Achieving complete electrooxidation of ethanol by single atomic Rh decoration of Pt nanocubes
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- Department of NanoEngineering, University of California San Diego, La Jolla, CA 92093, Department of Chemical Engineering, Columbia University, New York, NY 10027
- Department of Chemistry and Green-Nano Materials Research Center, Kyungpook National University, Daegu 41566, Republic of Korea
- Department of Chemical Engineering, Columbia University, New York, NY 10027, School of Materials Science and Engineering, Kyungpook National University, Daegu 41566, Republic of Korea
- Department of Physics, Florida A&,M University, Tallahassee, FL 32307
- Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY 11973
- Department of Chemistry, University of Ulsan, Ulsan 44776, Republic of Korea
- Department of NanoEngineering, University of California San Diego, La Jolla, CA 92093, Program of Chemical Engineering, University of California San Diego, La Jolla, CA 92093
- Department of Chemical Engineering, Columbia University, New York, NY 10027, Chemistry Division, Brookhaven National Laboratory, Upton, NY 11973
- Department of Chemistry and Green-Nano Materials Research Center, Kyungpook National University, Daegu 41566, Republic of Korea, Department of Hydrogen and Renewable Energy, Kyungpook National University, Daegu 41566, Republic of Korea
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. Finally, 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.
- Research Organization:
- Brookhaven National Laboratory (BNL), Upton, NY (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Research Foundation of Korea (NRF); ACS Petroleum Research Fund; National Science Foundation (NSF)
- Grant/Contract Number:
- FG02-13ER16381; SC0009476; SC0012704; SC0012653; NRF-2021R1A2C4001411; NRF-2021R1G1A1092280; 2020R1A4A1018393; 59989-DNI5; ACI-1548562; AC02-06CH11357; SC0012335; AC02-05CH11231
- OSTI ID:
- 1854052
- Alternate ID(s):
- OSTI ID: 1863090; OSTI ID: 1863091
- Report Number(s):
- BNL-222923-2022-JAAM; BNL-222925-2022-JAAM; e2112109119
- Journal Information:
- Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Vol. 119 Journal Issue: 11; ISSN 0027-8424
- Publisher:
- Proceedings of the National Academy of SciencesCopyright Statement
- Country of Publication:
- United States
- Language:
- English
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