Boosting oxygen reduction activity and enhancing stability through structural transformation of layered lithium manganese oxide

Xuepeng Zhong, M’hamed Oubla, Xiao Wang, Yangyang Huang, Huiyan Zeng, Shaofei Wang, Kun Liu, Jian Zhou, Lunhua He, Haihong Zhong, Nicolas Alonso-Vante, Chin-Wei Wang, Wen-Bin Wu, Hong-Ji Lin, Chien-Te Chen, Zhiwei Hu (), Yunhui Huang () and Jiwei Ma ()
Additional contact information
Xuepeng Zhong: Tongji University
M’hamed Oubla: Tongji University
Xiao Wang: Max Planck Institute for Chemical Physics of Solids
Yangyang Huang: Tongji University
Huiyan Zeng: Tongji University
Shaofei Wang: Australian Nuclear Science and Technology Organization
Kun Liu: Xi’an Jiaotong University
Jian Zhou: Xi’an Jiaotong University
Lunhua He: Chinese Academy of Sciences
Haihong Zhong: University of Poitiers
Nicolas Alonso-Vante: University of Poitiers
Chin-Wei Wang: National Synchrotron Radiation Research Center
Wen-Bin Wu: National Synchrotron Radiation Research Center
Hong-Ji Lin: National Synchrotron Radiation Research Center
Chien-Te Chen: National Synchrotron Radiation Research Center
Zhiwei Hu: Max Planck Institute for Chemical Physics of Solids
Yunhui Huang: Tongji University
Jiwei Ma: Tongji University

Nature Communications, 2021, vol. 12, issue 1, 1-12

Abstract: Abstract Structural degradation in manganese oxides leads to unstable electrocatalytic activity during long-term cycles. Herein, we overcome this obstacle by using proton exchange on well-defined layered Li2MnO3 with an O3-type structure to construct protonated Li2-xHxMnO3-n with a P3-type structure. The protonated catalyst exhibits high oxygen reduction reaction activity and excellent stability compared to previously reported cost-effective Mn-based oxides. Configuration interaction and density functional theory calculations indicate that Li2-xHxMnO3-n has fewer unstable O 2p holes with a Mn3.7+ valence state and a reduced interlayer distance, originating from the replacement of Li by H. The former is responsible for the structural stability, while the latter is responsible for the high transport property favorable for boosting activity. The optimization of both charge states to reduce unstable O 2p holes and crystalline structure to reduce the reaction pathway is an effective strategy for the rational design of electrocatalysts, with a likely extension to a broad variety of layered alkali-containing metal oxides.

Date: 2021
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Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-23430-3

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DOI: 10.1038/s41467-021-23430-3

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