Poly(Ionic Liquid)s-in-Salt Electrolytes with Co-coordination-Assisted Lithium-Ion Transport for Safe Batteries

Wang, Xiaoen; Chen, Fang Fang; Girard, Gaetan M. A.; Zhu, Haijin; MacFarlane, Douglas R.; Mecerreyes, David; Armand, Michel; Howlett, Patrick C.; Forsyth, Maria

doi:10.1016/j.joule.2019.07.008

Cited by 129 publications

(172 citation statements)

References 63 publications

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“…This electrostatic interaction or coordination was also mentioned by Smyrl et al in their earlier work when PDADMA TFSI was used with tetraglyme (G4)‐LiTFSI solvate ionic liquid . To confirm this interaction in polyIL‐based electrolytes, we have simplified the polymer electrolyte composition, by using PDADMA FSI and LiFSI binary solid electrolytes ( Figure a) and eliminating the ionic liquid component . Interestingly, the addition of LiFSI salt continuously decreases the glass transition temperature ( T g ), while the conventional PEO‐based electrolytes show an increase T g when salt concentrations is higher than 5 mol% .…”

Section: Ionic Polymer‐based Solid‐state Electrolytessupporting

confidence: 67%

Section: Ionic Polymer‐based Solid‐state Electrolytesmentioning

confidence: 99%

“…The enhanced Li + transport properties observed in superconcentrated electrolytes has been attributed to the formation of multidentate anion‐Li + ‐coordination in order to satisfy the Li + coordination environment. With increasing lithium salt content, the average number of anions coordinating with one Li + (coordination number) progressively decreased (i.e., on average each anion coordinates with more than one Li + ), which is indicative of ion clustering or aggregates . The formation of such aggregates results in a change of the transport mechanism present in these materials, shifting from a typical vehicular transport mechanism to a Li + hopping‐like transport mechanism, similar to the Grotthus transport mechanism in acid media.…”

Section: Ionic Polymer‐based Solid‐state Electrolytesmentioning

confidence: 99%

“…The simulations confirmed that the LiFSI salt plays a dual‐role as both the charge carrier and the polymer plasticizer. When increasing amounts of Li salt dissolved in the polyIL matrix, the overall anion coordination changes from being primarily associated with the polymer backbone to one where the majority of anions bridge between the polymer and the Li + , which reduces the interaction between polycations and anions, resulting in a reduced T g . When Li salt is added into the PEO matrix, the polymer chain will immediately solvate the Li + by strong PEO oxygen–Li coordination (Figure b).…”

Section: Simulation‐assisted Design Of New Solid‐state Electrolytesmentioning

confidence: 99%

“…a) The co‐coordination of polycations (green sticks), Li + ions (purple balls), and FSI anions (blue, yellow, red, and aqua colors are for N, S, O, and F atoms) in a PDADMA FSI‐LiFSI binary electrolyte. Adapted with permission . Copyright 2019, Elsevier.…”

Section: Simulation‐assisted Design Of New Solid‐state Electrolytesmentioning

confidence: 99%

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Toward High‐Energy‐Density Lithium Metal Batteries: Opportunities and Challenges for Solid Organic Electrolytes

et al. 2020

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The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adma.201905219.With increasing demands for safe, high capacity energy storage to support personal electronics, newer devices such as unmanned aerial vehicles, as well as the commercialization of electric vehicles, current energy storage technologies are facing increased challenges. Although alternative batteries have been intensively investigated, lithium (Li) batteries are still recognized as the preferred energy storage solution for the consumer electronics markets and next generation automobiles. However, the commercialized Li batteries still have disadvantages, such as low capacities, potential safety issues, and unfavorable cycling life. Therefore, the design and development of electromaterials toward high-energy-density, long-life-span Li batteries with improved safety is a focus for researchers in the field of energy materials. Herein, recent advances in the development of novel organic electrolytes are summarized toward solid-state Li batteries with higher energy density and improved safety. On the basis of new insights into ionic conduction and design principles of organic-based solid-state electrolytes, specific strategies toward developing these electrolytes for Li metal anodes, high-energy-density cathode materials (e.g., high voltage materials), as well as the optimization of cathode formulations are outlined. Finally, prospects for next generation solid-state electrolytes are also proposed.

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Section: Ionic Polymer‐based Solid‐state Electrolytessupporting

confidence: 67%

Section: Ionic Polymer‐based Solid‐state Electrolytesmentioning

confidence: 99%

Section: Ionic Polymer‐based Solid‐state Electrolytesmentioning

confidence: 99%

Section: Simulation‐assisted Design Of New Solid‐state Electrolytesmentioning

confidence: 99%

Section: Simulation‐assisted Design Of New Solid‐state Electrolytesmentioning

confidence: 99%

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Toward High‐Energy‐Density Lithium Metal Batteries: Opportunities and Challenges for Solid Organic Electrolytes

et al. 2020

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Solid‐State Batteries with Polymer Electrolytes

Iojoiu

Paillard

2020

Encyclopedia of Electrochemistry

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Expectations on solid‐state lithium batteries are at their highest as they are seen as a “next‐generation” technology, although solid polymer electrolytes have already enabled the commercialization of electrical vehicles for almost 10 years. These are powered by lithium metal batteries and use a polyethylene oxide (PEO)‐based electrolyte. Thus, after a quick review of the current state of the art on lithium batteries including various polymers electrolytes, we present some fundamentals about the lithium metal anode. We then give an overview of the different approaches that have been proposed in the past 40 years for improving the performance of these types of electrolytes. The trends that have led to the current generation of solid polymer electrolytes are reported first: They consisted in decreasing the crystallinity of PEO and increasing its chain segmental mobility while preventing electrolyte creeping at high temperature, and the use of plasticizers, fillers, statistical copolymers, and branched polymers such as cross‐linked and comb‐shaped polymers was developed. However, PEO and “dry” solid polymer electrolytes incorporating dissolved lithium salts, in general, suffer from intrinsic limitations. Thus, we then present as perspectives, the most promising polymer electrolyte concepts for improving lithium metal polymer batteries. In particular, the use of polycarbonates as alternative polymer matrixes, the use of polymers in hybrid organic/inorganic electrolytes, the use of block copolymers and liquid crystals for decorrelating conductivity from mechanical properties, and finally, the development of single‐ion conductors.

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