Journal
ELECTROCATALYSIS
Volume 10, Issue 3, Pages 232-242Publisher
SPRINGER
DOI: 10.1007/s12678-019-00517-6
Keywords
Oxygen reduction reaction; Nano-flake-like carbon; Nitrogen-doped carbon; Surface modification; Pt75Ni25(111); Pt-skin; Arc plasma deposition
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Funding
- New Energy and Industrial Technology Development Organization (NEDO) of Japan
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Oxygen reduction reaction (ORR) activity was investigated for nano-flake-like carbon-modified Pt75Ni25(111) surfaces. Surface cleaning through Ar+-sputtering and thermal annealing in an ultra-high vacuum (10(-8)Pa) resulted in a Pt-enriched topmost surface, i.e., a Pt(111)-skin on Pt75Ni25(111). Arc plasma deposition (APD) of graphite under 0.08PaN(2) and in vacuum (10(-6)Pa) generated nitrogen-doped and non-doped nano-flake-like carbon on the Pt(111)-skin surfaces, respectively. For the latter, non-doped carbon-modified Pt(111)-skin, the area-specific initial ORR activity estimated in O-2-saturated 0.1M HClO4 decreased with increasing thickness of the deposited carbon. In contrast, the former, nitrogen-doped carbon with 2 and 6 angstrom mass-thickness enhanced the ORR activity. The Pt 4f band energies for the nitrogen-doped Pt(111)-skin were measured by X-ray photoelectron spectroscopy (XPS) and showed the chemical shift to higher biding energy (0.2eV) compared with the corresponding bands for the non-doped and Pt(111)-skin surfaces. As for the electrochemical structural stability, a specific amount of the non-doped carbon species tends to suppress the degradation of the Pt(111)-skin under applying potential cycles. The results indicate that the surface modifications by the carbon hexagonal networks of the nano-flakes could be applicable to improve ORR performance of the practical Pt-M alloy catalysts.
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