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

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Abstract

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 °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.

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

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Article information


Submitted
29 Oct 2019
Accepted
18 Dec 2019
First published
06 Jan 2020

Energy Environ. Sci., 2020, Advance Article
Article type
Paper

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

M. Yoo, Y. Yu, H. Ha, S. Lee, J. Choi, S. Oh, E. Kang, H. Choi, H. An, K. Lee, J. Y. Park, R. Celestre, M. A. Marcus, K. Nowrouzi, D. Taube, D. A. Shapiro, W. Jung, C. Kim and H. Y. Kim, Energy Environ. Sci., 2020, Advance Article , DOI: 10.1039/C9EE03492G

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