Enhancing Oxygen Evolution Reaction via a Surface Reconstruction-Induced Lattice Oxygen Mechanism

Systematic control of surface reconstruction during catalysis remains challenging. Particularly, inducing a surface structure reconstruction following the lattice oxygen oxidation mechanism (LOM), which can reduce the overpotential in oxygen evolution reaction (OER) catalysts, has not been extensively investigated. The mechanism of the OER of transition-metal-oxide-based catalysts can be facilitated by manipulating the local coordination structure to modulate the reactivity of lattice oxygen. Herein, we report an in situ surface reconstruction strategy by doping F into LaNiO3 to distort the NiO6 octahedral sites, weaken the Ni–O bonds, and increase lattice oxygen reactivity during OER. The as-prepared LaNiO2.9F0.1 exhibits enhanced performances toward OER with a low overpotential of 320 mV at 10 mA cm–2, a small Tafel slope of 78 mV dec–1, and good long-term stability in alkaline media. Comprehensive analysis reveals that the in situ self-reconstructed surface favors the LOM pathway for the OER, resulting in a considerably improved performance. These results demonstrate that the lattice oxygen acts as a switch for directing the OER mechanism, and further, controlling the lattice oxygen reactivity emerges as a promising approach for dynamic self-reconstruction to highly active OER electrocatalysts.

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Publication Details

Journal
ACS Catalysis
Published
2024-09-30
DOI
https://doi.org/10.1021/acscatal.4c03594
Citations
56
Primary Topic
Electrocatalysts for Energy Conversion
Type
article
Field-Weighted Citation Impact
5.73

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article

Enhancing Oxygen Evolution Reaction via a Surface Reconstruction-Induced Lattice Oxygen Mechanism

Jeongwoo Han, Hyejeong Hyun, Alexander A. Ryabin, Bonho Koo et al.
56 citations
ACS Catalysis
Electrocatalysts for Energy Conversion
5.73
article

Enhancing Oxygen Evolution Reaction via a Surface Reconstruction-Induced Lattice Oxygen Mechanism

Jeongwoo Han, Hyejeong Hyun, Alexander A. Ryabin, Bonho Koo, Sebastian Kunze, Keun Hwa Chae, Chang Hyuck Choi, Sunghoon Han, Jongwoo Lim, Hyungjun Kim, Juwon Kim, Jian Wang, Sejun Kim, Subin Choi, Shu-Chih Haw
article en
56 citations

Abstract

Systematic control of surface reconstruction during catalysis remains challenging. Particularly, inducing a surface structure reconstruction following the lattice oxygen oxidation mechanism (LOM), which can reduce the overpotential in oxygen evolution reaction (OER) catalysts, has not been extensively investigated. The mechanism of the OER of transition-metal-oxide-based catalysts can be facilitated by manipulating the local coordination structure to modulate the reactivity of lattice oxygen. Herein, we report an in situ surface reconstruction strategy by doping F into LaNiO3 to distort the NiO6 octahedral sites, weaken the Ni–O bonds, and increase lattice oxygen reactivity during OER. The as-prepared LaNiO2.9F0.1 exhibits enhanced performances toward OER with a low overpotential of 320 mV at 10 mA cm–2, a small Tafel slope of 78 mV dec–1, and good long-term stability in alkaline media. Comprehensive analysis reveals that the in situ self-reconstructed surface favors the LOM pathway for the OER, resulting in a considerably improved performance. These results demonstrate that the lattice oxygen acts as a switch for directing the OER mechanism, and further, controlling the lattice oxygen reactivity emerges as a promising approach for dynamic self-reconstruction to highly active OER electrocatalysts.

ACS CatalysisVol. 14(20)
Pohang University of Science and Technology (KR), Seoul National University (KR), Korea Advanced Institute of Science and Technology (KR), City University of Hong Kong (HK), Yonsei University (KR), National University (SD), National Synchrotron Radiation Research Center (TW), Korea Institute of Science and Technology (KR)
Seoul National University, National Research Foundation of Korea
Openalex Percentile: Top 3%
Electrocatalysts for Energy Conversion
5.73
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