Sun, Kun and Cheng, Tao and Wu, Lina and Hu, Yongfeng and Zhou, Jigang and MacLennan, Aimee and Jiang, Zhaohua and Gao, Yunzhi and Goddard, William A., III and Wang, Zhijiang (2017) Ultrahigh Mass Activity for Carbon Dioxide Reduction Enabled by Gold-iron Core-shell Nanoparticles. Journal of the American Chemical Society, 139 (44). pp. 15608-15611. ISSN 0002-7863. doi:10.1021/jacs.7b09251. https://resolver.caltech.edu/CaltechAUTHORS:20171009-111707593
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Abstract
Wide application of carbon dioxide (CO_2) electrochemical energy storage requires catalysts with high mass activity. Alloy catalysts can achieve superior performance to single metals while reducing the cost by finely tuning the composition and morphology. We used in silico quantum mechanics rapid screening to identify Au–Fe as a candidate improving CO_2 reduction and then synthesized and tested it experimentally. The synthesized Au–Fe alloy catalyst evolves quickly into a stable Au–Fe core–shell nanoparticle (AuFe-CSNP) after leaching out surface Fe. This AuFe-CSNP exhibits exclusive CO selectivity, long-term stability, nearly a 100-fold increase in mass activity toward CO_2 reduction compared with Au NP, and 0.2 V lower in overpotential. Calculations show that surface defects due to Fe leaching contribute significantly to decrease the overpotential.
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| Additional Information: | © 2017 American Chemical Society. ACS AuthorChoice - This is an open access article published under an ACS AuthorChoice License, which permits copying and redistribution of the article or any adaptations for non-commercial purposes. Received: August 30, 2017; Published: October 9, 2017. T.C. and W.A.G. were supported by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under award no. DE-SC0004993. Z.W. acknowledges Mr. David Muir for his kind help on the EXAFS measurement and financial support from the National Natural Science Foundation of China (no. 51572062) and the Natural Science Foundation of Heilongjiang Province (no. B2015002). L.W. appreciates the financial support of National Natural Science Foundation of China (no. 81771903), Heilongjiang Province Foundation for Returness (no. LC2016034), and Wuliande Foundation of Harbin Medical University (grant no. WLD-QN1404). C.L.S. is supported by the NSERC, NRC, CIHR of Canada, and the University of Saskatchewan. The QM calculations used the resources of the Extreme Science and Engineering Discovery Environment (XSEDE) which is supported by National Science Foundation grant no. ACI-1053575. The authors declare no competing financial interest. | ||||||||||||||||||||||||
| Group: | JCAP | ||||||||||||||||||||||||
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| Issue or Number: | 44 | ||||||||||||||||||||||||
| DOI: | 10.1021/jacs.7b09251 | ||||||||||||||||||||||||
| Record Number: | CaltechAUTHORS:20171009-111707593 | ||||||||||||||||||||||||
| Persistent URL: | https://resolver.caltech.edu/CaltechAUTHORS:20171009-111707593 | ||||||||||||||||||||||||
| Official Citation: | Ultrahigh Mass Activity for Carbon Dioxide Reduction Enabled by Gold–Iron Core–Shell Nanoparticles. Kun Sun, Tao Cheng, Lina Wu, Yongfeng Hu, Jigang Zhou, Aimee Maclennan, Zhaohua Jiang, Yunzhi Gao, William A. Goddard, III, and Zhijiang Wang. Journal of the American Chemical Society 2017 139 (44), 15608-15611. DOI: 10.1021/jacs.7b09251 | ||||||||||||||||||||||||
| Usage Policy: | No commercial reproduction, distribution, display or performance rights in this work are provided. | ||||||||||||||||||||||||
| ID Code: | 82210 | ||||||||||||||||||||||||
| Collection: | CaltechAUTHORS | ||||||||||||||||||||||||
| Deposited By: | Ruth Sustaita | ||||||||||||||||||||||||
| Deposited On: | 09 Oct 2017 20:10 | ||||||||||||||||||||||||
| Last Modified: | 15 Nov 2021 19:48 |
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