Review on the First-Principles Calculation in Lithium-Sulfur Battery

Zhang Xiaofei; Li Shenhao; Wang Zhen; Yan Jian; Liu Jiaqin; Wu Yucheng

doi:10.7536/PC220819

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Prog Chem ›› 2023, Vol. 35 ›› Issue (3) : 375-389. DOI: 10.7536/PC220819

Review

Review on the First-Principles Calculation in Lithium-Sulfur Battery

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Abstract

Lithium-sulfur (Li-S) batteries are considered as a promising next-generation high-energy battery system due to their ultrahigh theoretical capacity, energy density and the merits of sulfur in terms of abundant resource and environmental friendliness. However, their practical application is confronted with several critical problems including insulation of sulfur and discharge products, shuttle effect of soluble lithium polysulfides, and sluggish reaction kinetics of sulfur, etc. Significant progress has been achieved in addressing these problems by sulfur electrode design, functional separator/interlayer, liquid-electrolyte modification, and solid-electrolyte strategy. Nevertheless, there is still a lack of in-depth understanding of real-time dynamic reaction process and mechanism as well as electrode/electrolyte interface regulation strategy in Li-S batteries. First-principles calculation has gradually developed into an important research tool in various disciplines such as materials, chemistry and energy, facilitating to understand the properties of reaction species, interactions between molecules or/and electrons, electrochemical reaction processes and laws, and dynamic evolution of electrode/electrolyte from the molecular/atomic level. It delivers distinct advantages beyond “experimental trial and error” method in studying the multi-electron and multi-ion redox process in Li-S battery. In this paper, important advances in the application of first principles calculation to study the interactions between electrodes and polysulfides, charge-discharge reaction mechanisms, and electrolytes in Li-S batteries are comprehensively reviewed, and the current challenge and enlightening directions for application of first-principles calculation to study Li-S batteries are also prospected.

Key words

Li-S battery / first-principles / theoretical calculation / electrode materials / charge-discharge mechanism / electrolyte

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Zhang Xiaofei , Li Shenhao , Wang Zhen , et al . Review on the First-Principles Calculation in Lithium-Sulfur Battery[J]. Progress in Chemistry. 2023, 35(3): 375-389 https://doi.org/10.7536/PC220819

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Funding

National Natural Science Foundation of China(51972093)

National Natural Science Foundation of China(U1810204)

National Natural Science Foundation of China(U1910210)

Nature Science Foundation of Anhui Province(2008085ME129)

Key Research and Development Plan of Anhui Province(202004b11020024)

Fundamental Research Funds for the Central Universities of China(PA2021GDSK0087)

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Received	Revised	Published
2022-08-18	2022-12-19	2023-03-24
Issue Date
2023-02-16

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