Decoupling of ion pairing and ion conduction in ultrahigh-concentration electrolytes enables wide-temperature solid-state batteries

Xu, Shengjun; Xu, Ruogu; Tong, Ying; Chen, Ke; Sun, Chengguo; Hu, Guofeng; Bai, Shuo; Cheng, Hui‐Ming; Sun, Zhenhua; Li, Feng

doi:10.1039/d2ee01053d

Cited by 41 publications

(32 citation statements)

References 38 publications

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“…[57] The method of adjusting the type and concentration of Li salts has been employed to construct stable interfacial layers. [58][59][60] Yao et al designed a quasiionic liquid/polymer electrolyte by incorporating [Li(DMF) 3 ] [TFSI] solvated complex with PVDF-HFP. Benefiting from the coordination of DMF to lithium ions, the obtained polymer electrolyte exhibits high room-temperature Li-ion conductivity and oxidation stability.…”

Section: Introductionmentioning

confidence: 99%

Two‐Dimensional Fluorinated Graphene Reinforced Solid Polymer Electrolytes for High‐Performance Solid‐State Lithium Batteries

Zhai

Yang

Wei

et al. 2022

Advanced Energy Materials

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void-free films, the PVDF-HFP matrix in SPEs is composed of micro-sized spherical particles with voids forming between the particles. These voids may reduce the mechanical strength and cause uneven distribution of lithium-ion flux, resulting in uncontrolled Li dendrite growth. Second, when matching with the Li metal anode, the alkaline radicals on the surface of Li metal rapidly induce the uncontrolled dehydrofluorination of PVDF-HFP (-resulting in the formation of unstable solid electrolyte interphase (SEI) with porous structure. [33,34] The porous structure of the SEI layer leads to continuous side reactions between Li metal and solvated molecules, resulting in the further deterioration of interfacial stability. In addition, the residual solvents such as N, N-dimethylformamide (DMF), and N-Methyl pyrrolidone (NMP) continue to decompose under high potential due to the relatively high highest occupied molecular orbital (HOMO) energy, which will cause the rapid capacity decay of high-voltage cathodes. [35,36] Tremendous efforts have been devoted to solve these problems. The incorporation of SiO 2 nanoparticles, LDH nanosheets, palygorskite nanowires, and glass fiber membranes into PVDF-based electrolytes was utilized to improve the mechanical properties and suppress the Li dendrite growth. [37][38][39][40][41] However, the ionic insulating feature of these additives inevitably leads to the uneven Li-ion flux distribution and hinders of forming the stable electrode/electrolyte interface. Introduction of Li-ion conducting active fillers such as Li 6.

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Section: Introductionmentioning

confidence: 99%

Two‐Dimensional Fluorinated Graphene Reinforced Solid Polymer Electrolytes for High‐Performance Solid‐State Lithium Batteries

Zhai

Yang

Wei

et al. 2022

Advanced Energy Materials

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“…39,40 DMSO could also help to generate a stable interface layer between Li metal and PVDF-based electrolytes, which is benecial for achieving long-life SSLMBs. 41 The use of the DMSO-THF mixture is to accelerate the evaporation of excessive solvent and effectively control the content of DMSO in the electrolyte lms, because THF is a widely used low-boiling-point solvent that can be easily removed from the electrolyte during the heating process.…”

Section: Resultsmentioning

confidence: 99%

An organic additive assisting with high ionic conduction and dendrite resistance of polymer electrolytes

et al. 2022

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“…Instead of explicitly including the chemistry of polymers and salts, as done previously, we choose a set of descriptors that represents the transport behavior of the system, i.e., ion diffusion and clustering behavior. Previous studies have suggested the significant effect of ion clustering on ion transport properties in SPEs [28,[75][76][77][78][79][80][81][82], which makes the distributions of cluster populations suitable descriptors for predicting transport properties. The comparison between the descriptors used in the current study with the previous studies is illustrated in Fig.…”

Section: B Featurization Methodsmentioning

confidence: 99%

Early prediction of ion transport properties in solid polymer electrolytes using machine learning and system behavior-based descriptors of molecular dynamics simulations

Khajeh¹,

Schweigert²,

Torrisi³

et al. 2022

Preprint

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Molecular dynamics simulations are useful tools to screen solid polymer electrolytes with suitable properties applicable in Li-ion batteries. However, due to the vast design space of solid polymer electrolytes, it is highly desirable to accelerate the discovery pipeline by reducing the computational time of ion transport properties from simulations. In this study, we show that with a judicious choice of descriptors, we are able to predict the equilibrium ion transport properties in LiTFSI-homopolymer systems within the first 0.5 ns of the production run of simulations. The new set of descriptors used in the current study includes the configuration of ion clusters and early time evolution of transport properties. Specifically, we find that descriptors that include information about ion clustering and dynamics of ion transport in the polymer environment outperform features extracted from only the molecular structure of the polymers. We show that these behavior-based descriptors have several advantages over polymer structure-based descriptors, as they encode system (polymer and salt) behavior rather than just the class of polymer and can be computed at any time point during the simulations. These characteristics increase the applicability of our descriptors to a wide range of polymer systems (e.g., co-polymers, blend of polymers, salt concentrations, and temperatures).

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Decoupling of ion pairing and ion conduction in ultrahigh-concentration electrolytes enables wide-temperature solid-state batteries

Abstract: Fast ion conduction and stable interfaces are predicted to be important in the development of new electrolytes. However, many unconventional solvents for electrolytes remain challenging, although they are fast ion...

Cited by 41 publications

References 38 publications

Two‐Dimensional Fluorinated Graphene Reinforced Solid Polymer Electrolytes for High‐Performance Solid‐State Lithium Batteries

Two‐Dimensional Fluorinated Graphene Reinforced Solid Polymer Electrolytes for High‐Performance Solid‐State Lithium Batteries

An organic additive assisting with high ionic conduction and dendrite resistance of polymer electrolytes

Early prediction of ion transport properties in solid polymer electrolytes using machine learning and system behavior-based descriptors of molecular dynamics simulations

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