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

SignificanceDirect ethanol fuel cells are attracting growing attention as portable power sources due to their advantages such as higher mass-energy density than hydrogen and less toxicity than methanol. However, it is challenging to achieve the complete electrooxidation to generate 12 electrons per...

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Published in:	Proceedings of the National Academy of Sciences - PNAS Vol. 119; no. 11; p. e2112109119
Main Authors:	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
Format:	Journal Article
Language:	English
Published:	United States National Academy of Sciences 15-03-2022 Proceedings of the National Academy of Sciences
Subjects:	Active control Carbon dioxide Catalysts Covalent bonds Density functional theory Electrocatalysts Ethanol ethanol oxidation reaction Fine structure INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY Interfacial properties Intermediates Oxidation Physical Sciences platinum nanocubes Rhodium Selectivity single atom catalyst Substrates Ultrastructure X ray absorption ethanol oxidation reaction platinum nanocubes single atom catalyst rhodium
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Summary:	SignificanceDirect ethanol fuel cells are attracting growing attention as portable power sources due to their advantages such as higher mass-energy density than hydrogen and less toxicity than methanol. However, it is challenging to achieve the complete electrooxidation to generate 12 electrons per ethanol, resulting in a low fuel utilization efficiency. This manuscript reports the complete ethanol electrooxidation by engineering efficient catalysts via single-atom modification. The combined electrochemical measurements, in situ characterization, and density functional theory calculations unravel synergistic effects of single Rh atoms and Pt nanocubes and identify reaction pathways leading to the selective C-C bond cleavage to oxidize ethanol to CO . This study provides a unique single-atom approach to tune the activity and selectivity toward complicated electrocatalytic reactions.
Bibliography:	ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23 FG02-13ER16381; SC0009476; SC0012704; SC0012653; NRF-2021R1A2C4001411; NRF-2021R1G1A1092280; 2020R1A4A1018393; 59989-DNI5; ACI-1548562; AC02-06CH11357; SC0012335; AC02-05CH11231 National Research Foundation of Korea (NRF) ACS Petroleum Research Fund National Science Foundation (NSF) USDOE Office of Science (SC), Basic Energy Sciences (BES) BNL-222923-2022-JAAM; BNL-222925-2022-JAAM Edited by Alexis Bell, University of California, Berkeley, CA; received June 30, 2021; accepted December 27, 2021 Author contributions: Q.C., Z.C., J.G.C., and S.-I.C. designed research; Q.C., Y.H., H.J.L., J.H.L., D.O., Z.L., J.K., M.J.K., L.S., and S.K. performed research; J.W.H. contributed new reagents/analytic tools; Q.C., J.H.L., D.O., and S.K. analyzed data; and Q.C., Y.H., H.J.L., J.H.L., D.O., S.K., Z.C., J.G.C., and S.-I.C. wrote the paper. 1Q.C., Y.H., H.J.L., and J.H.L. contributed equally to this work.
ISSN:	0027-8424 1091-6490 1091-6490
DOI:	10.1073/pnas.2112109119