DataVXACS Energy LettersPaper
journal article·2020-01-10Open access

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

Hui Wang, Xuefei Feng, Ying Chen, Yi-Sheng Liu, Kee Sung Han, Mingxia Zhou, Mark H. Engelhard, Vijayakumar Murugesan, Rajeev S. Assary, Tianbiao Leo Liu, Wesley Henderson, Zimin Nie, Meng Gu, Jie Xiao, Chongmin Wang, Kristin Persson, Donghai Mei, Ji-Guang Zhang, Karl T. Mueller, Jinghua Guo, Kevin Zavadil, Yuyan Shao, Jun Liu

ACS Energy Letters· Volume 5· Issue 1
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Source abstract

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 X-ray absorption spectroscopy (XAS), nuclear magnetic resonance (NMR), and density functional theory (DFT) calculations.
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Research context

Energy storage

OpenAlex topics: Advancements in Battery Materials · Advanced Battery Materials and Technologies · Supercapacitor Materials and Fabrication

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Energy & Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99352, United States

Joint Center for Energy Storage Research (JCESR), Lemont Illinois 60439, United States

Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States

Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99352, United States

Materials Science Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, United States

Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99352, United States

Energy Technologies Area, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States

Department of Materials Science and Engineering, University of California, Berkeley, Berkeley, California 94720, United States

Material, Physical, and Chemical Sciences, Sandia National Laboratories, Albuquerque, New Mexico 87185, United States

Funding

Basic Energy Sciences

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