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Atomic Vacancies Control of Pd‐Based Catalysts for Enhanced Electrochemical Performance
Author(s) -
Zuo Yunpeng,
Rao Dewei,
Li Shuo,
Li Tingting,
Zhu Guilin,
Chen Shuangming,
Song Li,
Chai Yang,
Han Heyou
Publication year - 2018
Publication title -
advanced materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.707
H-Index - 527
eISSN - 1521-4095
pISSN - 0935-9648
DOI - 10.1002/adma.201704171
Subject(s) - electrocatalyst , electrochemistry , materials science , catalysis , electrolyte , vacancy defect , electrode , electron transfer , reversible hydrogen electrode , chemical engineering , inorganic chemistry , nanotechnology , chemistry , crystallography , working electrode , organic chemistry , engineering
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.