Ion Transport in Polymer Electrolytes: Building New Bridges between Experiment and Molecular Simulation

Shao, Yunqi; Gudla, Harish; Mindemark, Jonas; Brandell, Daniel; Zhang, Chao

doi:10.1021/acs.accounts.3c00791

Cited by 3 publications

(1 citation statement)

References 59 publications

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“…23,24 Ab initio molecular dynamics (AIMD) simulations facilitate the investigation of interfacial reactions between electrolytes and electrodes. 25–28 Molecular dynamics simulations based on (reactive) force-field have been widely used to study the solvation sheath of ions, 29,30 ion transportation, 31–33 SEI formation, and dendrite growth. 34,35 The phase-field model can effectively simulate ionic diffusion, stress evolution, and electrodeposition during electrochemical processes.…”

Section: Introductionmentioning

confidence: 99%

Rational electrolyte design for Li-metal batteries operated under extreme conditions: a combined DFT, COSMO-RS, and machine learning study

Wu,

Zhan,

et al. 2024

J. Mater. Chem. A

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Section: Introductionmentioning

confidence: 99%

Rational electrolyte design for Li-metal batteries operated under extreme conditions: a combined DFT, COSMO-RS, and machine learning study

Wu,

Zhan,

et al. 2024

J. Mater. Chem. A

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Modulating the Li‐Ion Transport Pathway of Succinonitrile‐Based Plastic Crystalline Electrolytes for Solid‐State Lithium Metal Batteries

Ye,

Fu,

Zhang

et al. 2024

Adv Funct Materials

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Succinonitrile (SCN) based plastic crystal electrolytes (SPCEs) have attracted much attention for lithium metal batteries due to their considerable ionic conductivity and thermal stability. Insufficient mechanical properties, weak reductive stability, and the presence of free SCN molecules can result in adverse interfacial reactions. Polymer introduction has been explored to address these challenges. However, the introduction of polymer affects the SCN state, leading to reduced ionic conductivity, potentially due to limited segmental motion of the polymer at room temperature. Herein, a cross‐linked network polymer strategy is proposed to modify the Li‐ion transport pathway in SPCE, aiming to significantly improve the ionic conductivity. The strong interaction between the polymer matrix and SCN enhances their mutual solubility, reduces the crystallinity of SCN, and forms a rapid conduction pathway (polymer—[SCN—Li+]). The ionic conductivity of SPCE increases to 1.28 mS cm−1, with the Li‐ion migration number (tLi+ ) also rising to 0.7. Electrochemical performances in Li symmetrical, Li||LiFePO4 and Li||LiNi0.8Co0.1Mn0.1O2 cells show significant improvement at both room temperature and 0 °C. These findings suggest that designing polymer network structures in SPCEs holds promise for solid‐state lithium metal battery applications.

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Modeling solvation dynamics of transition metal redox ion through on-the-fly multi-objective Bayesian-optimized force field

Chen,

Huang,

Liu

et al. 2024

The Journal of Chemical Physics

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Modeling solvation dynamics and properties is crucial for developing electrolytes for electrochemical energy storage and conversion devices. This work reports an on-the-fly multi-objective Bayesian optimization (OTF-MOBO) method to parameterize force fields for modeling ionic solvation structures, thermodynamics, and transport properties using molecular dynamics simulations. By leveraging solvation-free energy and solvation radii as training data, we employ the data-driven OTF-MOBO algorithm to actively optimize the force field parameters. The modeling accuracy was evaluated in molecular dynamics simulations until the Pareto front in the parameter space was reached through minimized prediction errors in both solvation-free energy and solvation radii. Using transition metal redox ions (Fe3+/Fe2+, Cr3+/Cr2+, and Cu2+/Cu+) in aqueous solution as examples, we demonstrate that simple force fields combining the Lenard–Jones potential and Coulombic potential can achieve relative error below 2% in both solvation free energy and solvation radii. The optimized force fields can be further extrapolated to predict solvation entropy and diffusivities with relative error below 10% compared with experiments.

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Ion Transport in Polymer Electrolytes: Building New Bridges between Experiment and Molecular Simulation

Abstract: We clarif ied the def inition of the so-called Bruce−Vincent transference number in terms of the Onsager coef f icients, which allows a direct comparison between experiment and simulation.

Cited by 3 publications

References 59 publications

Rational electrolyte design for Li-metal batteries operated under extreme conditions: a combined DFT, COSMO-RS, and machine learning study

Rational electrolyte design for Li-metal batteries operated under extreme conditions: a combined DFT, COSMO-RS, and machine learning study

Modulating the Li‐Ion Transport Pathway of Succinonitrile‐Based Plastic Crystalline Electrolytes for Solid‐State Lithium Metal Batteries

Modeling solvation dynamics of transition metal redox ion through on-the-fly multi-objective Bayesian-optimized force field

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