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Title: Ultrahigh Mass Activity for Carbon Dioxide Reduction Enabled by Gold–Iron Core–Shell Nanoparticles

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.

Authors:
 [1]; ORCiD logo [2];  [3];  [4]; ORCiD logo [4];  [4];  [1];  [1]; ORCiD logo [2]; ORCiD logo [1]
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  1. MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, China
  2. Materials and Process Simulation Center (MSC) and Joint Center for Artificial Photosynthesis (JCAP), California Institute of Technology, Pasadena, California 91125, United States
  3. Molecular Imaging Research Center of Harbin Medical University, the Fourth Hospital of Harbin Medical University, Harbin 150001, China
  4. Canadian Light Source Inc., Saskatoon, Saskatchewan S7N 0X4, Canada
Publication Date:
Research Org.:
California Inst. of Technology (CalTech), Pasadena, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1415051
Alternate Identifier(s):
OSTI ID: 1508000
Grant/Contract Number:  
[SC0004993]
Resource Type:
Published Article
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
[Journal Name: Journal of the American Chemical Society Journal Volume: 139 Journal Issue: 44]; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Sun, Kun, Cheng, Tao, Wu, Lina, Hu, Yongfeng, Zhou, Jigang, Maclennan, Aimee, Jiang, Zhaohua, Gao, Yunzhi, Goddard, III, William A., and Wang, Zhijiang. Ultrahigh Mass Activity for Carbon Dioxide Reduction Enabled by Gold–Iron Core–Shell Nanoparticles. United States: N. p., 2017. Web. doi:10.1021/jacs.7b09251.
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Sun, Kun, Cheng, Tao, Wu, Lina, Hu, Yongfeng, Zhou, Jigang, Maclennan, Aimee, Jiang, Zhaohua, Gao, Yunzhi, Goddard, III, William A., & Wang, Zhijiang. Ultrahigh Mass Activity for Carbon Dioxide Reduction Enabled by Gold–Iron Core–Shell Nanoparticles. United States. doi:10.1021/jacs.7b09251.
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Sun, Kun, Cheng, Tao, Wu, Lina, Hu, Yongfeng, Zhou, Jigang, Maclennan, Aimee, Jiang, Zhaohua, Gao, Yunzhi, Goddard, III, William A., and Wang, Zhijiang. Wed . "Ultrahigh Mass Activity for Carbon Dioxide Reduction Enabled by Gold–Iron Core–Shell Nanoparticles". United States. doi:10.1021/jacs.7b09251.
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@article{osti_1415051,
title = {Ultrahigh Mass Activity for Carbon Dioxide Reduction Enabled by Gold–Iron Core–Shell Nanoparticles},
author = {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, III, William A. and Wang, Zhijiang},
abstractNote = {Wide application of carbon dioxide (CO2) 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 CO2 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 CO2 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.},
doi = {10.1021/jacs.7b09251},
journal = {Journal of the American Chemical Society},
number = [44],
volume = [139],
place = {United States},
year = {2017},
month = {10}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1021/jacs.7b09251
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Cited by: 25 works
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Figures / Tables:

Figure 1 Figure 1: (A−D) Sequence of reaction steps for CO2RR on gold (Au)−metal (M) binary alloys. The steps are (A) physisorbed CO2 ( -CO2), (B) *COOH, (C) *CO, (D)* (* indicates surface site). The color codes are Au, yellow; M, green; C, silver; O, red; and H, white. (E) Formation energiesmore » of *COOH and desorption energyies of CO for 20 Au−M alloys, where M is a fourth-row transition metal (from Sc to Zn) or fifth-row transition metal (from Y to Cd). For reference, the black triangle (blue shaded) indicates the properties for pure Au.« less
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Works referencing / citing this record:

Nanostructured amalgams with tuneable silver–mercury bonding sites for selective electroreduction of carbon dioxide into formate and carbon monoxide
journal, January 2019

  • Yang, Wanfeng; Chen, Sheng; Ren, Wenhao
  • Journal of Materials Chemistry A, Vol. 7, Issue 26
  • DOI: 10.1039/c9ta03611c

Enhanced selectivity and activity for electrocatalytic reduction of CO 2 to CO on an anodized Zn/carbon/Ag electrode
journal, January 2019

  • Gao, Yugang; Li, Fengping; Zhou, Peng
  • Journal of Materials Chemistry A, Vol. 7, Issue 28
  • DOI: 10.1039/c9ta04529e

Composition-dependent CO 2 electrochemical reduction activity and selectivity on Au–Pd core–shell nanoparticles
journal, January 2019

  • Zhu, Shangqian; Qin, Xueping; Wang, Qi
  • Journal of Materials Chemistry A, Vol. 7, Issue 28
  • DOI: 10.1039/c9ta05325e
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