Designing Gel Polymer Electrolyte with Synergetic Properties for Rechargeable Magnesium Batteries

Wang, Liping; Li, Zhenyou; Meng, Zhen; Xiu, Yanlei; Bosubabu, Dasari; Zhao‐Karger, Zhirong; Fichtner, Maximilian; Fichtner, Prof. Maximilian; Wang, Liping; Xiu, Mr. Yanlei

doi:10.1016/j.ensm.2022.03.006

Cited by 31 publications

(19 citation statements)

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“…Owing to lacking effective SEI layers, an important current electrolyte research consensus is to develop reductively stable electrolytes which are less liable to react with the Mg electrode in thermodynamics, such as reduction-resistant salts dissolved in ether-based solvent, and thus the exposed fresh Mg surface can support reversible Mg plating/stripping. − Although considerable advances have been accomplished in recent two decades, − these new-type electrolytes still suffer from many intractable problems, such as a complex synthesis process, high cost, and Cl – corrosion. Especially, they nearly all have the disadvantage of the high sensitivity to water content, which could be not suitable for practical commercial application.…”

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confidence: 99%

Solvent Molecule Design Enables Excellent Charge Transfer Kinetics for a Magnesium Metal Anode

Wang

Hua

et al. 2022

ACS Energy Lett.

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Lacking of suitable electrolytes is a fatal obstacle for the development of rechargeable magnesium batteries (RMBs). Herein, according to the design of a series of solvent molecules, we find 3methoxypropylamine possesses a middle coordination ability that can be used as an effective solvent and realize a reversible Mg anode with traditional Mg salts. Mechanism study indicates, attributed to its unique solvated structure, energy barriers in both the charge transfer process and desolvation process are extremely low, thus leading to the fast charge transfer kinetics. The relationship between solvated structures and performances is precisely revealed for the first time in RMBs. Additionally, electrolytes with amine solvents possess outstanding water-resistant properties owing to strong hydrogen bonds between amine groups and water. This work proposes a universal design principle of solvent molecules for RMBs, inspiring a new thinking of developing advanced electrolytes in the view of solvents.

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confidence: 99%

Solvent Molecule Design Enables Excellent Charge Transfer Kinetics for a Magnesium Metal Anode

Wang

Hua

et al. 2022

ACS Energy Lett.

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“…It is worth noting that dendritic growth in Zn‐based cells is suppressed for both PEO with an average molecular weight of 100000 g mol −1[25] and UHMW PMMA despite their different influence on the ionic conductivity; the ionic conductivity is decreased for PEO [32] while it remains unchanged for UHMW PMMA [29] . These results suggest the potential benefits of incorporating UHMW polymer gel electrolytes in Zn batteries as they can help to mitigate the dendrite growth without reducing the ionic conductivity.…”

Section: Introductionmentioning

confidence: 99%

Electrolytes for Zn Batteries: Deep Eutectic Solvents in Polymer Gels

et al. 2023

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Gel polymer electrolytes composed of deep eutectic solvent acetamide4:Zn(TFSI)2 and poly(ethylene oxide) (PEO) are prepared by using a fast, solvent‐free procedure. The effect of the PEO molecular weight and its concentration on the physicochemical and electrochemical properties of the electrolytes are studied. Gels prepared with ultrahigh molecular‐weight PEO present pseudo‐solid behavior and ionic conductivity even higher than that of the original liquid electrolyte. A decrease in the dendritic growth in soft gels with PEO contents up to 1 wt % is demonstrated. The changes in the chemical structure of the electrolyte produced by the strong interactions between ethylene oxide units and Zn2+ have also been studied. The addition of PEO takes the electrolyte out of its original eutectic composition, producing blend crystallization. However, it is possible to retain the eutectic point of the electrolyte in a gel form if the addition of PEO is accompanied by the reduction of acetamide.

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“…24 Gel polymer electrolytes (GPEs) were examined as well. 25,26 Mg(TFSI) 2 is an ether-soluble salt. Its ethereal solutions possess good ionic conductivity, a wide electrochemical stability window, and exceptional chemical stability; 24,27,28 for these reasons, they have been receiving great attention lately.…”

Section: ■ Introductionmentioning

confidence: 99%

Understanding the Unique Thermodynamic Behavior of MgTFSI₂/DME Solutions. Part 1: Phase Diagram, Partial Volumes, and Densities

Holin,

Gofer,

Major

et al. 2023

J. Phys. Chem. C

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A unique thermodynamic behavior was observed for solutions of magnesium bis(trifluoromethanesulfonyl) imide in 1,2-dimethoxyethane (DME), highly promising solutions for rechargeable Mg batteries: between 287 and 373 K, the solution exists as two immiscible phases, each with a different salt concentration, volume, and density. These characteristics depend strongly on temperature. To study this dependence, a phase diagram was constructed. In addition, partial phase volumes and densities were measured as a function of temperature. We observed that the temperature–molar fraction phase diagram exhibits closed-loop behavior, which is circumscribed by 287 and 373 K, with 333 K as an inversion locus. Below 287 K, the solution exists as a single homogeneous phase. At 287 K and above, the solution separates into two immiscible phases: a concentrated and dense lower phase and a dilute upper phase. As the temperature increases to 333 K, the lower phase becomes more concentrated and denser, and its partial volume decreases. The reverse trends are observed for the upper phase. From 333 K and above, the trends reverse: the upper phase becomes more concentrated but its partial volume continues to grow at the expense of the lower phase, while the lower phase concentration decreases. At 373 K, the two phases merge into a single homogeneous phase.

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Designing Gel Polymer Electrolyte with Synergetic Properties for Rechargeable Magnesium Batteries

Cited by 31 publications

References 50 publications

Solvent Molecule Design Enables Excellent Charge Transfer Kinetics for a Magnesium Metal Anode

Solvent Molecule Design Enables Excellent Charge Transfer Kinetics for a Magnesium Metal Anode

Electrolytes for Zn Batteries: Deep Eutectic Solvents in Polymer Gels

Understanding the Unique Thermodynamic Behavior of MgTFSI₂/DME Solutions. Part 1: Phase Diagram, Partial Volumes, and Densities

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Designing Gel Polymer Electrolyte with Synergetic Properties for Rechargeable Magnesium Batteries

Cited by 31 publications

References 50 publications

Solvent Molecule Design Enables Excellent Charge Transfer Kinetics for a Magnesium Metal Anode

Solvent Molecule Design Enables Excellent Charge Transfer Kinetics for a Magnesium Metal Anode

Electrolytes for Zn Batteries: Deep Eutectic Solvents in Polymer Gels

Understanding the Unique Thermodynamic Behavior of MgTFSI2/DME Solutions. Part 1: Phase Diagram, Partial Volumes, and Densities

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Understanding the Unique Thermodynamic Behavior of MgTFSI₂/DME Solutions. Part 1: Phase Diagram, Partial Volumes, and Densities