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3. A practical perspective on the potential of rechargeable Mg batteries

Author

European Commission, Agencia Estatal de Investigación (España), Blázquez, J. Alberto [0000-0003-3391-9788], Leonet, Olatz [0000-0002-4108-5886], Mukherjee, Ayan [0000-0001-7878-3787], Zhao-Karger, Zhirong [0000-0002-7233-9818], Li, Zhenyou [0000-0001-9624-2124], Fernández-Barquín, Ana [0000-0003-4035-4164], Mainar, Aroa R. [0000-0003-3400-5160], Jankowski, Piotr [0000-0003-0178-8955], Dutton, Siân E. [0000-0003-0984-5504], Grey, Clare P. [0000-0001-5572-192X], Drews, Janina [0000-0002-9800-6421], Häcker, Joachim [0000-0003-2031-9898], Danner, Timo [0000-0003-2336-6059], Latz, Arnulf [0000-0003-1449-8172], Sotta, Dane [0000-0002-6119-7113], Palacín, M. Rosa [0000-0001-7351-2005], Lastra, Juan Maria García [0000-0001-5311-3656], Fichtner, Maximilian [0000-0002-7127-1823], Kundu, Sumana [0000-0003-0621-8644], Noked, Malachi [0000-0001-8995-0632], Aurbach, Doron [0000-0002-6382-0888], Blázquez, J. Alberto, Maça, Rudi R., Leonet, Olatz, Azaceta, Eneko, Mukherjee, Ayan, Zhao-Karger, Zhirong, Li, Zhenyou, Kovalevsky, Aleksey, Fernández-Barquín, Ana, Mainar, Aroa R., Jankowski, Piotr, Rademacher, Laurin, Dey, Sunita, Dutton, Siân E., Grey, Clare P., Drews, Janina, Häcker, Joachim, Danner, Timo, Latz, Arnulf, Sotta, Dane, Palacín, M. Rosa, Martin, Jean Frédéric, Lastra, Juan Maria García, Fichtner, Maximilian, Kundu, Sumana, Kraytsberg, Alexander, Ein-Eli, Yair, Noked, Malachi, Aurbach, Doron, European Commission, Agencia Estatal de Investigación (España), Blázquez, J. Alberto [0000-0003-3391-9788], Leonet, Olatz [0000-0002-4108-5886], Mukherjee, Ayan [0000-0001-7878-3787], Zhao-Karger, Zhirong [0000-0002-7233-9818], Li, Zhenyou [0000-0001-9624-2124], Fernández-Barquín, Ana [0000-0003-4035-4164], Mainar, Aroa R. [0000-0003-3400-5160], Jankowski, Piotr [0000-0003-0178-8955], Dutton, Siân E. [0000-0003-0984-5504], Grey, Clare P. [0000-0001-5572-192X], Drews, Janina [0000-0002-9800-6421], Häcker, Joachim [0000-0003-2031-9898], Danner, Timo [0000-0003-2336-6059], Latz, Arnulf [0000-0003-1449-8172], Sotta, Dane [0000-0002-6119-7113], Palacín, M. Rosa [0000-0001-7351-2005], Lastra, Juan Maria García [0000-0001-5311-3656], Fichtner, Maximilian [0000-0002-7127-1823], Kundu, Sumana [0000-0003-0621-8644], Noked, Malachi [0000-0001-8995-0632], Aurbach, Doron [0000-0002-6382-0888], Blázquez, J. Alberto, Maça, Rudi R., Leonet, Olatz, Azaceta, Eneko, Mukherjee, Ayan, Zhao-Karger, Zhirong, Li, Zhenyou, Kovalevsky, Aleksey, Fernández-Barquín, Ana, Mainar, Aroa R., Jankowski, Piotr, Rademacher, Laurin, Dey, Sunita, Dutton, Siân E., Grey, Clare P., Drews, Janina, Häcker, Joachim, Danner, Timo, Latz, Arnulf, Sotta, Dane, Palacín, M. Rosa, Martin, Jean Frédéric, Lastra, Juan Maria García, Fichtner, Maximilian, Kundu, Sumana, Kraytsberg, Alexander, Ein-Eli, Yair, Noked, Malachi, and Aurbach, Doron

Abstract

Emerging energy storage systems based on abundant and cost-effective materials are key to overcome the global energy and climate crisis of the 21st century. Rechargeable Magnesium Batteries (RMB), based on Earth-abundant magnesium, can provide a cheap and environmentally responsible alternative to the benchmark Li-ion technology, especially for large energy storage applications. Currently, RMB technology is the subject of intense research efforts at laboratory scale. However, these emerging approaches must be placed in a real-world perspective to ensure that they satisfy key technological requirements. In an attempt to bridge the gap between laboratory advancements and industrial development demands, herein, we report the first non-aqueous multilayer RMB pouch cell prototypes and propose a roadmap for a new advanced RMB chemistry. Through this work, we aim to show the great unrealized potential of RMBs.

Published
2023

6. Recent developments and future prospects of magnesium–sulfur batteries.

Author

Liping Wang, Riedel, Sibylle, Drews, Janina, and Zhao-Karger, Zhirong

Subjects
LITHIUM sulfur batteries, ENERGY storage, SURFACE passivation, ENERGY density, STORAGE batteries
Abstract

Rechargeable magnesium (Mg) batteries are promising candidates for the next generation of energy storage systems due to their potential high-energy density, intrinsic safety features and cost-effectiveness. Among the various electrochemical couples, the combination of an Mg anode with a sulfur (S) cathode stands out as an attractive option, as it offers a remarkable theoretical volumetric energy density exceeding 3,200 Wh L–1 . However, owing to the unique properties of Mg-ion electrolytes, Mg polysulfides and the surface passivation of Mg metal anodes, the development of Mg–S batteries is facing multiple challenges. In this review, recent advancements in designing efficient electrolytes for Mg–S battery systems are summarized. Apart from electrolytes, we also discuss the progress made in fabricating new S cathode composites, Mg anodes and functional separators, focusing on their roles in addressing the critical issues of the Mg–S systems. Finally, it is worth pointing out that the collaborative research combining experimental investigations and theoretical modelling could provide deeper insights into the mechanisms of Mg–S battery systems and promote their development. Overall, the comprehensive insights about the S-redox reaction, polysulfide shuttle problems and degradation mechanism in Mg–S batteries are discussed, which is of profound importance for creating solutions to enhance the overall performance of Mg–S batteries. This review aims to providing an overview of the current state of the research to stimulate innovative thoughts on the fundamental guidelines for facilitating development of Mg–S batteries. [ABSTRACT FROM AUTHOR]

Published
2024
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7. A practical perspective on the potential of rechargeable Mg batteries

Author

Blázquez, J. Alberto, Maça, Rudi R., Leonet, Olatz, Azaceta, Eneko, Mukherjee, Ayan, Zhao-Karger, Zhirong, Li, Zhenyou, Kovalevsky, Aleksey, Fernández-Barquín, Ana, Mainar, Aroa R., Jankowski, Piotr, Rademacher, Laurin, Dey, Sunita, Dutton, Siân E., Grey, Clare P., Drews, Janina, Häcker, Joachim, Danner, Timo, Latz, Arnulf, Sotta, Dane, Palacin, M. Rosa, Martin, Jean-Frédéric, Lastra, Juan Maria García, Fichtner, Maximilian, Kundu, Sumana, Kraytsberg, Alexander, Ein-Eli, Yair, Noked, Malachi, Aurbach, Doron, Blázquez, J. Alberto, Maça, Rudi R., Leonet, Olatz, Azaceta, Eneko, Mukherjee, Ayan, Zhao-Karger, Zhirong, Li, Zhenyou, Kovalevsky, Aleksey, Fernández-Barquín, Ana, Mainar, Aroa R., Jankowski, Piotr, Rademacher, Laurin, Dey, Sunita, Dutton, Siân E., Grey, Clare P., Drews, Janina, Häcker, Joachim, Danner, Timo, Latz, Arnulf, Sotta, Dane, Palacin, M. Rosa, Martin, Jean-Frédéric, Lastra, Juan Maria García, Fichtner, Maximilian, Kundu, Sumana, Kraytsberg, Alexander, Ein-Eli, Yair, Noked, Malachi, and Aurbach, Doron

Abstract

Emerging energy storage systems based on abundant and cost-effective materials are key to overcome the global energy and climate crisis of the 21st century. Rechargeable Magnesium Batteries (RMB), based on Earth-abundant magnesium, can provide a cheap and environmentally responsible alternative to the benchmark Li-ion technology, especially for large energy storage applications. Currently, RMB technology is the subject of intense research efforts at laboratory scale. However, these emerging approaches must be placed in a real-world perspective to ensure that they satisfy key technological requirements. In an attempt to bridge the gap between laboratory advancements and industrial development demands, herein, we report the first non-aqueous multilayer RMB pouch cell prototypes and propose a roadmap for a new advanced RMB chemistry. Through this work, we aim to show the great unrealized potential of RMBs.

Published
2023

10. Modelling of Magnesium Intercalation into Chevrel Phase

Author

Drews, Janina, Dlugatch, Ben, Wiedemann, Johannes, Maça, Rudi Ruben, Wang, Liping, Blazquez, J. Alberto, Zhao-Karger, Zhirong, Fichtner, Maximilian, Aurbach, Doron, Danner, Timo, and Latz, Arnulf

Subjects
Magnesium Ionen Batterie, Kontinuum Modellierung, Elektrochemie
Published
2023

11. A practical perspective on the potential of rechargeable Mg batteries

Author

Blázquez, J. Alberto, primary, Maça, Rudi R., additional, Leonet, Olatz, additional, Azaceta, Eneko, additional, Mukherjee, Ayan, additional, Zhao-Karger, Zhirong, additional, Li, Zhenyou, additional, Kovalevsky, Aleksey, additional, Fernández-Barquín, Ana, additional, Mainar, Aroa R., additional, Jankowski, Piotr, additional, Rademacher, Laurin, additional, Dey, Sunita, additional, Dutton, Siân E., additional, Grey, Clare P., additional, Drews, Janina, additional, Häcker, Joachim, additional, Danner, Timo, additional, Latz, Arnulf, additional, Sotta, Dane, additional, Palacin, M. Rosa, additional, Martin, Jean-Frédéric, additional, Lastra, Juan Maria García, additional, Fichtner, Maximilian, additional, Kundu, Sumana, additional, Kraytsberg, Alexander, additional, Ein-Eli, Yair, additional, Noked, Malachi, additional, and Aurbach, Doron, additional

Published
2023
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13. Modeling of Magnesium Intercalation into Chevrel Phase Mo6S8: Report on Improved Cell Design.

Author

Drews, Janina, Wiedemann, Johannes, Maça Alaluf, Rudi Ruben, Wang, Liping, Blázquez, J. Alberto, Zhao‐Karger, Zhirong, Fichtner, Maximilian, Danner, Timo, and Latz, Arnulf

Subjects
MAGNESIUM ions, MAGNESIUM, PARTICLE size distribution, CRYSTAL structure, THERMODYNAMICS, MAGNESIUM compounds
Abstract

A good understanding of the limiting processes in rechargeable magnesium batteries is key to develop novel high‐capacity/high‐voltage cathode materials. Thereby, the performance of magnesium‐ion batteries can strongly depend on the morphology of the intercalation cathode. Moreover, high mass loadings are essential for commercialization. In this work the influence of different mass loadings are studied in addition to the impact of the particle size distribution of the active material. Therefore, a detailed continuum model is developed, which is able to describe the complex intercalation of magnesium into a Chevrel phase (CP) cathode. The model considers the thermodynamics, kinetics and interplay of the two energetically different intercalation sites of Mo6S8, which results from its unique crystal structure, as well as the impact of the desolvation on the electrochemical reactions and possible ion agglomeration. Ideal combinations of mass loading and electrolyte concentration as well as the desired CP particle size are determined for the state‐of‐the‐art magnesium tetrakis(hexafluoroisopropyloxy)borate Mg[B(hfip)4]2 electrolyte. [ABSTRACT FROM AUTHOR]

Published
2023
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14. Continuum Modelling as Tool for Optimizing the Cell Design of Magnesium Batteries

Author

Drews, Janina, Jankowski, Piotr, Häcker, Joachim, Maça, Rudi Ruben, Wang, Liping, Li, Zhenyou, Wiedemann, Johannes, García Lastra, Juan Maria, Vegge, Tejs, Wagner, Norbert, Friedrich, Kaspar Andreas, Blázquez, J. Alberto, Zhao-Karger, Zhirong, Fichtner, Maximilian, Danner, Timo, and Latz, Arnulf

Subjects
electron-transfer kinetics, continuum modelling, desolvation, rechargeable magnesium battery
Published
2022

15. Modelling of Magnesium Intercalation into Chevrel Phase Mo6S8

Author

Drews, Janina, Maça, Rudi Ruben, Li, Zhenyou, Wiedemann, Johannes, Danner, Timo, Blazquez, J. Alberto, Zhao-Karger, Zhirong, Fichtner, Maximilian, and Latz, Arnulf

Subjects
continuum modelling, Chevrel Phase, rechargeable magnesium battery
Published
2022

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

Author

Drews, Janina, primary, Jankowski, Piotr, additional, Häcker, Joachim, additional, Li, Zhenyou, additional, Danner, Timo, additional, García Lastra, Juan Maria, additional, Vegge, Tejs, additional, Wagner, Norbert, additional, Friedrich, K. Andreas, additional, Zhao-Karger, Zhirong, additional, Fichtner, Maximilian, additional, and Latz, Arnulf, additional

Published
2021
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17. Modeling of Electron-Transfer Kinetics in Magnesium Electrolytes: Influence of the Solvent on the Battery Performance

Author

Drews, Janina, Jankowski, Piotr, Häcker, Joachim, Li, Zhenyou, Danner, Timo, Lastra, Juan Maria García, Vegge, Tejs, Wagner, Norbert, Friedrich, K. Andreas, Zhao-Karger, Zhirong, Fichtner, Maximilian, Latz, Arnulf, Drews, Janina, Jankowski, Piotr, Häcker, Joachim, Li, Zhenyou, Danner, Timo, Lastra, Juan Maria García, Vegge, Tejs, Wagner, Norbert, Friedrich, K. Andreas, Zhao-Karger, Zhirong, Fichtner, Maximilian, and Latz, Arnulf

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 impact 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 calculations 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 desolvation 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 Mg[B(hfip)4]2 salt. It becomes apparent that not necessarily a whole solvent molecule must be stripped from the solvated Mg2+ cation before the first reduction step can take place. It seems to be sufficient to have one coordination site available, so that the Mg2+ cation is able to get closer to the electrode surface. Thereby, the initial desolvation determines the deposition reaction for mono-, tri- and tetraglyme, whereas the influence of the desolvation on the plating reaction is minor for diglyme and THF. Overall, we can give a clear recommendation for diglyme to be applied as solvent in magnesium electrolytes.

Published
2021

20. Modeling of ion agglomeration in magnesium electrolytes and its impacts on the battery performance

Author

Drews, Janina, Danner, Timo, Jankowski, Piotr, Vegge, Tejs, García Lastra, Juan Maria, Liu, Runyu, Zhao-Karger, Zhirong, Fichtner, Maximilian, Latz, Arnulf, Drews, Janina, Danner, Timo, Jankowski, Piotr, Vegge, Tejs, García Lastra, Juan Maria, Liu, Runyu, Zhao-Karger, Zhirong, Fichtner, Maximilian, and Latz, Arnulf

Abstract

The choice of electrolyte has a crucial influence on the performance of rechargeable magnesium batteries. In multivalent electrolytes an agglomeration of ions to pairs or bigger clusters may affect the transport in the electrolyte and the reaction at the electrodes. In this work we include the formation of clusters in our general model for magnesium batteries. In our model we consistently take into account the effect of cluster formation on transport, thermodynamics and kinetics. The model is used to analyze the effect of ion clustering in a Mg[B(hfip) 4 ] 2 \ DME electrolyte. It becomes apparent that the ion agglomeration is able to explain experimentally observed phenomena at high salt concentrations.

Published
2020

21. The Effect of Chlorides on the Performance of DME/Mg[B(HFIP)4]2Solutions for Rechargeable Mg Batteries

Author

Dlugatch, Ben, Drews, Janina, Attias, Ran, Gavriel, Bar, Ambar, Adar, Danner, Timo, Latz, Arnulf, and Aurbach, Doron

Abstract

One of the major issues in developing electrolyte solutions for rechargeable magnesium batteries is understanding the positive effect of chloride anions on Mg deposition-dissolution processes on the anode side, as well as intercalation-deintercalation of Mg2+ions on the cathode side. Our previous results suggested that Cl−ions are adsorbed on the surface of Mg anodes and Chevrel phase MgxMo6S8cathodes. This creates a surface add-layer that reduces the activation energy for the interfacial Mg ions transportation and related charge transfer, as well as promotes the transport of Mg2+from the solution phase to the Mg anode surface and into the cathodes’ host materials. Here, this work further examines the effect of adding chlorides to the state-of-the-art Mg[B(HFIP)4]2/DME electrolyte solution, specifically focusing on reversible magnesium deposition, as well as the performance of Mg cells with benchmark Chevrel phase cathodes. It was observed that the presence of chlorides in these solutions facilitates both Mg deposition, and Mg2+ions intercalation, whereby this effect is more pronounced as the purity level of the solution is lowered.

Published
2023
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22. Modeling of Ion Agglomeration in Magnesium Electrolytes and its Impacts on Battery Performance

Author

Drews, Janina, Danner, Timo, Jankowski, Piotr, Vegge, Tejs, Garc��a Lastra, Juan Maria, Liu, Runyu, Zhao���Karger, Zhirong, Fichtner, Maximilian, and Latz, Arnulf

Subjects
DDC 540 / Chemistry & allied sciences, Computational chemistry, Electrolytes, ion aggregation, Elektrolyt, Magnesium, 7. Clean energy, Electric batteries, Batterie
Abstract

Raised overpotential by clustering?! A new continuum model that considers ion aggregation is presented and applied to magnesium tetrakis(hexafluoroisopropyloxy)borate in dimethoxyethane as electrolyte. Thereby, the properties of ion clusters and their effects on the battery performance are analyzed. Simulations imply that cluster formation can be essential to explain the concentration-dependence of experimental data. The choice of electrolyte has a crucial influence on the performance of rechargeable magnesium batteries. In multivalent electrolytes an agglomeration of ions to pairs or bigger clusters may affect the transport in the electrolyte and the reaction at the electrodes. In this work the formation of clusters is included in a general model for magnesium batteries. In this model, the effect of cluster formation on transport, thermodynamics and kinetics is consistently taken into account. The model is used to analyze the effect of ion clustering in magnesium tetrakis(hexafluoroisopropyloxy)borate in dimethoxyethane as electrolyte. It becomes apparent that ion agglomeration is able to explain experimentally observed phenomena at high salt concentrations., publishedVersion

23. Modeling of Ion Agglomeration in Magnesium Electrolytes and its Impacts on Battery Performance

Author

Drews, Janina, Danner, Timo, Jankowski, Piotr, Vegge, Tejs, García Lastra, Juan Maria, Liu, Runyu, Zhao‐Karger, Zhirong, Fichtner, Maximilian, and Latz, Arnulf

Subjects
7. Clean energy
Abstract

The choice of electrolyte has a crucial influence on the performance of rechargeable magnesium batteries. In multivalent electrolytes an agglomeration of ions to pairs or bigger clusters may affect the transport in the electrolyte and the reaction at the electrodes. In this work the formation of clusters is included in a general model for magnesium batteries. In this model, the effect of cluster formation on transport, thermodynamics and kinetics is consistently taken into account. The model is used to analyze the effect of ion clustering in magnesium tetrakis(hexafluoroisopropyloxy)borate in dimethoxyethane as electrolyte. It becomes apparent that ion agglomeration is able to explain experimentally observed phenomena at high salt concentrations.

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

Author

Drews J, Jankowski P, Häcker J, Li Z, Danner T, García Lastra JM, Vegge T, Wagner N, Friedrich KA, Zhao-Karger Z, Fichtner M, and Latz A

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 impact 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 calculations 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 desolvation 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 magnesium 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., (© 2021 The Authors. ChemSusChem published by Wiley-VCH GmbH.)

Published
2021
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