Reversible Electrochemical Interface of Mg Metal and Conventional Electrolyte Enabled by Intermediate Adsorption

Autor: Wang, H, Feng, X, Chen, Y, Liu, YS, Han, KS, Zhou, M, Engelhard, MH, Murugesan, V, Assary, RS, Liu, TL, Henderson, W, Nie, Z, Gu, M, Xiao, J, Wang, C, Persson, K, Mei, D, Zhang, JG, Mueller, KT, Guo, J, Zavadil, K, Shao, Y, Liu, J
Rok vydání: 2020
Zdroj: ACS Energy Letters, vol 5, iss 1
Popis: 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 X-ray absorption spectroscopy (XAS), nuclear magnetic resonance (NMR), and density functional theory (DFT) calculations.
Databáze: OpenAIRE