science Foundation of Fujian Province [2017J06009, 2019J01131]
Supported single-atom catalysts have been emerging as promising materials in a variety of energy catalysis applications. However, studying the role of metal-support interactions at the molecular level remains a major challenge, primarily due to the lack of precise atomic structures. In this work, by replacing the frequently used TiO2 support with its molecular analogue, titanium-oxo cluster (TOC), we successfully produced a new kind of Ti-O material doped with single silver sites. The as-obtained Ag10Ti28 cluster, containing four exposed and six embedded Ag sites, is the largest noble-metal-doped Ti-O cluster reported to date. Density functional theory (DFT) calculations show that the Ag10Ti28 core exhibits properties distinct from those of metallic Ag-based materials. This Ti-O material doped with single Ag sites presents a high epsilon(d) and moderate CO binding capacity comparable to that of metallic Cu-based catalysts, suggesting that it might display different catalytic performance from the common Ag-based catalysts, for example, for CO2 reduction. These results prove that the synergism of active surface metal atoms and the Ti-O cluster support result in unique physical properties, which might open a new direction for single-atom-included catalysts.
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