Journal
ADVANCED MATERIALS
Volume 30, Issue 1, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201704171
Keywords
compressive strain; enhanced electrochemical performance; exterior atomic vacancy; oxygen reduction reaction; PdCuCo alloys
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Funding
- National Key R D Program [2016YFD0500706]
- National Natural Science Foundation of China [21375043, 21778020]
- Sci-tech Innovation Foundation of Huazhong Agriculture University [2662017PY042]
- Research Grant Council of Hong Kong [PolyU 152145/15E]
- Hong Kong Polytechnic University [1-BBA3, 1-ZVK1, 1-ZVGH]
- Natural Science Foundation of Jiangsu Province [BK20140526]
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Structure-engineered Pd-based catalysts at the atomic level can effectively improve the catalytic performance for oxygen or small organic molecules electrocatalysis, comparable to or even superior to that of commercial Pt/C. Here, PdCuCo anisotropic structure (AS) electrocatalysts are synthesized with abundant vacancy defects on the exterior surface, which is unambiguously verified by aberration-corrected transmission electron microscopy. The PdCuCo-AS with vacancy (v-PdCuCo-AS) shows excellent electrochemical activity toward oxygen reduction (ORR) and oxidation of alcohols. The mass activity of the v-PdCuCo-AS is 0.18 A mg(-1) at 0.9 V versus reversible hydrogen electrode (RHE), which is 15.55 times larger than that of the commercial Pd/C catalyst in acidic electrolyte. According to the theoretical calculations, this significant improvement can be understood as a result of the promoted charge transfer by polarized electronic structures of the v-PdCuCo-AS in the processes of ORR. The synergistic effect of the correlated defects and the compressive strain caused by the doping Co and Cu atoms effectively improve the electrocatalysis activity for the ORR in acidic/alkaline electrolyte on the v-PdCuCo-AS stems. This approach provides a strategy to design other AS structures for improving their electrochemical performance.
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