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

Sun, Kun; Cheng, Tao; Wu, Lina; Hu, Yongfeng; Zhou, Jigang; Maclennan, Aimee; Jiang, Zhaohua; Gao, Yunzhi; Goddard, III, William A.; Wang, Zhijiang

doi:10.1021/jacs.7b09251

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

Abstract

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.

Authors:

Sun, Kun ^[1];

^[2]; Wu, Lina ^[3]; Hu, Yongfeng ^[4];

^[4]; Maclennan, Aimee ^[4]; Jiang, Zhaohua ^[1]; Gao, Yunzhi ^[1];

^[2];

^[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
Materials and Process Simulation Center (MSC) and Joint Center for Artificial Photosynthesis (JCAP), California Institute of Technology, Pasadena, California 91125, United States
Molecular Imaging Research Center of Harbin Medical University, the Fourth Hospital of Harbin Medical University, Harbin 150001, China
Canadian Light Source Inc., Saskatoon, Saskatchewan S7N 0X4, Canada

Publication Date:: 2017-10-11

Research Org.:: California Institute 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.  https://doi.org/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.  https://doi.org/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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Cited by: 161 works

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Figures / Tables:

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 »

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

Abstract

Citation Formats

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