Boosting Initial Coulombic Efficiency in Li‐Rich Mn‐based Cathodes by Tuning Orbital Hybridization

Li-rich manganese-based oxides (LRMO) are promising cathode materials for next-generation lithium-ion batteries due to their high-capacity and low-cost merits. However, the low initial coulombic efficiency (ICE) and irreversible oxygen release of LRMO severely hinder their commercialization processes. Here, we employ glyoxal treatment to modulate the hybridization between transition metal (TM) 3d and oxygen (O) 2p orbitals in LRMO. This approach is found to reduce the Co/Mn t<sub>2g</sub>-O 2p hybridization in LRMO while simultaneously activating the Co<sup>2+</sup>/Co<sup>3+</sup> redox below the Fermi level. Our findings demonstrate that tuning TM 3d-O 2p orbital hybridization can be a viable approach to improve the ICE of LMRO. Specifically, the ICE of LRMO can be elevated from 85.3% to 102.5%, and a high specific capacity of 291.2 mAh g<sup>-1</sup> can be achieved at 0.1 C. Moreover, the treated LRMO cathodes exhibit significantly enhanced capacity retention.

Authors

Institutions

Publication Details

Journal
Angewandte Chemie International Edition
Published
2025-05-06
DOI
https://doi.org/10.1002/anie.202501777
Citations
23
Primary Topic
Advancements in Battery Materials
Type
article
Field-Weighted Citation Impact
16.80

Funders

Controls
|||
ALL TIME
JAN
FEB
MAR
APR
MAY
JUN
JUL
AUG
SEP
OCT
article

Boosting Initial Coulombic Efficiency in Li‐Rich Mn‐based Cathodes by Tuning Orbital Hybridization

Yinguo Xiao, Mihai Chu, Junrong Zhang, Ze He et al.
23 citations
Angewandte Chemie International Edition
Advancements in Battery Materials
16.80
article

Boosting Initial Coulombic Efficiency in Li‐Rich Mn‐based Cathodes by Tuning Orbital Hybridization

Yinguo Xiao, Mihai Chu, Junrong Zhang, Ze He, Wei Tang, Tao Zeng, Lunhua He, Maolin Yang, Guojie Chen, Zhongyuan Huang, Yuguang Pu, Rui Wang, Limin Wang, Ziwei Chen, Zheng Jiao, Wenguang Zhao, Xiaohu Wang, Jinqi Li, Xiaoyu Gao
article en
23 citations

Abstract

Li-rich manganese-based oxides (LRMO) are promising cathode materials for next-generation lithium-ion batteries due to their high-capacity and low-cost merits. However, the low initial coulombic efficiency (ICE) and irreversible oxygen release of LRMO severely hinder their commercialization processes. Here, we employ glyoxal treatment to modulate the hybridization between transition metal (TM) 3d and oxygen (O) 2p orbitals in LRMO. This approach is found to reduce the Co/Mn t<sub>2g</sub>-O 2p hybridization in LRMO while simultaneously activating the Co<sup>2+</sup>/Co<sup>3+</sup> redox below the Fermi level. Our findings demonstrate that tuning TM 3d-O 2p orbital hybridization can be a viable approach to improve the ICE of LMRO. Specifically, the ICE of LRMO can be elevated from 85.3% to 102.5%, and a high specific capacity of 291.2 mAh g<sup>-1</sup> can be achieved at 0.1 C. Moreover, the treated LRMO cathodes exhibit significantly enhanced capacity retention.

Angewandte Chemie International EditionVol. 64(28)
King University (US), Sun Yat-sen University (CN), Peking University (CN), University of Cambridge (GB), China Spallation Neutron Source (CN), Peking University Shenzhen Hospital (CN), Politecnico di Milano (IT)
Salt Science Research Foundation, Diamond Light Source, National Natural Science Foundation of China, Basic and Applied Basic Research Foundation of Guangdong Province
Affordable and clean energy
Openalex Percentile: Top 1%
Advancements in Battery Materials
16.80
DOIOpen Access PDFOpenAlex
AI Navigator

Ask Laika to Summarize, Analyze, and Connect papers live on the map.

Summarize Papers & Methodologies

Extract key findings, datasets, and comparative methods across publications.

Benchmark Rankings & Visual Analytics

Rank top research institutions, authors, funders, topics, and journals by Field-Weighted Citation Impact (FWCI) and paper volume with instant charts.

Connect Distant Disciplines

Bridge topological clusters on the map to find hidden collaborative intersections.