Enabling an Inorganic-Rich Interface via Cationic Surfactant for High-Performance Lithium Metal BatteriesOACSTPCDEI
Enabling an Inorganic-Rich Interface via Cationic Surfactant for High-Performance Lithium Metal Batteries
An anion-rich elec-tric double layer(EDL)region is favorable for fabricating an inor-ganic-rich solid-electrolyte inter-phase(SEI)towards stable lithium metal anode in ester electrolyte.Herein,cetyltrimethylammonium bromide(CTAB),a cationic sur-factant,is adopted to draw more ani-ons into EDL by ionic interactions that shield the repelling force on anions during lithium plating.In situ electrochemical surface-enhanced Raman spectroscopy results combined with molecular dynamics simulations validate the enrichment of NO3-/FSI-anions in the EDL region due to the positively charged CTA+.In-depth analysis of SEI structure by X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry results confirmed the formation of the inorganic-rich SEI,which helps improve the kinetics of Li+transfer,lower the charge transfer activation energy,and homogenize Li deposition.As a result,the Li‖Li symmetric cell in the designed electrolyte displays a prolongated cycling time from 500 to 1300 h compared to that in the blank electrolyte at 0.5 mA cm-2 with a capacity of 1 mAh cm-2.Moreover,Li‖LiFePO4 and Li‖LiCoO2 with a high cathode mass loading of＞10 mg cm-2 can be stably cycled over 180 cycles.
Zejun Sun;Yu Long;Meng Wang;Jingyu Mao;Haotian Yang;Baihua Cui;Yukun Xiao;Ganwen Chen;Qi Zhang;Zhenxiang Xing;Jisheng Pan;Jinlin Yang;Gang Wu;Wei Chen;Hongfei Xu;Chonglai Jiang;Yuxiang Niu;Xu Lian;Yuan Liu;Ruiqi Su;Dayu Liu
Department of Chemistry,National University of Singapore,3 Science Drive 3,Singapore 117543,SingaporeDepartment of Chemistry,National University of Singapore,3 Science Drive 3,Singapore 117543,Singapore||Joint School of National University of Singapore and Tianjin University,International Campus of Tianjin University,Binhai New City,Fuzhou 350207,People's Republic of ChinaDepartment of Physics,National University of Singapore,2 Science Drive 3,Singapore 117542,SingaporeAgency for Science,Technology,and Research(A*STAR),Institute of Materials Research and Engineering,Innovis,2 Fusionopolis Way,#08-03,Singapore 138634,SingaporeAgency for Science,Technology and Research(A*STAR),Institute of High-Performance Computing,1 Fusionopolis Way,#16-16 Connexis,Singapore 138632,SingaporeDepartment of Chemistry,National University of Singapore,3 Science Drive 3,Singapore 117543,Singapore||Department of Physics,National University of Singapore,2 Science Drive 3,Singapore 117542,Singapore||Joint School of National University of Singapore and Tianjin University,International Campus of Tianjin University,Binhai New City,Fuzhou 350207,People's Republic of China
Cationic surfactantLithium nitrate additiveSolid-electrolyte interphaseElectric double layerLithium metal batteries
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The authors acknowledge the financial support from Singapore Ministry of Education under its AcRF Tier 2 Grant No MOE-T2EP10123-0001,Singapore National Research Foundation Investigatorship under Grant No NRF-NRFI08-2022-0009,and Academic Excellence Foundation of BUAA for PhD Students(applicant:Hongfei Xu).
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