Qinwen Cui, Songlin Yu, Yi Li, Xingyu Li, Xiaolin Zhao, Wujie Qiu, Jianjun Liu
{"title":"调制富锂阴极的耦合多面体畸变以协同抑制容量和电压衰减","authors":"Qinwen Cui, Songlin Yu, Yi Li, Xingyu Li, Xiaolin Zhao, Wujie Qiu, Jianjun Liu","doi":"10.1002/adma.202505616","DOIUrl":null,"url":null,"abstract":"<p>Achieving significant enhancements in both capacity and voltage stability remains a formidable challenge for Li-rich layered cathodes. The severe performance degradation is attributed to large lattice strain, irreversible oxygen release and transition metal migration, but the most critical factor responsible for structural destabilization is still elusive. Here, based on density functional theory calculations, machine learning and experimental validation, a multi-hierarchy screening of complex multi-element doping systems is developed from electrochemical activity, lattice strain, oxygen stability and transition metal migration barrier. It is further identified that the coupled polyhedral distortion parameter D+σ<sup>2</sup> of the substitution element is the most significant feature that affects the structural stability during cycling. The Li-rich layered cathode developed based on the predicted results exhibits remarkable long-term capacity stability (95.8% capacity retention over 300 cycles) and negligible voltage loss (0.02% voltage decay per cycle). This study provides a general approach by modulating coupled polyhedral distortion for the rational design of cathode materials and can be expanded to the discovery of other advanced electrodes.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"37 29","pages":""},"PeriodicalIF":26.8000,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Modulating Coupled Polyhedral Distortion in Li-Rich Cathodes for Synergistically Inhibiting Capacity and Voltage Decay\",\"authors\":\"Qinwen Cui, Songlin Yu, Yi Li, Xingyu Li, Xiaolin Zhao, Wujie Qiu, Jianjun Liu\",\"doi\":\"10.1002/adma.202505616\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Achieving significant enhancements in both capacity and voltage stability remains a formidable challenge for Li-rich layered cathodes. The severe performance degradation is attributed to large lattice strain, irreversible oxygen release and transition metal migration, but the most critical factor responsible for structural destabilization is still elusive. Here, based on density functional theory calculations, machine learning and experimental validation, a multi-hierarchy screening of complex multi-element doping systems is developed from electrochemical activity, lattice strain, oxygen stability and transition metal migration barrier. It is further identified that the coupled polyhedral distortion parameter D+σ<sup>2</sup> of the substitution element is the most significant feature that affects the structural stability during cycling. The Li-rich layered cathode developed based on the predicted results exhibits remarkable long-term capacity stability (95.8% capacity retention over 300 cycles) and negligible voltage loss (0.02% voltage decay per cycle). This study provides a general approach by modulating coupled polyhedral distortion for the rational design of cathode materials and can be expanded to the discovery of other advanced electrodes.</p>\",\"PeriodicalId\":114,\"journal\":{\"name\":\"Advanced Materials\",\"volume\":\"37 29\",\"pages\":\"\"},\"PeriodicalIF\":26.8000,\"publicationDate\":\"2025-04-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Advanced Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://advanced.onlinelibrary.wiley.com/doi/10.1002/adma.202505616\",\"RegionNum\":1,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Materials","FirstCategoryId":"88","ListUrlMain":"https://advanced.onlinelibrary.wiley.com/doi/10.1002/adma.202505616","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Modulating Coupled Polyhedral Distortion in Li-Rich Cathodes for Synergistically Inhibiting Capacity and Voltage Decay
Achieving significant enhancements in both capacity and voltage stability remains a formidable challenge for Li-rich layered cathodes. The severe performance degradation is attributed to large lattice strain, irreversible oxygen release and transition metal migration, but the most critical factor responsible for structural destabilization is still elusive. Here, based on density functional theory calculations, machine learning and experimental validation, a multi-hierarchy screening of complex multi-element doping systems is developed from electrochemical activity, lattice strain, oxygen stability and transition metal migration barrier. It is further identified that the coupled polyhedral distortion parameter D+σ2 of the substitution element is the most significant feature that affects the structural stability during cycling. The Li-rich layered cathode developed based on the predicted results exhibits remarkable long-term capacity stability (95.8% capacity retention over 300 cycles) and negligible voltage loss (0.02% voltage decay per cycle). This study provides a general approach by modulating coupled polyhedral distortion for the rational design of cathode materials and can be expanded to the discovery of other advanced electrodes.
期刊介绍:
Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.