Achieving complete electrooxidation of ethanol by single atomic Rh decoration of Pt nanocubes
Abstract
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.
- Authors:
-
[1];
[3];
[6];
[4];
[7];
[9]
- 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
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Research Foundation of Korea (NRF); ACS Petroleum Research Fund; National Science Foundation (NSF)
- OSTI Identifier:
- 1854052
- Alternate Identifier(s):
- OSTI ID: 1863090; OSTI ID: 1863091
- Report Number(s):
- BNL-222923-2022-JAAM; BNL-222925-2022-JAAM
Journal ID: ISSN 0027-8424; e2112109119
- Grant/Contract Number:
- FG02-13ER16381; SC0009476; SC0012704; SC0012653; NRF-2021R1A2C4001411; NRF-2021R1G1A1092280; 2020R1A4A1018393; 59989-DNI5; ACI-1548562; AC02-06CH11357; SC0012335; AC02-05CH11231
- Resource Type:
- Published Article
- Journal Name:
- Proceedings of the National Academy of Sciences of the United States of America
- Additional Journal Information:
- Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 119 Journal Issue: 11; Journal ID: ISSN 0027-8424
- Publisher:
- Proceedings of the National Academy of Sciences
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; single atom catalyst; rhodium; platinum nanocubes; ethanol oxidation reaction
Citation Formats
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., and Choi, Sang-Il. Achieving complete electrooxidation of ethanol by single atomic Rh decoration of Pt nanocubes. United States: N. p., 2022.
Web. doi:10.1073/pnas.2112109119.
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. Achieving complete electrooxidation of ethanol by single atomic Rh decoration of Pt nanocubes. United States. https://doi.org/10.1073/pnas.2112109119
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., and Choi, Sang-Il. Wed .
"Achieving complete electrooxidation of ethanol by single atomic Rh decoration of Pt nanocubes". United States. https://doi.org/10.1073/pnas.2112109119.
@article{osti_1854052,
title = {Achieving complete electrooxidation of ethanol by single atomic Rh decoration of Pt nanocubes},
author = {Chang, Qiaowan and Hong, Youngmin and Lee, Hye Jin and Lee, Ji Hoon and Ologunagba, Damilola and Liang, Zhixiu and Kim, Jeonghyeon and Kim, Mi Ji and Hong, Jong Wook and Song, Liang and Kattel, Shyam and Chen, Zheng and Chen, Jingguang G. and Choi, Sang-Il},
abstractNote = {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.},
doi = {10.1073/pnas.2112109119},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 11,
volume = 119,
place = {United States},
year = {Wed Mar 09 00:00:00 EST 2022},
month = {Wed Mar 09 00:00:00 EST 2022}
}
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