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Insights into layered-tunnel dynamic structural evolution based on local coordination chemistry regulation for high-energy-density and long-cycle-life sodium-ion oxide cathodes

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InfoMat 2023年第10期5卷 32-42页

作者： Yao Xiao Yi-Feng Liu Hong-Wei Li Jia-Yang Li Jing-Qiang Wang Hai-Yan Hu Yu Su Zhuang-Chun Jian Hu-Rong Yao Shuang-Qiang Chen Xian-Xiang Zeng Xiong-Wei Wu Jia-Zhao Wang Yan-Fang Zhu Shi-Xue Dou Shu-Lei Chou Institute for Carbon Neutralization College of Chemistry and Materials EngineeringWenzhou UniversityWenzhouthe People's Republic of China Wenzhou Key Laboratory of sodium-ion Batteries Wenzhou University Technology Innovation Institute for Carbon NeutralizationWenzhouthe People's Republic of China State Key Laboratory of Electrical Insulation and Power Equipment School of Electrical EngineeringXi'an Jiaotong UniversityXi'anthe People'sRepublic of China School of Chemistry and Materials Science Hunan Agricultural UniversityChangshathe People's Republic of China Institute for Superconducting and Electronic Materials Australian Institute for Innovative Materials University of Wollongong Innovation CampusNorth WollongongNew South WalesAustralia Fujian Provincial Key Laboratory of Quantum Manipulation and New Energy Materials College of Physics and EnergyFujian Normal UniversityFuzhouthe People's Republic of China

The pursuit of high energy density while achieving long cycle life remains a challenge in developing transition metal(TM)oxide cathode materials for sodium-ion batteries(SIBs).Here,we present a concept of precisely manipulating structural evolution via local coordination chemistry regulation to design high-performance composite cathode *** controllable structural evolution process is realized by tuning magnesium content in Na0.6Mn1-xMgxO2,which is elucidated by a combination of experimental analysis and theoretical *** substitution of Mg into Mn sites not only induces a unique structural evolu-tion from layered–tunnel structure to layered structure but also mitigates the Jahn–Teller distortion of Mn3+.Meanwhile,benefiting from the strong ionic inter-action between Mg2+and O2-,local environments around O2-coordinated with electrochemically inactive Mg2+are anchored in the TM layer,providing a pinning effect to stabilize crystal structure and smooth electrochemical *** layered–tunnel Na0.6Mn0.95Mg0.05O2 cathode material delivers 188.9 mAh g-1 of specific capacity,equivalent to 508.0 Wh kg-1 of energy density at 0.5C,and exhibits 71.3%of capacity retention after 1000 cycles at 5C as well as excellent compatibility with hard carbon *** work may provide new insights of manipulating structural evolution in composite cathode materials via local coordi-nation chemistry regulation and inspire more novel design of high-performance SIB cathode materials.

关键词： dynamic structural evolution high-energy-density layered-tunnel structure local coordination chemistry sodium-ion oxide cathodes

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