Enhancing Li cycling coulombic efficiency while mitigating “shuttle effect” of Li-S battery through sustained release of LiNO_(3)

作     者：Qi Jin Kaixin Zhao Lili Wu Lu Li Long Kong Xitian Zhang Qi Jin;Kaixin Zhao;Lili Wu;Lu Li;Long Kong;Xitian Zhang

作者机构：Key Laboratory for Photonic and Electronic Bandgap MaterialsMinistry of EducationSchool of Physics and Electronic EngineeringHarbin Normal UniversityHarbin 150025HeilongjiangChina Frontiers Science Center for Flexible Electronics and Xi’an Institute of Flexible Electronics(IFE)Northwestern Polytechnical UniversityXi’an 710129ShaanxiChina 

出 版 物：《Journal of Energy Chemistry》 (能源化学（英文版）)

年 卷 期：2023年第84卷第9期

页      面：22-29页

核心收录：

学科分类：081702[工学-化学工艺] 0808[工学-电气工程] 0809[工学-电子科学与技术（可授工学、理学学位）] 08[工学] 0817[工学-化学工程与技术] 0805[工学-材料科学与工程（可授工学、理学学位）] 0703[理学-化学] 

基　　金：partially supported by grants from the National Natural Science Foundation of China (52072099, 52102228) Team program of the Natural Science Foundation of Heilongjiang Province, China (TD2021E005) The National general entrepreneurial practice program (202210231088S) The National general innovation training program (202210231076)。 

主　　题：Lithium-sulfur battery Solid electrolyte interphase LiNO_(3) Coulombic efficiency Shuttle effect 

摘      要：In practical lithium-sulfur batteries(LSBs),the shuttle effect and Li cycling coulombic efficiency(CE) are strongly affected by the physicochemical properties of solid electrolyte interphase(SEI).LiNO_(3) is widely used as an additive in electrolytes to build a high-quality SEI,but its self-sacrificial nature limits the ability to mitigate the shuttle effect and stabilize Li anode during long-term cycling.To counteract LiNO_(3) consumption during long-term cycling without using a high initial concentration,inspired by sustainedrelease drugs,we encapsulated LiNO_(3) in lithiated Nafion polymer and added an electrolyte co-solvent(1,1,2,2-tetrafluoroethylene 2,2,2-trifluoromethyl ether) with poor LiNO_(3) solubility to construct highquality and durable F-and N-rich SEI.Theoretical calculations,experiments,multiphysics simulations,and in-situ observations confirmed that the F-and N-rich SEI can modulate lithium deposition behavior and allow persistent repair of SEI during prolonged cycling.Hence,the F-and N-rich SEI improves the Li anode cycling CE to 99.63% and alleviates the shuttle effect during long-term cycling.The lithium anode with sustainable F-and N-rich SEI shows a stable Li plating/stripping over 2000 h at 1 mA cm^(-2).As expected,Li‖S full cells with this SEI achieved a long lifespan of 250 cycles,far exceeding cells with a routine SEI.The Li‖S pouch cell based on F-and N-rich SEI also can achieve a high energy density of about300 Wh kg^(-1) at initial cycles.This strategy provides a novel design for high-quality and durable SEls in LSBs and may also be extendable to other alkali metal batteries.