Tuning the electronic structure of Ag-Pd alloys to enhance performance for alkaline oxygen reduction

José A. Zamora Zeledón, Michaela Burke Stevens, G. T. Kasun Kalhara Gunasooriya, Alessandro Gallo, Alan T. Landers, Melissa E. Kreider, Christopher Hahn, Jens K. Nørskov and Thomas F. Jaramillo ()
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José A. Zamora Zeledón: Stanford University
Michaela Burke Stevens: Stanford University
G. T. Kasun Kalhara Gunasooriya: Technical University of Denmark
Alessandro Gallo: Stanford University
Alan T. Landers: SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory
Melissa E. Kreider: Stanford University
Christopher Hahn: Stanford University
Jens K. Nørskov: Technical University of Denmark
Thomas F. Jaramillo: Stanford University

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: Abstract Alloying is a powerful tool that can improve the electrocatalytic performance and viability of diverse electrochemical renewable energy technologies. Herein, we enhance the activity of Pd-based electrocatalysts via Ag-Pd alloying while simultaneously lowering precious metal content in a broad-range compositional study focusing on highly comparable Ag-Pd thin films synthesized systematically via electron-beam physical vapor co-deposition. Cyclic voltammetry in 0.1 M KOH shows enhancements across a wide range of alloys; even slight alloying with Ag (e.g. Ag0.1Pd0.9) leads to intrinsic activity enhancements up to 5-fold at 0.9 V vs. RHE compared to pure Pd. Based on density functional theory and x-ray absorption, we hypothesize that these enhancements arise mainly from ligand effects that optimize adsorbate–metal binding energies with enhanced Ag-Pd hybridization. This work shows the versatility of coupled experimental-theoretical methods in designing materials with specific and tunable properties and aids the development of highly active electrocatalysts with decreased precious-metal content.

Date: 2021
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DOI: 10.1038/s41467-021-20923-z

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