析氧
催化作用
双功能
氧化物
化学工程
钙钛矿(结构)
非阻塞I/O
化学
氧气
氧化还原
金属
无机化学
电化学
材料科学
纳米技术
电极
物理化学
冶金
生物化学
工程类
有机化学
作者
Zhongliang Xiao,Haoliang Huang,Sixia Hu,Zhuanglin Weng,Ying-Wen Huang,Bing Du,Xierong Zeng,Yuying Meng,Chuanwei Huang
标识
DOI:10.1002/smtd.202300793
摘要
The high-efficient and low-cost oxygen evolution reaction (OER) is decisive for applications of oxide catalysts in metal-air batteries, electrolytic cells, and energy-storage technologies. Delicate regulations of active surface and catalytic reaction pathway of oxide materials principally determine thermodynamic energy barrier and kinetic rate during catalytic reactions, and thus have crucial impacts on OER performance. Herein, a synergistic modulation of catalytically active surface and reaction pathway through facile topotactic transformations switching from perovskite (PV) LaNiO3.0 film to infinite-layer (IL) LaNiO2.0 film is demonstrated, which absolutely contributes to improving OER performance. The square-planar NiO4 coordination of IL-LaNiO2.0 brings about more electrochemically active metal (Ni+ ) sites on the film surface. Meanwhile, the oxygen-deficient driven PV- IL topotactic transformations lead to a reaction pathway converted from absorbate evolution mechanism to lattice-oxygen-mediated mechanism (LOM). The non-concerted proton-electron transfer of LOM pathway, evidenced by the pH-dependent OER kinetics, further boosts the OER activity of IL-LaNiO2.0 films. These findings will advance the in-depth understanding of catalytic mechanisms and open new possibilities for developing highly active perovskite-derived oxide catalysts.
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