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

Journal Article · · Journal of the American Chemical Society
 [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)

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.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1504452
Journal Information:
Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 48 Vol. 140; ISSN 0002-7863
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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Enhanced Electrocatalytic Hydrogen Oxidation on Ni/NiO/C Derived from a Nickel‐Based Metal–Organic Framework journal June 2019
Enhanced Electrocatalytic Hydrogen Oxidation on Ni/NiO/C Derived from a Nickel-Based Metal-Organic Framework journal June 2019
Boosting Stability and Activity of Oxygen Evolution Catalyst in Acidic Medium: Bimetallic Ir−Fe Oxides on Reduced Graphene Oxide Prepared through Ultrasonic Spray Pyrolysis journal April 2019
Size‐Dependent Phase Transformation of Noble Metal Nanomaterials journal August 2019
Uniform Pd 0.33 Ir 0.67 nanoparticles supported on nitrogen-doped carbon with remarkable activity toward the alkaline hydrogen oxidation reaction journal January 2019
Shaping well-defined noble-metal-based nanostructures for fabricating high-performance electrocatalysts: advances and perspectives journal January 2019
Modulating the surface segregation of PdCuRu nanocrystals for enhanced all-pH hydrogen evolution electrocatalysis journal January 2019