Acta Phys. -Chim. Sin. ›› 2021, Vol. 37 ›› Issue (2): 2008089.doi: 10.3866/PKU.WHXB202008089

Special Issue: Lithium Metal Anodes

• REVIEW • Previous Articles     Next Articles

Application of Computational Simulation on the Study of Lithium Metal Anodes

Guangbin Hua1, Yanchen Fan2, Qianfan Zhang1,*()   

  1. 1 School of Materials Science and Engineering, Beihang University, Beijing 100191, China
    2 School of Microelectronics, Southern University of Science and Technology, Shenzhen 518055, Guangdong Province, China
  • Received:2020-08-31 Published:2020-10-22
  • Contact: Qianfan Zhang
  • About author:Qianfan Zhang, Email:
  • Supported by:
    the Beijing Natural Science Foundation, China(2192029)


Lithium-metal anode batteries have the potential to serve as next-generation, high energy density batteries with high specific capacity and low electrode potential. However, due to the high reactivity of lithium, complex interfacial reactions and uncontrollable dendrite growth obstruct their application. These lithium-metal anode interfacial reactions are often accompanied by the organic electrolyte spontaneously decomposing and combustible gas subsequently escaping, which is a safety concern. It also affects the form of the solid electrolyte interphase (SEI), which is important for stabilizing the interface between the Li-metal anode and electrolyte. Uncontrollable Li dendrite growth could penetrate the separator or electrolyte, creating the risk of a short circuit. Therefore, it is necessary to optimize the lithium nucleation and deposition processes. Solid state electrolytes (SSEs) have also attracted attention for improving the energy density and safety of Li-ion batteries; however, problems such as poor ionic conductivity still exist. Computational simulations, such as molecular dynamics (MD) simulations and first-principles calculations based on density function theory (DFT), can help elucidate reaction mechanisms, explore electrode materials, and optimize battery design. In this review, we summarize the theoretical perspective gained from computational simulation studies of lithium-metal anodes. This review is organized into four sections: interfacial reactions, SEIs, lithium nucleation, and SSEs. We first explore organic-electrolyte interfacial reaction mechanisms that were revealed through MD simulations and how electrolyte additives, electrolyte concentration, operating temperature affect them. For SEI, DFT can provide an in-depth understanding of the surface chemical reaction, surface morphology, electrochemical properties, and kinetic characteristics of SEI. We review the developments in SEI transmission mechanisms and SEI materials' properties alteration by lithium metal. We further explore artificial SEI design requirements and compare the performances of artificial SEIs, including double-layer, fluorine-, and sulfur-SEIs. Lithium dendrite growth as a result of lithium nucleation and deposition is then discussed, focusing on computational studies that evaluated how doped graphene, 3D carbon fibers, porous metals, and other matrix materials regulated these processes and inhibited dendrite growth. Computational simulations evaluating transport phenomena and interface reactions between SSEs and lithium-metal anodes are then explored, followed by ideas for further design optimization. Finally, potential research directions and perspectives in this field are proposed and discussed.

Key words: Lithium metal anode, Computational simulation, Interfacial reaction, Solid electrolyte interface, Lithium nucleation


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