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.
| Original language | English |
|---|---|
| Article number | 620 |
| Journal | Nature Communications |
| Volume | 12 |
| Issue number | 1 |
| Number of pages | 9 |
| ISSN | 2041-1723 |
| DOIs | |
| Publication status | Published - 2021 |
Bibliographical note
Funding Information:This work was supported by the Toyota Research Institute. Some of the research efforts involving thin film synthesis and XAS characterization were supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science Program to the SUNCAT Center for Interface Science and Catalysis. Part of this work was performed at the Stanford Nano Shared Facilities (SNSF), supported by the National Science Foundation under Award ECCS-1542152. We thank SNSF Manger of the Surface Analysis Laboratory, Juliet Jamtgaard, for her valuable assistance in setting up XPS experiments and interpreting the corresponding results. Use of the Stanford Synchrotron Radiation Lightsource (SSRL) at SLAC National Accelerator Laboratory is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Science, under Contract DE-AC02-76SF00515. We thank SSRL Scientists Erik Nelson and Matthew Latimer for their assistance in setting up and operating beamline 14-3. J.A.Z.Z. gratefully acknowledges support of the Gates Millennium Graduate Fellowship/Scholarship and the Stanford’s Office of VPGE EDGE Fellowship.
