Enhancing the Reversibility of Lattice Oxygen Redox Through Modulated Transition Metal–Oxygen Covalency for Layered Battery Electrodes
Abstract
Utilizing reversible lattice oxygen redox (OR) in battery electrodes is an essential strategy to overcome the capacity limitation set by conventional transition metal redox. However, lattice OR reactions are often accompanied with irreversible oxygen oxidation, leading to local structural transformations and voltage/capacity fading. Herein, it is proposed that the reversibility of lattice OR can be remarkably improved through modulating transition metal-oxygen covalency for layered electrode of Na-ion batteries. By developing a novel layered P2-Na0.6 Mg0.15 Mn0.7 Cu0.15 O2 electrode, it is demonstrated that the highly electronegative Cu dopants can improve the lattice OR reversibility to 95% compared to 73% for Cu-free counterpart, as directly quantified through high-efficiency mapping of resonant inelastic X-ray scattering. Crucially, the large energetic overlap between Cu 3d and O 2p states dictates the rigidity of oxygen framework, which effectively mitigates the structural distortion of local oxygen environment upon (de)sodiation and leads to the enhanced lattice OR reversibility. The electrode also exhibits a completely solid-solution reaction with an ultralow volume change of only 0.45% and a reversible metal migration upon cycling, which together ensure the improved electrochemical performance. Finally, these results emphasize the critical role of transition metal-oxygen covalency for enhancing the reversibility of lattice OR towardmore »
- Authors:
-
[1]
- Soochow University, Suzhou (China)
- Chinese Academy of Sciences (CAS), Fuzhou (China)
- Nanjing Univ. (China); Collaborative Innovation Center of Advanced Microstructures (CICAM), Nanjing (China)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
- Tsinghua Univ., Beijing (China)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; National Natural Science Foundation of China (NSFC); Natural Science Foundation of Jiangsu Province; Gusu Innovative and Entrepreneurial Talent
- OSTI Identifier:
- 1958131
- Grant/Contract Number:
- AC02-05CH11231; 11905154; BK20190814; ZXL2019245
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Materials
- Additional Journal Information:
- Journal Volume: 34; Journal Issue: 20; Journal ID: ISSN 0935-9648
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; lattice oxygen redox; layered electrodes; metal-oxygen covalency; Na-ion batteries; RIXS; structural stability
Citation Formats
Cheng, Chen, Chen, Chi, Chu, Shiyong, Hu, Haolv, Yan, Tianran, Xia, Xiao, Feng, Xuefei, Guo, Jinghua, Sun, Dan, Wu, Jinpeng, Guo, Shaohua, and Zhang, Liang. Enhancing the Reversibility of Lattice Oxygen Redox Through Modulated Transition Metal–Oxygen Covalency for Layered Battery Electrodes. United States: N. p., 2022.
Web. doi:10.1002/adma.202201152.
Cheng, Chen, Chen, Chi, Chu, Shiyong, Hu, Haolv, Yan, Tianran, Xia, Xiao, Feng, Xuefei, Guo, Jinghua, Sun, Dan, Wu, Jinpeng, Guo, Shaohua, & Zhang, Liang. Enhancing the Reversibility of Lattice Oxygen Redox Through Modulated Transition Metal–Oxygen Covalency for Layered Battery Electrodes. United States. https://doi.org/10.1002/adma.202201152
Cheng, Chen, Chen, Chi, Chu, Shiyong, Hu, Haolv, Yan, Tianran, Xia, Xiao, Feng, Xuefei, Guo, Jinghua, Sun, Dan, Wu, Jinpeng, Guo, Shaohua, and Zhang, Liang. Mon .
"Enhancing the Reversibility of Lattice Oxygen Redox Through Modulated Transition Metal–Oxygen Covalency for Layered Battery Electrodes". United States. https://doi.org/10.1002/adma.202201152. https://www.osti.gov/servlets/purl/1958131.
@article{osti_1958131,
title = {Enhancing the Reversibility of Lattice Oxygen Redox Through Modulated Transition Metal–Oxygen Covalency for Layered Battery Electrodes},
author = {Cheng, Chen and Chen, Chi and Chu, Shiyong and Hu, Haolv and Yan, Tianran and Xia, Xiao and Feng, Xuefei and Guo, Jinghua and Sun, Dan and Wu, Jinpeng and Guo, Shaohua and Zhang, Liang},
abstractNote = {Utilizing reversible lattice oxygen redox (OR) in battery electrodes is an essential strategy to overcome the capacity limitation set by conventional transition metal redox. However, lattice OR reactions are often accompanied with irreversible oxygen oxidation, leading to local structural transformations and voltage/capacity fading. Herein, it is proposed that the reversibility of lattice OR can be remarkably improved through modulating transition metal-oxygen covalency for layered electrode of Na-ion batteries. By developing a novel layered P2-Na0.6 Mg0.15 Mn0.7 Cu0.15 O2 electrode, it is demonstrated that the highly electronegative Cu dopants can improve the lattice OR reversibility to 95% compared to 73% for Cu-free counterpart, as directly quantified through high-efficiency mapping of resonant inelastic X-ray scattering. Crucially, the large energetic overlap between Cu 3d and O 2p states dictates the rigidity of oxygen framework, which effectively mitigates the structural distortion of local oxygen environment upon (de)sodiation and leads to the enhanced lattice OR reversibility. The electrode also exhibits a completely solid-solution reaction with an ultralow volume change of only 0.45% and a reversible metal migration upon cycling, which together ensure the improved electrochemical performance. Finally, these results emphasize the critical role of transition metal-oxygen covalency for enhancing the reversibility of lattice OR toward high-capacity electrodes employing OR chemistry.},
doi = {10.1002/adma.202201152},
journal = {Advanced Materials},
number = 20,
volume = 34,
place = {United States},
year = {Mon Apr 11 00:00:00 EDT 2022},
month = {Mon Apr 11 00:00:00 EDT 2022}
}
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