@article{32303, author = {Hui Wang and Xuefei Feng and Ying Chen and Yi-Sheng Liu and Kee Sung Han and Mingxia Zhou and Mark H Engelhard and Vijayakumar Murugesan and Rajeev S Assary and Tianbiao Leo Liu and Wesley Henderson and Zimin Nie and Meng Gu and Jie Xiao and Chongmin Wang and Kristin A Persson and Donghai Mei and Ji-Guang Zhang and Karl T Mueller and Jinghua Guo and Kevin Zavadil and Yuyan Shao and Jun Liu}, title = {Reversible Electrochemical Interface of Mg Metal and Conventional Electrolyte Enabled by Intermediate Adsorption}, abstract = {

Conventional electrolytes made by mixing simple Mg2+ salts and aprotic solvents, analogous to those in Li-ion batteries, are incompatible with Mg anodes because Mg metal readily reacts with such electrolytes, producing a passivation layer that blocks Mg2+ transport. Here, we report that, through tuning a conventional electrolyteMg(TFSI)2 (TFSI− is N(SO2CF3)2 −)with an Mg(BH4)2 cosalt, highly reversible Mg plating/stripping with a high Coulombic efficiency is achieved by neutralizing the first solvation shell of Mg cationic clusters between Mg2+ and TFSI− and enhanced reductive stability of free TFSI−. A critical adsorption step between Mg0 atoms and active Mg cation clusters involving BH4 − anions is identified to be the key enabler for reversible Mg plating/stripping through analysis of the distribution of relaxation times (DRT) from operando electrochemical impedance spectroscopy (EIS), operando electrochemical Xray absorption spectroscopy (XAS), nuclear magnetic resonance (NMR), and density functional theory (DFT) calculations

}, year = {2020}, journal = {ACS Energy Letters}, volume = {5}, pages = {200 - 206}, month = {12/2019}, issn = {2380-8195}, doi = {10.1021/acsenergylett.9b02211}, language = {eng}, }