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

Autor: Zamora Zeledón JA; Department of Chemical Engineering, Stanford University, 443 Via Ortega, Stanford, CA, 94305, USA.; SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA, 94025, USA., Stevens MB; Department of Chemical Engineering, Stanford University, 443 Via Ortega, Stanford, CA, 94305, USA.; SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA, 94025, USA., Gunasooriya GTKK; Catalysis Theory Center, Department of Physics, Technical University of Denmark, 2800 Kongens, Lyngby, Denmark., Gallo A; Department of Chemical Engineering, Stanford University, 443 Via Ortega, Stanford, CA, 94305, USA.; SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA, 94025, USA., Landers AT; SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA, 94025, USA.; Department of Chemistry, Stanford University, 333 Campus Drive, Stanford, CA, 94305, USA., Kreider ME; Department of Chemical Engineering, Stanford University, 443 Via Ortega, Stanford, CA, 94305, USA.; SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA, 94025, USA., Hahn C; Department of Chemical Engineering, Stanford University, 443 Via Ortega, Stanford, CA, 94305, USA.; SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA, 94025, USA., Nørskov JK; Catalysis Theory Center, Department of Physics, Technical University of Denmark, 2800 Kongens, Lyngby, Denmark., Jaramillo TF; Department of Chemical Engineering, Stanford University, 443 Via Ortega, Stanford, CA, 94305, USA. jaramillo@stanford.edu.; SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA, 94025, USA. jaramillo@stanford.edu.
Jazyk: angličtina
Zdroj: Nature communications [Nat Commun] 2021 Jan 27; Vol. 12 (1), pp. 620. Date of Electronic Publication: 2021 Jan 27.
DOI: 10.1038/s41467-021-20923-z
Abstrakt: 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. Ag 0.1 Pd 0.9 ) 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.
Databáze: MEDLINE