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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) (TEST- 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 MI-. A critical adsorption step between Mg-0 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.

Authors:
; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Science - Office of Basic Energy Sciences - Joint Center for Energy Storage Research (JCESR)
OSTI Identifier:
1595940
DOE Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 5; Journal Issue: 1
Country of Publication:
United States
Language:
English

Citation Formats

Wang, Hui, Feng, Xuefie, Chen, Ying, Liu, Yi-Sheng, Han, Kee Sung, Zhou, Mingxia, Engelhard, Mark H., Murugesan, Vijayakumar, Assary, Rajeev S., and Liu, Tianbiao Leo. Reversible electrochemical interface of Mg metal and conventional electrolyte enabled by intermediate adsorption. United States: N. p., 2020. Web. doi:10.1021/acsenergylett.9b02211.
Wang, Hui, Feng, Xuefie, Chen, Ying, Liu, Yi-Sheng, Han, Kee Sung, Zhou, Mingxia, Engelhard, Mark H., Murugesan, Vijayakumar, Assary, Rajeev S., & Liu, Tianbiao Leo. Reversible electrochemical interface of Mg metal and conventional electrolyte enabled by intermediate adsorption. United States. doi:10.1021/acsenergylett.9b02211.
Wang, Hui, Feng, Xuefie, Chen, Ying, Liu, Yi-Sheng, Han, Kee Sung, Zhou, Mingxia, Engelhard, Mark H., Murugesan, Vijayakumar, Assary, Rajeev S., and Liu, Tianbiao Leo. Wed . "Reversible electrochemical interface of Mg metal and conventional electrolyte enabled by intermediate adsorption". United States. doi:10.1021/acsenergylett.9b02211.
@article{osti_1595940,
title = {Reversible electrochemical interface of Mg metal and conventional electrolyte enabled by intermediate adsorption},
author = {Wang, Hui and Feng, Xuefie and Chen, Ying and Liu, Yi-Sheng and Han, Kee Sung and Zhou, Mingxia and Engelhard, Mark H. and Murugesan, Vijayakumar and Assary, Rajeev S. and Liu, Tianbiao Leo},
abstractNote = {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) (TEST- 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 MI-. A critical adsorption step between Mg-0 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.},
doi = {10.1021/acsenergylett.9b02211},
journal = {ACS Energy Letters},
number = 1,
volume = 5,
place = {United States},
year = {2020},
month = {1}
}