Electro-catalyst design with superior performance and reduced precious metal content (compared to state-of-the-art Pt/C) has been a challenge in proton exchange membrane fuel cells, preventing their widespread adoption. Metallic glasses have recently shown promising performance and large electrochemical surface area in catalytic reactions. The electro-catalytic behavior of recently developed Pt-, Pd-, and Pt/Pd-based metallic glasses was evaluated in this study using scanning electrochemical microscopy. The influence of chemistry and electronic structure on catalytic behavior was studied using scanning kelvin probe technique. The work function for the metallic glasses was lower by 75 mV to 175 mV compared to pure Pt. This resulted in higher catalytic activity for the amorphous alloys, which was attributed to the ease of charge transfer on the surface. The binding energy for the metallic glasses, measured using X-ray photoelectron spectroscopy, was higher by 0.2 eV to 0.4 eV. This explained easier removal of adsorbed species from the surface of amorphous alloys. The synergistic effect of Pt and Pd in alloys containing both the noble metals was demonstrated towards hydrogen oxidation reaction.
The compositional dependence and influence of relaxation state on the deformation behavior of a Pt–Pd-based bulk metallic glasses model system was investigated, where platinum is systematically replaced by topologically equivalent palladium atoms. The hardness and modulus increased with rising Pd content as well as by annealing below the glass transition temperature. Decreasing strain-rate sensitivity and increasing serration length are observed in nano indentation with increase in Pd content as well as thermal relaxation. Micro-pillar compression for alloys with different Pt/Pd ratios validated the greater tendency for shear localization and brittle behavior of the Pd-rich alloys. Based on total scattering experiments with synchrotron X-ray radiation, a correlation between the increase in stiffer 3-atom cluster connections and reduction in strain-rate sensitivity, as a measure of ductility, with Pd content and thermal history is suggested.
more » « less- NSF-PAR ID:
- 10373760
- Publisher / Repository:
- Nature Publishing Group
- Date Published:
- Journal Name:
- Scientific Reports
- Volume:
- 12
- Issue:
- 1
- ISSN:
- 2045-2322
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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