Identifying Hidden Li–Si–O Phases for Lithium-Ion Batteries via First-Principle Thermodynamic Calculations

作     者：Jiale Qu Chao Ning Xiang Feng Bonan Yao Bo Liu Ziheng Lu Tianshuai Wang Zhi Wei Seh Siqi Shi Qianfan Zhang Jiale Qu;Chao Ning;Xiang Feng;Bonan Yao;Bo Liu;Ziheng Lu;Tianshuai Wang;Zhi Wei Seh;Siqi Shi;Qianfan Zhang

作者机构：School of Materials Science and EngineeringBeihang UniversityBeijing 100191China College of Mathematics and PhysicsJinggangshan UniversityJi’an 343009China Department of Materials Science&MetallurgyUniversity of CambridgeCambridge CB30FSUK Institute of Materials Research and EngineeringAgency for ScienceTechnology and Research(A^(*)STAR)Singapore 138634Singapore School of Materials Science and EngineeringShanghai UniversityShanghai 200444China 

出 版 物：《Energy & Environmental Materials》 (能源与环境材料（英文）)

年 卷 期：2022年第5卷第3期

页      面：865-871页

核心收录：

学科分类：0808[工学-电气工程] 08[工学] 0805[工学-材料科学与工程（可授工学、理学学位）] 

基　　金：supported by the Beijing Natural Science Foundation(2192029) the National Key Research and Development Program of China(2017YFB0702100) the National Natural Science Foundation of China(11404017,12004145) the Technology Foundation for Selected Overseas Chinese Scholars the Ministry of Human Resources and Social Security of China supported by the Academic Excellence Foundation of BUAA for PhD Students supported by the Faraday Institution(grant number FIRG017) supported by the Singapore National Research Foundation(NRF-NRFF2017-04) supported by Jiangxi Provincial Natural Science Foundation(20212BAB214032) 

主　　题：anode material crystal structure prediction first-principle calculations ternary alloy phase 

摘      要：SiO–based materials are promising alloys and conversion-type anode materials for lithium-ion batteries and are recently found to be excellent dendrite-proof layers for lithium-metal ***,only a small fraction of the Li–Si–O compositional space has been reported,significantly impeding the understanding of the phase transition mechanisms and the rational design of these materials both as anodes and as protection layers for lithium-metal ***,we identify three new thermodynamically stable phases within the Li–Si–O ternary system(Li_(2)SiO_(5),Li_(4)SiO_(6),and Li_(4)SiO_(8))in addition to the existing records via first-principle *** electronic structure simulation shows that Li_(2)SiO_(5)and Li_(4)SiO_(8)phases are metallic in nature,ensuring high electronic conductivity required as *** calculations demonstrate that the mechanical strength of Li–Si–O phases is much higher than that of lithium *** diffusion barriers of interstitial Li range from 0.1 to 0.6 eV and the interstitial Li hopping serves as the dominating diffusion mechanism in the Li–Si–O ternary systems compared with vacancy *** findings provide a new strategy for future discovery of improved alloying anodes for lithium-ion batteries and offer important insight towards the understanding of the phase transformation mechanism of alloy-type protection layers on lithium-metal anodes.