SEI/dead Li-turning capacity loss for high-performance anode-free solid-state lithium batteries  

作　　者：Qianwen Yin Tianyu Li Hongzhang Zhang Guiming Zhong Xiaofei Yang Xianfeng Li 

机构地区：[1]Division of Energy Storage,Dalian National Laboratory for Clean Energy,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,Liaoning,China [2]University of Chinese Academy of Sciences,Beijing 100049,China [3]Key Laboratory of Long-Duration and Large-Scale Energy Storage,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,Liaoning,China [4]Laboratory of Advanced Spectro-Electrochemistry and Lithium-Ion Batteries,Dalian National Laboratory for Clean Energy,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,Liaoning,China

出　　处：《Journal of Energy Chemistry》2024年第9期145-152,共8页能源化学（英文版）

基　　金：supported by the CAS Project of Young Scientists in Basic Research(YSBR-058);the National Natural Science Foundation of China(22279135);the Outstanding Youth Foundation of Liaoning Province(2023JH3/10200019);the Dalian Science and Technology Innovation Fund(2023JJ11CG004);the Energy Revolution S&T Program of Yulin Innovation Institute of Clean Energy(YIICE E411010316)。

摘　　要：Anode-free solid-state lithium metal batteries(AF-SSLBs)have the potential to deliver higher energy density and improved safety beyond lithium-metal batteries.However,the unclear mechanism for the fast capacity decay in AF-SSLBs,either determined by dead Li or solid electrolyte interface(SEI),limits the proposal of effective strategies to prolong cycling life.To clarify the underlying mechanism,herein,the evolution of SEI and dead Li is quantitatively analyzed by a solid-state nuclear magnetic resonance(ss-NMR)technology in a typical LiPF6-based polymer electrolyte.The results show that the initial capacity loss is attributed to the formation of SEI,while the dead Li dominates the following capacity loss and the growth rate is 0.141 mA h cm^(−2)cycle−1.To reduce the active Li loss,the combination of inorganic-rich SEI and self-healing electrostatic shield effect is proposed to improve the reversibility of Li deposition/dissolution behavior,which reduces the capacity loss rate for the initial SEI and following dead Li generation by 2.3 and 20.1 folds,respectively.As a result,the initial Coulombic efficiency(ICE)and stable CE increase by 15.1%and 15.3%in Li-Cu cells,which guides the rational design of high-performance AF-SSLBs.

关 键 词：Solid-state lithium batteries Solid-state NMR Anode-free SEI Dead Li 

分 类 号：TM912[电气工程—电力电子与电力传动] O646[理学—物理化学]