Tackling application limitations of high-safetyγ-butyrolactone electrolytes:Exploring mechanisms and proposing solutions  

作　　者：Haojun Wu Zhangyating Xie Guanjie Li Lei Zheng Zhiwei Zhao Jiarong He Yanbin Shen Jiahao Hu Zhangquan Peng Guiming Zhong Lidan Xing Weishan Li 

机构地区：[1]School of Chemistry,South China Normal University,Guangzhou 510006,Guangdong,China [2]National and Local Joint Engineering Research Center of MPTES in High Energy and Safety LIBs,Engineering Research Center of MTEES(Ministry of Education),Research Center of BMET(Guangdong Province),and Key Lab.of ETESPG(GHEI),South China Normal University,Guangzhou 510006,Guangdong,China [3]Laboratory of Advanced Spectroelectrochemistry and Li-ion Batteries,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,Liaoning,China [4]i-Lab,CAS Center for Excellence in Nanoscience,Suzhou Institute of Nano-Tech and Nano-Bionics(SINANO),Chinese Academy of Sciences,Suzhou 215123,Jiangsu,China [5]School of Chemical Engineering,Faculty of Sciences,Engineering and Technology,The University of Adelaide,SA 5005,Australia

出　　处：《Journal of Energy Chemistry》2024年第6期193-201,I0005,共10页能源化学（英文版）

基　　金：financially supported by the National Natural Science Foundation of China(21972049,22272175);the National Key R&D Program of China(2022YFA1504002);the“Scientist Studio Funding”from Tianmu Lake Institute of Advanced Energy Storage Technologies Co.,Ltd.;Dalian Supports High-Level Talent Innovation and Entrepreneurship Projects(2021RD14);the Dalian Institute of Chemical Physics(DICP I202213);the 21C Innovation Laboratory,Contemporary Ampere Technology Ltd.by project No.21C-OP-202208。

摘　　要：Developing wide-temperature and high-safety lithium-ion batteries(LIBs)presents significant challenges attributed to the absence of suitable solvents possessing broad liquid range and non-flammability properties.γ-Butyrolactone(GBL)has emerged as a promising solvent;however,its incompatibility with graphite anode has hindered its application.This limitation necessitates a comprehensive investigation into the underlying mechanisms and potential solutions.In this study,we achieve a molecular-level understanding of the perplexing interphase formation process by employing in-situ spectroelectrochemical techniques and density function calculations.Our findings reveal that,even at high salt concentrations,GBL consistently occupies the primary Li^(+)solvation sheath,leading to extensive GBL decomposition and the formation of a high-impedance and inorganic-poor solid-electrolyte interphase(SEI)layer.Contrary to manipulating solvation structures,our research demonstrates that the utilization of filmforming additives with higher reduction potential facilitates the pre-establishment of a robust SEI film on the graphite anode.This approach effectively inhibits GBL decomposition and significantly enhances the battery's lifespan.This study provides the first reported intrinsic understanding of the unique GBLgraphite incompatibility and offers valuable insights for the development of wide-temperature and high-safety LIBs.

关 键 词：γ-Butyrolactone/Graphite incompatibility Unique solvation structure SEI film Lithium-ion batteries 

分 类 号：O646.1[理学—物理化学] TM912[理学—化学]