Chinese Journal of Catalysis ›› 2022, Vol. 43 ›› Issue (3): 851-861.DOI: 10.1016/S1872-2067(21)63895-0

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Hierarchical AgAu alloy nanostructures for highly efficient electrocatalytic ethanol oxidation

Caiqin Wanga,b, Danil Bukhvalova, M. Cynthia Gohb,#(), Yukou Duc, Xiaofei Yanga,*()   

  1. aCollege of Science & Institute of Materials Physics and Chemistry, Nanjing Forestry University, Nanjing 210037, Jiangsu, China
    bDepartment of Chemistry, University of Toronto, Toronto, Canada
    cCollege of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123, Jiangsu, China
  • Received:2021-06-02 Revised:2021-06-02 Online:2022-03-18 Published:2022-02-18
  • Contact: M. Cynthia Goh, Xiaofei Yang
  • Supported by:
    Natural Science Foundation of Jiangsu Province(BK20190762);Science Fund for Distinguished Young Scholars, Nanjing Forestry University(JC2019002)

Abstract:

The ethanol oxidation reaction is a significant anodic reaction for direct alcohol fuel cells. The most commonly used catalysts for this reaction are Pt-based materials; however, Pt-based electrocatalysts cause carbon monoxide poisoning with intermediates before the complete transformation of alcohol to CO2. Herein, we present hierarchical AgAu bimetallic nanoarchitectures for ethanol electrooxidation, which were fabricated via a partial galvanic reduction reaction between Ag and HAuCl4. The ethanol electrooxidation performance of the optimal AgAu nanohybrid was increased to 1834 mA mg‒1, which is almost 10 times higher than that of the pristine Au catalyst (190 mA mg‒1) in alkaline solutions. This was achieved by introducing Ag into the Au catalyst and controlling the time of the replacement reaction. The heterostructure also presents a higher current density than that of commercial Pt/C (1574 mA mg‒1). Density functional theory calculations revealed that the enhanced activity and stability may stem from unavoidable defects on the surface of the integrated AgAu nanoarchitectures. Ethanol oxidation reactions over these defects are more energetically favorable, which facilitates the oxidative removal of carbonaceous poison and boosts the combination with radicals on adjacent Au active sites.

Key words: AgAu nanohybrids, Hierarchical nanostructures, Defected surface, DFT calculation, Ethanol electrooxidation