Solid-state polymer electrolytes for high-performance lithium metal batteries

Abstract

Electrochemical cells based on alkali metal anodes are receiving intensive scientific interest as potentially transformative technology platforms for electrical energy storage. Chemical, morphological, mechanical and hydrodynamic instabilities at the metal anode produce uneven metal electrodeposition and poor anode reversibility, which, are among the many known challenges that limit progress. Here, we report that solid-state electrolytes based on crosslinked polymer networks can address all of these challenges in cells based on lithium metal anodes. By means of transport and electrochemical analyses, we show that manipulating thermodynamic interactions between polymer segments covalently anchored in the network and “free” segments belonging to an oligomeric electrolyte hosted in the network pores, one can facilely create hybrid electrolytes that simultaneously exhibit liquid-like barriers to ion transport and solid-like resistance to morphological and hydrodynamic instability.

Comprehensive Review of Polymer Architecture for All-Solid-State Lithium Rechargeable Batteries

“…Zhang et al demonstrated a facile approach by UV irradiation to prepare a flexible PEO-based crosslinked electrolyte (PTT) consisting of linear PEO, tetraglyme (TEGDME), and tetraethylene glycol dimethacrylate (TEGDMA) ( Figure 10) [97]. The SPE exhibits superior electrochemical properties with high ionic conductivity (2.7 × 10 −4 S•cm −1 at 24 • C), high transference number (0.56), wide electrochemical stability window that exceeds 5 V (Li + /Li), and low interfacial resistance; similar SPEs have also been reported [98,99]. In the work of Choudhury et al [98], the crosslinked polymer matrix comprised of PEGDMA and bis(2-methoxyethyl) ether (diglyme), and the T g and mechanical strength were found to increase with the PEGDMA content as shown in Figure 11.…”

“…The SPE exhibits superior electrochemical properties with high ionic conductivity (2.7 × 10 −4 S•cm −1 at 24 °C), high transference number (0.56), wide electrochemical stability window that exceeds 5 V (Li + /Li), and low interfacial resistance; similar SPEs have also been reported [98,99]. In the work of Choudhury et al [98], the crosslinked polymer matrix comprised of PEGDMA and bis(2-methoxyethyl) ether (diglyme), and the Tg and mechanical strength were found to increase with the PEGDMA content as shown in Figure 11. The authors observed that the materials behaved as single-phase soft solids at a critical PEGDMA content of 40%.…”

“…Nevertheless, the use of a liquid plasticizer remains advantageous for ion conduction and improving the flexibility of the SPE membrane [101,102]. [98]. Reproduced with permission from [98].…”

Greener Routes to Biomass Waste Valorization: Lignin Transformation Through Electrocatalysis for Renewable Chemicals and Fuels Production

“…SPEs are at horoughly explored topic in lithiumion battery research, as it pertainst ot he improvemento ft he energy density of the lithium-ion battery. [195][196][197] The application of SPE electrolyzers and PEM reactors can also be found in chemicalf uel cells, where the catalyst-loaded electrodes are fused onto both sides of the membrane to form am embrane electrode assembly (MEA). [198] In some examples, the catalytic metals are deposited directly on membrane surfaces.…”

Mechanical Integrity Degradation and Control of All-Solid-State Lithium Battery with Physical Aging Poly (Vinyl Alcohol)-Based Electrolyte

“…With the deepening research on all-solid-state batteries (ASSBs), an intensive scientific interest in the development of inherent safety, non-leakage, and stable high-performance electrochemical equipment has emerged to accommodate a wide range of new engineering applications, including medical implants, flexible electronics, and textiles [ 1 , 2 ]. In contrast to inorganic counterparts with a brittle crystalline phase, the solid polymer electrolyte (SPE) exhibits excellent interfacial compatibility, and superior elasticity to endure greater mechanical deformation, contributing to be cast into the complicated architectures for lithium-ion and lithium-metal batteries [ 3 , 4 , 5 ]. Consequently, a wide array of polymers such as poly (ethylene oxide) (PEO) [ 6 , 7 , 8 , 9 ], polyacrylonitrile (PAN) [ 10 , 11 , 12 , 13 ], poly (vinylidene fluoride) (PVdF) [ 14 , 15 ], and its copolymer with hexafluoropropylene (PVdF-HFP) [ 16 , 17 ], poly (methyl methacrylate) (PMMA) [ 18 , 19 , 20 ], and poly (vinyl alcohol) (PVA) [ 21 , 22 , 23 , 24 ], as well as their mixtures [ 25 , 26 , 27 , 28 ], have been adopted as the potential matrices for solid electrolytes.…”