TY - JOUR
T1 - Tuning of lattice oxygen reactivity and scaling relation to construct better oxygen evolution electrocatalyst
AU - Huang, Zhen-Feng
AU - Xi, Shibo
AU - Song, Jiajia
AU - Dou, Shuo
AU - Li, Xiaogang
AU - Du, Yonghua
AU - Diao, Caozheng
AU - Xu, Zhichuan J.
AU - Wang, Xin
PY - 2021
Y1 - 2021
N2 - 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).
AB - 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).
UR - https://www.scopus.com/pages/publications/85108829741
UR - https://www.scopus.com/record/pubmetrics.uri?eid=2-s2.0-85108829741&origin=recordpage
U2 - 10.1038/s41467-021-24182-w
DO - 10.1038/s41467-021-24182-w
M3 - RGC 21 - Publication in refereed journal
C2 - 34183651
SN - 2041-1723
VL - 12
JO - Nature Communications
JF - Nature Communications
M1 - 3992
ER -
SDG 7 Affordable and Clean Energy