{"title":"固态电池中锂金属间界面形态发生的连续计算研究","authors":"Mostafa Faghih Shojaei, Rahul Gulati, Krishna Garikipati","doi":"10.1016/j.jmps.2025.106073","DOIUrl":null,"url":null,"abstract":"<div><div>The design of solid state batteries with lithium anodes is attracting attention for the prospect of high capacity and improved safety over liquid electrolyte systems. The nature of transport with lithium as the current carrier has as a consequence the accretion or stripping away of the anode with every charge–discharge cycle. While this poses challenges from the growth of protrusions (dendrites) to loss of contact, there lurks an opportunity: Morphogenesis at the anode–electrolyte interface layer can be studied, and may ultimately be controlled as a factor in solid state battery design. The accessible interface morphologies, the dynamic paths to them, and mechanisms to control them expand considerably if lithium alloys are introduced in the anode. The thermodynamics and kinetics of lithium intermetallics present principled approaches for morphogenic interface design. In this communication we adopt a computational approach to such an exploration. With phase field models that are parameterized by a combination of first principles atomistic calculations and experiments, we present phenomenological studies of two lithium intermetallics: Li–Mg and Li–Zn. An array of parametric investigations follows on the influence of kinetics, charge–discharge rate, cycling, transport mechanisms and grain structure. The emphasis across these computations is on the dynamic morphogenesis of the intermetallic interface. Specifically, the plating, segregation and smooth distribution of Li, Mg and Zn, the growth and disappearance of voids, evolution of solid electrolyte–anode contact area, and grain boundary structure are investigated. The computational platform is a framework for future studies of morphogenic electrolyte–anode interfaces with more extensive inputs from first principles atomistics and experiments.</div></div>","PeriodicalId":17331,"journal":{"name":"Journal of The Mechanics and Physics of Solids","volume":"200 ","pages":"Article 106073"},"PeriodicalIF":5.0000,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"A continuum, computational study of morphogenesis in lithium intermetallic interfaces in solid state batteries\",\"authors\":\"Mostafa Faghih Shojaei, Rahul Gulati, Krishna Garikipati\",\"doi\":\"10.1016/j.jmps.2025.106073\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The design of solid state batteries with lithium anodes is attracting attention for the prospect of high capacity and improved safety over liquid electrolyte systems. The nature of transport with lithium as the current carrier has as a consequence the accretion or stripping away of the anode with every charge–discharge cycle. While this poses challenges from the growth of protrusions (dendrites) to loss of contact, there lurks an opportunity: Morphogenesis at the anode–electrolyte interface layer can be studied, and may ultimately be controlled as a factor in solid state battery design. The accessible interface morphologies, the dynamic paths to them, and mechanisms to control them expand considerably if lithium alloys are introduced in the anode. The thermodynamics and kinetics of lithium intermetallics present principled approaches for morphogenic interface design. In this communication we adopt a computational approach to such an exploration. With phase field models that are parameterized by a combination of first principles atomistic calculations and experiments, we present phenomenological studies of two lithium intermetallics: Li–Mg and Li–Zn. An array of parametric investigations follows on the influence of kinetics, charge–discharge rate, cycling, transport mechanisms and grain structure. The emphasis across these computations is on the dynamic morphogenesis of the intermetallic interface. Specifically, the plating, segregation and smooth distribution of Li, Mg and Zn, the growth and disappearance of voids, evolution of solid electrolyte–anode contact area, and grain boundary structure are investigated. The computational platform is a framework for future studies of morphogenic electrolyte–anode interfaces with more extensive inputs from first principles atomistics and experiments.</div></div>\",\"PeriodicalId\":17331,\"journal\":{\"name\":\"Journal of The Mechanics and Physics of Solids\",\"volume\":\"200 \",\"pages\":\"Article 106073\"},\"PeriodicalIF\":5.0000,\"publicationDate\":\"2025-03-05\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of The Mechanics and Physics of Solids\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0022509625000493\",\"RegionNum\":2,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"MATERIALS SCIENCE, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of The Mechanics and Physics of Solids","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0022509625000493","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
A continuum, computational study of morphogenesis in lithium intermetallic interfaces in solid state batteries
The design of solid state batteries with lithium anodes is attracting attention for the prospect of high capacity and improved safety over liquid electrolyte systems. The nature of transport with lithium as the current carrier has as a consequence the accretion or stripping away of the anode with every charge–discharge cycle. While this poses challenges from the growth of protrusions (dendrites) to loss of contact, there lurks an opportunity: Morphogenesis at the anode–electrolyte interface layer can be studied, and may ultimately be controlled as a factor in solid state battery design. The accessible interface morphologies, the dynamic paths to them, and mechanisms to control them expand considerably if lithium alloys are introduced in the anode. The thermodynamics and kinetics of lithium intermetallics present principled approaches for morphogenic interface design. In this communication we adopt a computational approach to such an exploration. With phase field models that are parameterized by a combination of first principles atomistic calculations and experiments, we present phenomenological studies of two lithium intermetallics: Li–Mg and Li–Zn. An array of parametric investigations follows on the influence of kinetics, charge–discharge rate, cycling, transport mechanisms and grain structure. The emphasis across these computations is on the dynamic morphogenesis of the intermetallic interface. Specifically, the plating, segregation and smooth distribution of Li, Mg and Zn, the growth and disappearance of voids, evolution of solid electrolyte–anode contact area, and grain boundary structure are investigated. The computational platform is a framework for future studies of morphogenic electrolyte–anode interfaces with more extensive inputs from first principles atomistics and experiments.
期刊介绍:
The aim of Journal of The Mechanics and Physics of Solids is to publish research of the highest quality and of lasting significance on the mechanics of solids. The scope is broad, from fundamental concepts in mechanics to the analysis of novel phenomena and applications. Solids are interpreted broadly to include both hard and soft materials as well as natural and synthetic structures. The approach can be theoretical, experimental or computational.This research activity sits within engineering science and the allied areas of applied mathematics, materials science, bio-mechanics, applied physics, and geophysics.
The Journal was founded in 1952 by Rodney Hill, who was its Editor-in-Chief until 1968. The topics of interest to the Journal evolve with developments in the subject but its basic ethos remains the same: to publish research of the highest quality relating to the mechanics of solids. Thus, emphasis is placed on the development of fundamental concepts of mechanics and novel applications of these concepts based on theoretical, experimental or computational approaches, drawing upon the various branches of engineering science and the allied areas within applied mathematics, materials science, structural engineering, applied physics, and geophysics.
The main purpose of the Journal is to foster scientific understanding of the processes of deformation and mechanical failure of all solid materials, both technological and natural, and the connections between these processes and their underlying physical mechanisms. In this sense, the content of the Journal should reflect the current state of the discipline in analysis, experimental observation, and numerical simulation. In the interest of achieving this goal, authors are encouraged to consider the significance of their contributions for the field of mechanics and the implications of their results, in addition to describing the details of their work.