Journal
ACS CATALYSIS
Volume 10, Issue 17, Pages 9967-9976Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c02690
Keywords
electrochemical deposition; dealloying; porous film; electrocatalysis; ORR; alkaline media
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Funding
- Center for AlkalineBased Energy Solutions, an Energy Frontier Research Center program - US Department of Energy [DE-SC0019445]
- National Science Foundation [DMR 1808383]
- S3IP, State University of New York at Binghamton
- National Science Foundation Materials Research Science and Engineering Center program [DMR-1719875]
- ACS PRF [58196-ND10]
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Fraction-controlled Pt-Cu-based porous films were prepared using an electrochemical deposition-stripping synthetic approach, and their structure, composition, and electronic structure were characterized using scanning/transmission electron microscopy-energy dispersive X-ray spectroscopy, and X-ray photoelectron spectroscopy techniques. These materials exhibited superb electrocatalytic activity toward the oxygen reduction reaction (ORR) in alkaline media. For example, the mass activity of a Pt45Cu55 film, at 0.90 V (vs RHE), was 3.5x higher than that of commercial Pt/C (40 wt % Pt). This activity enhancement is attributed, in part, to the ligand effect of the Cu component. The introduction of Au, as a third metal constituent to the porous films, further improved the ORR performance significantly. The synergistic effect(s) of Au and Pt appear to have a critical impact on the enhancement of the ORR activity. Compositional optimization identified the dealloyed Pt37Cu56Au7 porous film as the best performing electrocatalyst. It also exhibited the highest mass and specific activities (0.871 A/mg(Pt), 1.85 mA/cm(2)) which were 7.20x and 8.15x higher than those of commercial Pt/C (40 wt % Pt), respectively. This ternary alloy thin-film catalyst also exhibited the longest durability, among all tested samples in this study.
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