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Multiple Metal-Nitrogen Bonds Synergistically Boosting the Activity and Durability of High-Entropy Alloy Electrocatalysts

Zhao X 1 , Cheng H 2 , Chen X 3 , Zhang Q 4 , Li C 4 , Xie J 4 Show all authors , Marinkovic N 5 , Ma L 6 , Zheng JC 7 , Sasaki K 1

Affiliations 

  • 1 Chemistry Department, Brookhaven National Laboratory, Upton, New York 11973, United States
  • 2 Department of Applied Physics, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong, China
  • 3 Department of Mechanical Engineering & Materials Science and Engineering Program, State University of New York at Binghamton, Binghamton, New York 13902, United States
  • 4 Department of Mechanical and Energy Engineering, Purdue School of Engineering and Technology, Indiana University-Purdue University Indianapolis, Indianapolis, Indiana 46202, United States
  • 5 Department of Chemical Engineering, Columbia University, New York, New York 10027, United States
  • 6 National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, New York 11973, United States
  • 7 Department of Physics and Fujian Provincial Key Laboratory of Theoretical and Computational Chemistry, Xiamen University, Xiamen 361005, China
J Am Chem Soc, 2024 Feb 07;146(5):3010-3022.
PMID: 38278519 DOI: 10.1021/jacs.3c08177

Abstract

The development of Pt-based catalysts for use in fuel cells that meet performance targets of high activity, maximized stability, and low cost remains a huge challenge. Herein, we report a nitrogen (N)-doped high-entropy alloy (HEA) electrocatalyst that consists of a Pt-rich shell and a N-doped PtCoFeNiCu core on a carbon support (denoted as N-Pt/HEA/C). The N-Pt/HEA/C catalyst showed a high mass activity of 1.34 A mgPt-1 at 0.9 V for the oxygen reduction reaction (ORR) in rotating disk electrode (RDE) testing, which substantially outperformed commercial Pt/C and most of the other binary/ternary Pt-based catalysts. The N-Pt/HEA/C catalyst also demonstrated excellent stability in both RDE and membrane electrode assembly (MEA) testing. Using operando X-ray absorption spectroscopy (XAS) measurements and theoretical calculations, we revealed that the enhanced ORR activity of N-Pt/HEA/C originated from the optimized adsorption energy of intermediates, resulting in the tailored electronic structure formed upon N-doping. Furthermore, we showed that the multiple metal-nitrogen bonds formed synergistically improved the corrosion resistance of the 3d transition metals and enhanced the ORR durability.

* Title and MeSH Headings from MEDLINE®/PubMed®, a database of the U.S. National Library of Medicine.

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