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Published November 8, 2017 | Version Submitted + Published + Supplemental Material
Journal Article Open

Ultrahigh Mass Activity for Carbon Dioxide Reduction Enabled by Gold-iron Core-shell Nanoparticles

Creators

  • 1. ROR icon Harbin Institute of Technology
  • 2. ROR icon California Institute of Technology
  • 3. ROR icon Harbin Medical University
  • 4. ROR icon Canadian Light Source (Canada)

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.

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.

Attached Files

Published - jacs.7b09251

Submitted - ja-2017-092512-MS-oct8-Tao.pdf

Supplemental Material - ja7b09251_si_001.pdf

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Additional details

Identifiers

Eprint ID
82210
Resolver ID
CaltechAUTHORS:20171009-111707593

Funding

Department of Energy (DOE)
DE-SC0004993
National Natural Science Foundation of China
51572062
Natural Science Foundation of Heilongjiang Province
B2015002
National Natural Science Foundation of China
81771903
Heilongjiang Province Foundation for Returness
LC2016034
Wuliande Foundation of Harbin Medical University
WLD-QN1404
Natural Sciences and Engineering Research Council of Canada (NSERC)
National Research Council of Canada
Canadian Institutes of Health Research (CIHR)
University of Saskatchewan
NSF
ACI-1053575

Dates

Created
2017-10-09
Created from EPrint's datestamp field
Updated
2021-11-15
Created from EPrint's last_modified field

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