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


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.

SUBMITTER: Zamora Zeledon JA 

PROVIDER: S-EPMC7840808 | biostudies-literature | 2021 Jan

REPOSITORIES: biostudies-literature

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

Zamora Zeledón José A JA   Stevens Michaela Burke MB   Gunasooriya G T Kasun Kalhara GTKK   Gallo Alessandro A   Landers Alan T AT   Kreider Melissa E ME   Hahn Christopher C   Nørskov Jens K JK   Jaramillo Thomas F TF  

Nature communications 20210127 1


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  ...[more]

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