Atomic Ensemble and Electronic Effects in Ag-Rich AgPd Nanoalloy Catalysts for Oxygen Reduction in Alkaline Media
Open accessAbstract
The ability to design and characterize uniform, bimetallic alloy nanoparticles, where the less active metal enhances the activity of the more active metal, would be of broad interest in catalysis. Herein, we demonstrate that simultaneous reduction of Ag and Pd precursors provides uniform, Ag-rich AgPd alloy nanoparticles (~5 nm) with high activities for the oxygen reduction reaction (ORR) in alkaline media. The particles are crystalline and uniformly alloyed, as shown by X-ray diffraction and probe corrected scanning transmission electron microscopy. The ORR mass activity per total metal was 60% higher for the AgPd(2) alloy relative to pure Pd. The mass activities were 2.7 and 3.2 times higher for Ag(9)Pd (340 mA/mg(metal)) and Ag(4)Pd (598 mA/mg(metal)), respectively, than those expected for a linear combination of mass activities of Ag (60 mA/mg(Ag)) and Pd (799 mA/mg(Pd)) particles, based on rotating disk voltammetry. Moreover, these synergy factors reached 5-fold on a Pd mass basis. For silver-rich alloys (Ag(≥4)Pd), the particle surface is shown to contain single Pd atoms surrounded by Ag from cyclic voltammetry and CO stripping measurements. This morphology is favorable for the high activity through a combination of modified electronic structure, as shown by XPS, and ensemble effects, which facilitate the steps of oxygen bond breaking and desorption for the ORR. This concept of tuning the heteroatomic interactions on the surface of small nanoparticles with low concentrations of precious metals for high synergy in catalytic activity may be expected to be applicable to a wide variety of nanoalloys.
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The existing state of Pd and Pt atoms on the surfaces of the aerogels is not highly-dispersed individual atoms.
“the appearance of the obvious Hupd peak”
From Realization of Au81Pd2Pt9-S8B4.6A3.4 aerogels as superior catalysts toward HER and ORR by synergism of coarse and fine tuning d-band center of Pt (2023) · cites this paper as [49]
In Results and Discussion (page not provided), Hupd peaks emerge in Pd-rich AgPd alloys, where the authors report Pd–Pd contacts rather than only isolated Pd atoms. That supports the interpretation of a peak for Pd in those alloys, but the paper does not establish the surface arrangement of Pd and Pt atoms in the cited aerogels. (LLM, conf=0.86)
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References 62 · Cited by 295
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- Authors
- Slanac, D. A., Hardin, W. G., Johnston, K. P., & Stevenson, K. J.
- Affiliations
- Texas Materials Institute (US)
- Corresponding author
- Johnston, Keith P.
- Stevenson, Keith J.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2012-05-31
- Volume
- 134
- Issue
- 23
- Pages
- 9812-9819
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- PMC
- PMC4890639
- OpenAlex
- W1966412580
- Cited by
- 295
- References
- 62
- Citations by year
- 2026: 7 · 2025: 9 · 2024: 12 · 2023: 21 · 2022: 27 · 2021: 25 · 2020: 25 · 2019: 20 · 2018: 23 · 2017: 28 · 2016: 29 · 2015: 18 · 2014: 20 · 2013: 28 · 2012: 3
- FWCI
- 8.47
- Type
- journal article
- Language
- en
- Open access
- green
- www.ncbi.nlm.nih.gov
- Locations
- Journal of the American Chemical Society (publishedVersion)
- PubMed (publishedVersion)
- Europe PMC (PubMed Central) (acceptedVersion)
- PubMed Central (acceptedVersion)
- Funders
- National Science Foundation
- Welch Foundation
- Canadian Institutes of Health Research
- National Center for Research Resources (G12RR013646)
- Division of Chemistry
- National Institute on Minority Health and Health Disparities (G12MD007591)
- Topics
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
- Physical Sciences › Materials Science › Materials Chemistry › Catalytic Processes in Materials Science
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
- Keywords
- oxygen reduction reaction, alkaline solution, bimetallic nanoparticles, electronic structure, CO stripping, noble metal catalysts
- MeSH terms
- Alloys, Catalysis, Electrons, Oxidation-Reduction, Oxygen, Palladium, Silver, Nanoparticles, Electrochemical Techniques
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