Progress in Theoretical Calculation and Simulation of Sulfide Solid Electrolytes and Their Application in All-Solid-State Batteries

Abstract

Along with the development of electric vehicles and electronic devices, all-solid-state batteries (ASSBs) have become the next-generation energy storage batteries, owing to their safety and chemical stability. Sulfide Solid Electrolytes (SSEs) are deemed to be crucial materials for ASSBs because of their ultrahigh ionic conductivity (10⁻³-10⁻² S cm⁻¹), but are still plagued by the narrow electrochemical window and poor interfacial stability. In this paper, we summarize our systematic research progress on sulfide SSEs from the view of how theoretical calculations and simulations play a crucial role in material design. First-principles calculation gives evidence of the structure’s stability and ion migration mechanism for electrolytes, MD and AIMD simulations provide insights for the dynamic diffusion behavior and the interface reaction mechanism. High-throughput screening and machine learning have accelerated new electrolyte designs. Scientists discovered Li₁₀GeP₂S₁₂ and explored ion dynamics in a crystal lattice of that material. There are also material interface phenomena such as space charge layers and chemical breakdown. These problems can be managed by developing and tuning appropriate computational models to steer material doping and protective layer design. In this paper, we demonstrate that the combination of computer simulations and real experiments is valuable.

Keywords

Sulfide solid electrolyte / All-solid-state battery / Theoretical calculation and simulation in SSEs

Acknowledgments

This work was supported by Guangdong Province NaturaScience Foundation (2023A1515011122) and South China Normal University Extracurricular Research General Project Cultivation Program (24XZGB07). Youth Teacher Research and Cultivation Fund of South China Normal University (Project No. 671866), presided over, 30,000 CNY.

Author Contributions

Conceptualization, Y.F.; Methodology, J.L. and Z.Z.; Validation, Y.F., J.L. and Y.H.; Formal Analysis, G.H. and L.L.; Investigation, Y.F., Z.W. and H.H.; Resources, J.L.; Data Curation, H.H. and G.H.; Writing-Original Draft Preparation, Y.F.; Writing-Review & Editing, J.L., Z.Z. and J.C.; Visualization, Z.L. and G.H; Supervision, J.Z. and L.Z.; Project Administration, J.L. and Y.H.

Ethics Statement

Not applicable.

Informed Consent Statement

Not applicable.

Data Availability Statement

Data sharing is not applicable to this article, as no new data were created in this study.

Funding

This research was funded by Guangdong Province NaturaScience Foundation (2023A1515011122); South China Normal University Extracurricular Research General Project Cultivation Program (24XZGB07) and Youth Teacher Research and Cultivation Fund of South China Normal University (Project No. 671866).

Declaration of Competing Interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

AI Statement

During the preparation of this work, the authors used Deepseek in order to improve readability and language. After using this tool, the authors reviewed and edited the content as needed and take full responsibility for the content of the publication. Explanation of the use of AI. 1. Since my learning ability is still insufficient, and I do not express and summarize the literature data well, thus, I use AI tools to make the data presentation more accurate. 2. In the process of writing the article, because I need to use another language, and in order to better present the article, I used AI to help me correct the grammar of the sentence and the smoothness of the sentence.

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