• 文献标题:   Correlation between theoretical descriptor and catalytic oxygen reduction activity of graphene supported palladium and palladium alloy electrocatalysts
  • 文献类型:   Article
  • 作  者:   SEO MH, CHOI SM, LEE DU, KIM WB, CHEN ZW
  • 作者关键词:   oxygen reduction reaction, palladium, graphene, electrocatalyst, density functional theory, dissolution potential
  • 出版物名称:   JOURNAL OF POWER SOURCES
  • ISSN:   0378-7753 EI 1873-2755
  • 通讯作者地址:   Univ Waterloo
  • 被引频次:   19
  • DOI:   10.1016/j.jpowsour.2015.08.079
  • 出版年:   2015

▎ 摘  要

The oxygen reduction reaction, ORR, performances of graphene-supported palladium (Pd) and palladium alloys (Pd3X: X = Ag, Co and Fe) catalysts with highly dispersed catalyst particles are investigated in acidic and alkaline conditions using a rotating disk electrode, RDE. Graphene nanosheet, GNS, supported Pd based catalysts are fabricated without surfactant through the impregnation of Pd and 2nd metal precursors on GNS, leading to small and uniformly dispersed nanoparticles, even when high metal loading of up to 60 wt.% are deposited on supports. The ab-initio density functional theory, DFT, calculations, which are based on the d-band center theory, have been applied to correlate with the results of the OR performances obtained by half-cell tests. Additionally, the cohesive energy, E-coh, and dissolution potential, U-m, for the Pd nanoparticles have been calculated to understand thermodynamic stability. To elucidate the d-band center shift, the Pd 3d(5/2) core-level binding energies for Pd/GNS, Pd3Ag/GNS, Pd3Fe/GNS and Pd3Co/GNS have been investigated by X-ray photoelectron spectroscopy, XPS. The GNS-supported Pd, or Pd-based alloy-nanoparticle catalyst shows good ORR activity under acidic and alkaline conditions, suggesting it may offer potential replacement for Pt for use in cathode electrodes of anion-exchange membrane fuel cell, AEMFC, and acid based polymer electrolyte fuel cell, PEMFC. (C) 2015 Elsevier B.V. All rights reserved.