Achieving complete electrooxidation of ethanol by single atomic Rh decoration of Pt nanocubes

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초록

The development of single site electrocatalysts such as single-atom catalyst (SAC) has demonstrated the advantages of high precious metal utilization and tunable metal support interfacial properties. However, the fundamental understanding of unalloyed single metal atom decorated on a metallic substrate is still lacking. Herein, we report unalloyed single atomic, partially oxidized Rh on the Pt nanocube surface as the electrocatalyst to completely oxidize ethanol to CO2 at a record-low potential of 0.35 V. In situ X-ray absorption fine structure measurements and density functional theory calculations reveal that the single-atom Rh sites facilitate the C-C bond cleavage and the removal of the *CO intermediates. This work not only reveals the fundamental role of unalloyed, partially oxidized SAC in ethanol oxidation reaction but also offers a unique single-atom approach using low-coordination active sites on shape-controlled nanocatalysts to tune the activity and selectivity toward complicated catalytic reactions.

키워드

single atom catalyst; rhodium; platinum nanocubes; ethanol oxidation reaction; OXYGEN REDUCTION; CARBONYL CLUSTERS; PLATINUM; SPECTROSCOPY; OXIDATION; CATALYSTS; RHODIUM; METAL; ELECTROCATALYSTS; NANOPARTICLES
제목
Achieving complete electrooxidation of ethanol by single atomic Rh decoration of Pt nanocubes
저자
Chang, Qiaowan; Hong, Youngmin; Lee, Hye Jin; Lee, Ji Hoon; Ologunagba, Damilola; Liang, Zhixiu; Kim, Jeonghyeon; Kim, Mi Ji; Hong, Jong Wook; Song, Liang; Kattel, Shyam; Chen, Zheng; Chen, Jingguang G.; Choi, Sang-Il
DOI
10.1073/pnas.2112109119
발행일
2022-03-15
유형
Article
저널명
Proceedings of the National Academy of Sciences of the United States of America
권
119
호
11