Alloy-composition-dependent oxygen reduction reaction activity and electrochemical stability of Pt-based bimetallic systems: a model electrocatalyst study of Pt/PtxNi100−x(111)

Literature Information

Publication Date 2018-04-03
DOI 10.1039/C8CP01217B
Impact Factor 3.676
Authors

Naoto Todoroki, Ryutaro Kawamura, Masato Asano, Ren Sasakawa, Shuntaro Takahashi, Toshimasa Wadayama


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Abstract

The oxygen reduction reaction (ORR) activity and electrochemical stability of well-defined n monolayer (ML)-Pt/PtxNi100−x(111) (n = 2 and 4; x = 75, 50, and 25) model electrocatalyst surfaces were investigated in this study. The initial activity of the as-prepared two-monolayered Pt-covered PtxNi100−x(111) substrates (2ML-Pt/PtxNi100−x(111)) increased with increasing Ni composition in the PtxNi100−x(111) substrate. In particular, 2ML-Pt/Pt25Ni75(111) showed the initial activity that was 25 times higher than that of clean Pt(111) although the higher Ni composition resulted in destabilization of the catalyst upon the application of potential cycles (PCs). As for 4ML-Pt/PtxNi100−x(111), activity enhancements were insensitive to alloy composition and thicker Pt shell layers stabilized the catalyst against PC applications. In particular, the activities of 4ML-Pt/Pt50Ni50(111) and 4ML-Pt/Pt25Ni75(111) gradually increased during 1000 PCs probably because of the PC-induced mono-atomic heights and nanometer-size islands that had (110) and (100) steps introduced into the topmost (111) terraces. Thus, the simultaneous tuning of core–alloy composition and Pt shell thickness is vital for developing practical, highly efficient Pt-based alloy ORR electrocatalysts.

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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
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Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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