Engineering an Insoluble Cathode Electrolyte Interphase Enabling High Performance NCM811//Graphite Pouch Cell at 60 °C

作     者：Chen, Yuqing He, Qiu Mo, Ying Zhou, Wang Zhao, Yun Piao, Nan Liu, Chi Xiao, Peitao Liu, Hui Li, Baohua Chen, Shi Wang, Li He, Xiangming Xing, Lidan Liu, Jilei 

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.