期刊
NATURE COMMUNICATIONS
卷 12, 期 1, 页码 -出版社
NATURE RESEARCH
DOI: 10.1038/s41467-021-20923-z
关键词
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资金
- Toyota Research Institute
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science Program
- National Science Foundation [ECCS-1542152]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Science [DE-AC02-76SF00515]
- Gates Millennium Graduate Fellowship/Scholarship
- Stanford's Office of VPGE EDGE Fellowship
Alloying is a powerful tool to enhance the electrocatalytic activity of Pd-based catalysts while reducing precious metal content. Experimental results show that even slight alloying with Ag can significantly improve the intrinsic activity of the catalysts.
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 0.1M 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 0.9V 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. Electrocatalyst development is key to improving the performance and viability of many electrochemical energy technologies. Here, the authors design Ag-Pd alloys with specifically tuned electronic structures to have enhanced oxygen reduction electrocatalysis and decreased precious metal content.
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