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Modeling of Electron-Transfer Kinetics in Magnesium Electrolytes: Influence of the Solvent on the Battery Performance

Drews, Janina and Jankowski, Piotr and Häcker, Joachim and Li, Zhenyou and Danner, Timo and García Lastra, Juan Maria and Vegge, Tejs and Wagner, Norbert and Friedrich, Kaspar Andreas and Zhao-Karger, Zhirong and Fichtner, Maximilian and Latz, Arnulf (2021) Modeling of Electron-Transfer Kinetics in Magnesium Electrolytes: Influence of the Solvent on the Battery Performance. ChemSusChem. Wiley. doi: 10.1002/cssc.202101498. ISSN 1864-5631.

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Official URL: https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cssc.202101498

Abstract

The performance of rechargeable magnesium batteries is strongly dependent on the choice of electrolyte. The desolvation of multivalent cations usually goes along with high energy barriers, which can have a crucial im- pact on the plating reaction. This can lead to significantly higher overpotentials for magnesium deposition compared to magnesium dissolution. In this work we combine experimental measurements with DFT calcula- tions and continuum modelling to analyze Mg deposition in various solvents. Jointly, these methods provide a better understanding of the electrode reactions and especially the magnesium deposition mechanism. Thereby, a kinetic model for electrochemical reactions at metal electrodes is developed, which explicitly couples desolva- tion to electron transfer and, furthermore, qualitatively takes into account effects of the electrochemical double layer. The influence of different solvents on the battery performance is studied for the state-of-the-art magne- sium tetrakis(hexafluoroisopropyloxy)borate electrolyte salt. It becomes apparent that not necessarily a whole solvent molecule must be stripped from the solvated magnesium cation before the first reduction step can take place. For Mg reduction it seems to be sufficient to have one coordination site available, so that the magnesium cation is able to get closer to the electrode surface. Thereby, the initial desolvation of the magnesium cation determines the deposition reaction for mono-, tri- and tetraglyme, whereas the influence of the desolvation on the plating reaction is minor for diglyme and tetrahydrofuran. Overall, we can give a clear recommendation for diglyme to be applied as solvent in magnesium electrolytes.

Item URL in elib:https://elib.dlr.de/143907/
Document Type:Article
Title:Modeling of Electron-Transfer Kinetics in Magnesium Electrolytes: Influence of the Solvent on the Battery Performance
Authors:
AuthorsInstitution or Email of AuthorsAuthor's ORCID iD
Drews, Janinajanina.drews (at) dlr.dehttps://orcid.org/0000-0002-9800-6421
Jankowski, PiotrTechnical University of Denmark (DTU)https://orcid.org/0000-0003-0178-8955
Häcker, JoachimJoachim.Haecker (at) dlr.dehttps://orcid.org/0000-0003-2031-9898
Li, ZhenyouKarlsruhe Institute of Technology (KIT)https://orcid.org/0000-0001-9624-2124
Danner, TimoTimo.Danner (at) dlr.dehttps://orcid.org/0000-0003-2336-6059
García Lastra, Juan MariaTechnical University of Denmark (DTU)https://orcid.org/0000-0001-5311-3656
Vegge, TejsTechnical University of Denmark (DTU)https://orcid.org/0000-0002-1484-0284
Wagner, NorbertNorbert.Wagner (at) dlr.dehttps://orcid.org/0000-0002-2596-8689
Friedrich, Kaspar AndreasAndreas.Friedrich (at) dlr.dehttps://orcid.org/0000-0002-2968-5029
Zhao-Karger, ZhirongKarlsruhe Institute of Technology (KIT)https://orcid.org/0000-0002-7233-9818
Fichtner, MaximilianKarlsruhe Institute of Technology (KIT)https://orcid.org/0000-0002-7127-1823
Latz, Arnulfarnulf.latz (at) dlr.dehttps://orcid.org/0000-0003-1449-8172
Date:30 August 2021
Journal or Publication Title:ChemSusChem
Refereed publication:Yes
Open Access:Yes
Gold Open Access:No
In SCOPUS:Yes
In ISI Web of Science:Yes
DOI :10.1002/cssc.202101498
Publisher:Wiley
ISSN:1864-5631
Status:Published
Keywords:Computational electrochemistry Deposition mechanism Desolvation Electron-transfer kinetics Rechargeable magnesium batteries
HGF - Research field:Energy
HGF - Program:Materials and Technologies for the Energy Transition
HGF - Program Themes:Electrochemical Energy Storage
DLR - Research area:Energy
DLR - Program:E SP - Energy Storage
DLR - Research theme (Project):E - Electrochemical Storage
Location: Stuttgart
Institutes and Institutions:Institute of Engineering Thermodynamics > Computational Electrochemistry
Institute of Engineering Thermodynamics > Electrochemical Energy Technology
Deposited By: Drews, Janina
Deposited On:29 Oct 2021 11:13
Last Modified:24 May 2022 23:47

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