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作者机构:Hunan Univ Coll Mat Sci & Engn Hunan Joint Int Lab Adv Mat & Technol Clean Energ Hunan Prov Key Lab Adv Carbon Mat & Appl Technol Changsha 410082 Peoples R China Wuhan Univ Technol Int Sch Mat Sci & Engn State Key Lab Silicate Mat Architectures Wuhan 430070 Hubei Peoples R China Tsinghua Shenzhen Int Grad Sch SIGS Shenzhen Key Lab Power Battery Safety Shenzhen 518055 Peoples R China Tsinghua Shenzhen Int Grad Sch SIGS Shenzhen Geim Graphene Ctr Shenzhen 518055 Peoples R China Chinese Acad Sci Inst Met Res Shenyang Natl Lab Mat Sci 72 Wenhua Rd Shenyang 110016 Peoples R China Hunan Agr Univ Sch Chem & Mat Sci Changsha 410128 Peoples R China Natl Univ Def Technol Coll Aerosp Sci & Engn Changsha 410073 Peoples R China Univ Macau Inst Appl Phys & Mat Engn Joint Key Lab Minist Educ Ave Univ Taipa 999078 Macau Peoples R China Tsinghua Univ Inst Nucl & New Energy Technol Beijing 100084 Peoples R China South China Normal Univ Key Lab ETESPG GHEI Engn Res Ctr MTEES Minist EducRes Ctr BMET Guangdong ProvEngn Lab Guangzhou 510006 Peoples R China South China Normal Univ Innovat Platform ITBMD Guangzhou Municipal Sch Chem Guangzhou 510006 Peoples R China
出 版 物:《ADVANCED ENERGY MATERIALS》 (激光物理学评论)
年 卷 期:2022年第12卷第33期
页 面:2201631-2201631页
核心收录:
学科分类:0820[工学-石油与天然气工程] 070207[理学-光学] 07[理学] 08[工学] 0805[工学-材料科学与工程(可授工学、理学学位)] 0703[理学-化学] 0803[工学-光学工程] 0702[理学-物理学]
基 金:National Natural Science Foundation of China [U21A2081, 22075074] Outstanding Young Scientists Research Funds from Hunan Province [2020JJ2004] Major Science and Technology Program of Hunan Province [2020WK2013]
主 题:cathode electrolyte interphases dynamic evolution electrolyte additives high temperatures in situ FTIR unsaturation
摘 要:High-energy lithium-ion batteries (LIBs) can be realized with the use of nickel-rich materials, however, their reversible operation requires long-term cathode-electrolyte interfacial (CEI) stability, especially for high-temperature applications, but how the CEIs evolves during operation is still a mystery. The unstable CEIs have been recently ascribed to them generating/disappearing/regenerating during Li+ extraction/insertion by in situ Fourier Transform Infrared Spectroscopy spectrum. Herein, a strategy of insoluble CEI is proposed toward addressing the interfacially induced deterioration of cathodes with a focus on Ni-rich layered oxides. Incorporating unsaturated units (C=C/C C) to siloxane as electrolyte additives advances the commercial LiNi0.3Co0.1Mn0.1O2/graphite cells up to around 300 cycles at 60 degrees C with more than 85% capacity retention, along with the LiCoO2 cells reaching similar to 90% capacity retention over 350 cycles under 80 degrees C. The experimentally and theoretically detailed investigation shows that the higher unsaturation bond with high reactive sites show more polymerization via a 3D topological pathway to form insoluble CEI species, leading to suppression of parasitic reactions, corrosive acid, transition-metal dissolution, stress corrosive cracking, and impedance growth. The scientific discoveries of this study highlight the pivotal role of electrode-electrolyte interactions and recapitulates the tried-and-true electrolyte approach for the future development of high-energy batteries under extreme temperature conditions.