A tailored oxide interface creates dense Pt single-atom catalysts with high catalytic activity

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Highly reactive dense Pt single-atoms stabilized on an oxide support can resolve a grand challenge in the economic use of Pt in catalysis. The maximized number density of reaction sites provided by dense Pt single-atoms guarantees the improved catalytic performance of Pt combined with high efficiency. By manipulating the chemical nature of multi-component interfaces, we synthesized CO-tolerant dense Pt single-atoms highly reactive for the CO oxidation reaction, which governs the key steps for chemical energy conversion and emission control. The addition of 1 wt% of Ce to TiO2 support particles creates a CeOx-TiO2 interface that stabilizes Pt single-atoms by strong electronic interactions. Dense Pt single-atoms formed on CeOx/TiO2 oxides exhibit 15.1 times greater specific mass activity toward CO oxidation at 140 degrees C compared with a bare Pt/TiO2 catalyst. We elaborate how the CeOx-TiO2 interfaces activate the interface-mediated Mars-van Krevelen mechanism of CO oxidation and protect Pt single-atoms from CO-poisoning. Through a comprehensive interpretation of the formation and activation of dense Pt single-atoms using operando X-ray absorption spectroscopy, density functional theory calculations, and experimental catalyst performance tests, we provide a key that enables the catalytic performance of noble metal single-atom catalysts to be optimized by atomic-scale tuning of the metal-support interface.
Publisher
Royal Society of Chemistry
Issue Date
2020-04
Language
English
Article Type
Article
Citation

ENERGY & ENVIRONMENTAL SCIENCE, v.13, no.4, pp.1231 - 1239

ISSN
1754-5692
DOI
10.1039/c9ee03492g
URI
http://hdl.handle.net/10203/274162
Appears in Collection
CH-Journal Papers(저널논문)MS-Journal Papers(저널논문)
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