Huiyuan Chen, Chunhua Shu, Hao Deng, Kerong He, Wei Hu
{"title":"富锂阴极Li1.25Ni0.5Mn0.25O2运行过程中晶格氧的热力学稳定性研究","authors":"Huiyuan Chen, Chunhua Shu, Hao Deng, Kerong He, Wei Hu","doi":"10.1007/s10008-025-06316-y","DOIUrl":null,"url":null,"abstract":"<div><p>Li-rich layered cathode materials are considered to be the most promising cathode materials for high energy density Li-ion batteries due to its high capacity. However, oxygen evolution leads to serious failure problems and hinders its wide application. To disclose the mechanism of oxygen evolution, the lattice distortion and thermodynamic stability of lattice oxygen in Li-rich layered cathode materials Li<sub>1.25-<i>x</i></sub>Ni<sub>0.5</sub>Mn<sub>0.25</sub>O<sub>2</sub> are investigated by employing first-principles computational methods in this work. The results show that the change of lattice volume is mainly related to the expansion or collapse of the cell in the z-direction. In the ground state, oxygen vacancies (O-vacancies) easily occur when the Li content is below 0.7. The formation of O-vacancies in cathode materials is closely related to temperature and oxygen partial pressure. Increasing the temperature promotes the formation of O-vacancies. However, increasing the oxygen partial pressure is favorable to suppress the formation of O-vacancies. This study provides a theoretical basis for the design of Li-rich cathodes with high stability.</p></div>","PeriodicalId":665,"journal":{"name":"Journal of Solid State Electrochemistry","volume":"29 10","pages":"4399 - 4405"},"PeriodicalIF":2.6000,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"A study of the thermodynamic stability of lattice oxygen in Li-rich cathode Li1.25Ni0.5Mn0.25O2 during operation\",\"authors\":\"Huiyuan Chen, Chunhua Shu, Hao Deng, Kerong He, Wei Hu\",\"doi\":\"10.1007/s10008-025-06316-y\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Li-rich layered cathode materials are considered to be the most promising cathode materials for high energy density Li-ion batteries due to its high capacity. However, oxygen evolution leads to serious failure problems and hinders its wide application. To disclose the mechanism of oxygen evolution, the lattice distortion and thermodynamic stability of lattice oxygen in Li-rich layered cathode materials Li<sub>1.25-<i>x</i></sub>Ni<sub>0.5</sub>Mn<sub>0.25</sub>O<sub>2</sub> are investigated by employing first-principles computational methods in this work. The results show that the change of lattice volume is mainly related to the expansion or collapse of the cell in the z-direction. In the ground state, oxygen vacancies (O-vacancies) easily occur when the Li content is below 0.7. The formation of O-vacancies in cathode materials is closely related to temperature and oxygen partial pressure. Increasing the temperature promotes the formation of O-vacancies. However, increasing the oxygen partial pressure is favorable to suppress the formation of O-vacancies. This study provides a theoretical basis for the design of Li-rich cathodes with high stability.</p></div>\",\"PeriodicalId\":665,\"journal\":{\"name\":\"Journal of Solid State Electrochemistry\",\"volume\":\"29 10\",\"pages\":\"4399 - 4405\"},\"PeriodicalIF\":2.6000,\"publicationDate\":\"2025-04-16\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Solid State Electrochemistry\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s10008-025-06316-y\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"ELECTROCHEMISTRY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Solid State Electrochemistry","FirstCategoryId":"5","ListUrlMain":"https://link.springer.com/article/10.1007/s10008-025-06316-y","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"ELECTROCHEMISTRY","Score":null,"Total":0}
A study of the thermodynamic stability of lattice oxygen in Li-rich cathode Li1.25Ni0.5Mn0.25O2 during operation
Li-rich layered cathode materials are considered to be the most promising cathode materials for high energy density Li-ion batteries due to its high capacity. However, oxygen evolution leads to serious failure problems and hinders its wide application. To disclose the mechanism of oxygen evolution, the lattice distortion and thermodynamic stability of lattice oxygen in Li-rich layered cathode materials Li1.25-xNi0.5Mn0.25O2 are investigated by employing first-principles computational methods in this work. The results show that the change of lattice volume is mainly related to the expansion or collapse of the cell in the z-direction. In the ground state, oxygen vacancies (O-vacancies) easily occur when the Li content is below 0.7. The formation of O-vacancies in cathode materials is closely related to temperature and oxygen partial pressure. Increasing the temperature promotes the formation of O-vacancies. However, increasing the oxygen partial pressure is favorable to suppress the formation of O-vacancies. This study provides a theoretical basis for the design of Li-rich cathodes with high stability.
期刊介绍：
The Journal of Solid State Electrochemistry is devoted to all aspects of solid-state chemistry and solid-state physics in electrochemistry.
The Journal of Solid State Electrochemistry publishes papers on all aspects of electrochemistry of solid compounds, including experimental and theoretical, basic and applied work. It equally publishes papers on the thermodynamics and kinetics of electrochemical reactions if at least one actively participating phase is solid. Also of interest are articles on the transport of ions and electrons in solids whenever these processes are relevant to electrochemical reactions and on the use of solid-state electrochemical reactions in the analysis of solids and their surfaces.
The journal covers solid-state electrochemistry and focusses on the following fields: mechanisms of solid-state electrochemical reactions, semiconductor electrochemistry, electrochemical batteries, accumulators and fuel cells, electrochemical mineral leaching, galvanic metal plating, electrochemical potential memory devices, solid-state electrochemical sensors, ion and electron transport in solid materials and polymers, electrocatalysis, photoelectrochemistry, corrosion of solid materials, solid-state electroanalysis, electrochemical machining of materials, electrochromism and electrochromic devices, new electrochemical solid-state synthesis.
The Journal of Solid State Electrochemistry makes the professional in research and industry aware of this swift progress and its importance for future developments and success in the above-mentioned fields.
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