Tuning of lattice oxygen reactivity and scaling relation to construct better oxygen evolution electrocatalyst
Huang, Zhen-Feng Xi, Shibo Song, Jiajia Dou, Shuo Li, Xiaogang Du, Yonghua Diao, Caozheng Xu, Zhichuan J. Wang, Xin
Huang, Zhen-Feng
Song, Jiajia
Dou, Shuo
Li, Xiaogang
Du, Yonghua
Xu, Zhichuan J.
Wang, Xin
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Abstract
Developing efficient and low-cost electrocatalysts for oxygen evolution reaction is crucial in realizing practical energy systems for sustainable fuel production and energy storage from renewable energy sources. However, the inherent linear scaling relation for most catalytic materials imposes a theoretical overpotential ceiling, limiting the development of efficient electrocatalysts. Herein, using modeled NaxMn3O7 materials, we report an effective strategy to construct better oxygen evolution electrocatalyst through tuning both lattice oxygen reactivity and scaling relation via alkali metal ion mediation. Specifically, the number of Na+ is linked with lattice oxygen reactivity, which is determined by the number of oxygen hole in oxygen lone-pair states formed by native Mn vacancies, governing the barrier symmetry between O–H bond cleavage and O–O bond formation. On the other hand, the presence of Na+ could have specific noncovalent interaction with pendant oxygen in *OOH to overcome the limitation from linear scaling relation, reducing the overpotential ceiling. Combining in situ spectroscopy-based characterization with first-principles calculations, we demonstrate that an intermediate level of Na+ mediation (NaMn3O7) exhibits the optimum oxygen evolution activity. This work provides a new rational recipe to develop highly efficient catalyst towards water oxidation or other oxidative reactions through tuning lattice oxygen reactivity and scaling relation. © 2021, The Author(s).
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Source Title
Nature Communications
Publisher
Nature Research
Series/Report No.
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Rights
Attribution 4.0 International
Date
2021-06-28
DOI
10.1038/s41467-021-24182-w
Type
Article