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Title: BCC-Phased PdCu Alloy as a Highly Active Electrocatalyst for Hydrogen Oxidation in Alkaline Electrolytes

Abstract

We report that anion-exchange membrane fuel cells hold promise to greatly reduce cost by employing nonprecious metal cathode catalysts. More efficient anode catalysts are needed, however, to improve the sluggish hydrogen oxidation reaction in alkaline electrolytes. We report that BCC-phased PdCu alloy nanoparticles, synthesized via a wet-chemistry method with a critical thermal treatment, exhibit up to 20-fold HOR improvement in both mass and specific activities, compared with the FCC-phased PdCu counterparts. HOR activity of the BCC-phased PdCu is 4 times or 2 times that of Pd/C or Pt/C, respectively, in the same alkaline electrolyte. In situ HE-XRD measurements reveal that the transformation of PdCu crystalline structure favors, at low annealing temperature (<300 °C), the formation of FCC structure. At higher annealing temperatures (300–500 °C), a BCC structure dominates the PdCu NPs. Density functional theory (DFT) computations unravel a similar H binding strength and a much stronger OH binding of the PdCu BCC surface (cf. FCC surface), both of which are simultaneously close to those of Pt surfaces. The synergistic optimization of both H and OH binding strengths is responsible for the enhancement of HOR activity on BCC-phased PdCu, which could serve as an efficient anode catalyst for anion-exchange membrane fuelmore » cells. Lastly, this work might open a new route to develop efficient HOR catalysts from the perspective of crystalline structure transformation.« less

Authors:
 [1];  [1]; ORCiD logo [2];  [2];  [3];  [4];  [3];  [3];  [4];  [5];  [2]; ORCiD logo [4]
  1. Iowa State Univ., Ames, IA (United States)
  2. Pennsylvania State Univ., University Park, PA (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Ames Lab. and Iowa State Univ., Ames, IA (United States)
  5. Wichita State University (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
OSTI Identifier:
1504452
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 140; Journal Issue: 48; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Qiu, Yang, Xin, Le, Li, Yawei, McCrum, Ian T., Guo, Fangmin, Ma, Tao, Ren, Yang, Liu, Qi, Zhou, Lin, Gu, Shuang, Janik, Michael J., and Li, Wenzhen. BCC-Phased PdCu Alloy as a Highly Active Electrocatalyst for Hydrogen Oxidation in Alkaline Electrolytes. United States: N. p., 2018. Web. doi:10.1021/jacs.8b08356.
Qiu, Yang, Xin, Le, Li, Yawei, McCrum, Ian T., Guo, Fangmin, Ma, Tao, Ren, Yang, Liu, Qi, Zhou, Lin, Gu, Shuang, Janik, Michael J., & Li, Wenzhen. BCC-Phased PdCu Alloy as a Highly Active Electrocatalyst for Hydrogen Oxidation in Alkaline Electrolytes. United States. doi:10.1021/jacs.8b08356.
Qiu, Yang, Xin, Le, Li, Yawei, McCrum, Ian T., Guo, Fangmin, Ma, Tao, Ren, Yang, Liu, Qi, Zhou, Lin, Gu, Shuang, Janik, Michael J., and Li, Wenzhen. Mon . "BCC-Phased PdCu Alloy as a Highly Active Electrocatalyst for Hydrogen Oxidation in Alkaline Electrolytes". United States. doi:10.1021/jacs.8b08356.
@article{osti_1504452,
title = {BCC-Phased PdCu Alloy as a Highly Active Electrocatalyst for Hydrogen Oxidation in Alkaline Electrolytes},
author = {Qiu, Yang and Xin, Le and Li, Yawei and McCrum, Ian T. and Guo, Fangmin and Ma, Tao and Ren, Yang and Liu, Qi and Zhou, Lin and Gu, Shuang and Janik, Michael J. and Li, Wenzhen},
abstractNote = {We report that anion-exchange membrane fuel cells hold promise to greatly reduce cost by employing nonprecious metal cathode catalysts. More efficient anode catalysts are needed, however, to improve the sluggish hydrogen oxidation reaction in alkaline electrolytes. We report that BCC-phased PdCu alloy nanoparticles, synthesized via a wet-chemistry method with a critical thermal treatment, exhibit up to 20-fold HOR improvement in both mass and specific activities, compared with the FCC-phased PdCu counterparts. HOR activity of the BCC-phased PdCu is 4 times or 2 times that of Pd/C or Pt/C, respectively, in the same alkaline electrolyte. In situ HE-XRD measurements reveal that the transformation of PdCu crystalline structure favors, at low annealing temperature (<300 °C), the formation of FCC structure. At higher annealing temperatures (300–500 °C), a BCC structure dominates the PdCu NPs. Density functional theory (DFT) computations unravel a similar H binding strength and a much stronger OH binding of the PdCu BCC surface (cf. FCC surface), both of which are simultaneously close to those of Pt surfaces. The synergistic optimization of both H and OH binding strengths is responsible for the enhancement of HOR activity on BCC-phased PdCu, which could serve as an efficient anode catalyst for anion-exchange membrane fuel cells. Lastly, this work might open a new route to develop efficient HOR catalysts from the perspective of crystalline structure transformation.},
doi = {10.1021/jacs.8b08356},
journal = {Journal of the American Chemical Society},
issn = {0002-7863},
number = 48,
volume = 140,
place = {United States},
year = {2018},
month = {11}
}

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