An efficient Hauser-base electrolyte for rechargeable magnesium batteries  

作　　者：Mingxiang Cheng Yaru Wang Duo Zhang Shuxin Zhang Yang Yang Xuecheng Lv Jiulin Wang Yanna NuLi 

机构地区：[1]School of Chemistry and Chemical Engineering,Shanghai Electrochemical Energy Devices Research Center,Shanghai Jiao Tong University,Shanghai 200240,China [2]School of Energy and Power Engineering,Dalian University of Technology,Dalian 116024,Liaoning,China

出　　处：《Journal of Energy Chemistry》2023年第1期1-10,I0001,共11页能源化学（英文版）

基　　金：financial support from the National Natural Science Foundation of China(Nos.21975159,2157316);the Shanghai Aerospace Science and Technology Innovation Fund(No.SAST2018-117);the Oceanic Interdisciplinary Program of Shanghai Jiao Tong University(No.WH410260401/006)。

摘　　要：Rechargeable magnesium batteries(RMBs)are considered the promising candidates for post lithium-ion batteries due to the abundant storage,high capacity,and dendrite-rare characteristic of Mg anode.However,the lack of practical electrolytes impedes the development and application of RMBs.Here,through a one-step reaction of LiCl congenital-containing Knochel–Hauser base TMPL(2,2,6,6-tetrame thylpiperidinylmagnesium chloride lithium chloride complex)with Lewis acid AlCl_(3),we successfully synthesized an efficient amino-magnesium halide TMPLA electrolyte.Raman and mass spectroscopy identified that the electrolyte comprises the typical di-nuclear copolymer[Mg_(2)Cl_(3)·6THF]+cation group and[(TMP)2AlCl_(2)]-anion group,further supported by the results of density functional theory calculations(DFT)and the Molecular dynamics(MD)simulations.The TMPLA electrolyte exhibits promising electrochemical performance,including available anodic stability(>2.65 V vs.SS),high ionic conductivity(6.05mS cm^(-1)),and low overpotential(<0.1 V)as well as appropriate Coulombic efficiency(97.3%)for Mg plating/stripping.Both the insertion Mo6S8cathode and conversion Cu S cathode delivered a desirable electrochemical performance with high capacity and good cycling stability based on the TMPLA electrolyte.In particular,when compatible with low cost and easily synthesized Cu S,the Cu S||Mg cell displayed an extremely high discharge capacity of 458.8 mAh g^(-1)for the first cycle and stabilized at 170.2 mAh g^(-1)with high Coulombic efficiency(99.1%)after 50 cycles at 0.05 C.Our work proposes an efficient electrolyte with impressive compatibility with Mg anode and insertion/conversion cathode for practical RMBs and provides a more profound knowledge of the Lewis acid–base reaction mechanisms.

关 键 词：Rechargeable magnesium batteries Mg-Li dual-salt electrolyte Hauser-base In-situ synthesis Lewis acid–base reaction CuS cathode 

分 类 号：TM912[电气工程—电力电子与电力传动]