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Guo et al. Energy Mater. 2025, 5, 500041 https://dx.doi.org/10.20517/energymater.2024.214 Page 13 of 21

Figure 9. Schematic diagram of the simulation and modeling methods in solid lithium polymer battery.

pathway, and to partially study the complex degradation pathways and reactions at electrode surfaces [93,94] .
DFT is primarily utilized to investigate the electronic structure and chemical properties of SSB materials at
the microscopic scale. By calculating parameters such as the energy band structure and the density of states,
one can gain a profound understanding of the electrochemical performance and ion transport mechanisms
of the materials. Wu et al. developed a computational method that combines DFT and Ab initio MD
(AIMD) calculations, which was used to investigate the Li-nucleation process at the interface between
electrolytes and metal electrodes, where Li atoms were introduced on the electrode surface . Figure 10A
[25]
depicts the flowchart illustrating the simulation process for the PEO-lithium anode system. The
comprehensive computational analysis was conducted in a sequential manner, encompassing four distinct
stages. Figure 10B and C illustrates the distribution of atomic charges among oxygen and carbon atoms
within the PEO system and the PEO-Li anode system, respectively, at various stages of Li-nucleation. This
study found that highly reactive Li atoms induced PEO decomposition during the simulated nucleation
process, and the resulting SEI films contained lithium alkoxide, ethylene, and lithium ethylene complexes.

Phase-field simulation
Multi-physics simulations comprehensively consider the interactions among various physical fields, such as
electrochemistry, thermodynamics, and mechanics, within SSBs. By establishing coupled multi-physics
models, these simulations facilitate a comprehensive understanding of the complex behaviors exhibited by
SSBs during operation. A phase-field model, as a mathematical tool, is utilized to address interfacial
problems, making it suitable for exploring interfacial issues in lithium batteries [95-97] . Currently, phase-field
simulations of lithium dendrites are predominantly based on a single physical field, which limits the ability
to comprehensively study the interactions between various influencing factors. Geng et al. developed a
mechanical stress-thermodynamic phase-field theory to investigate the growth mechanisms of lithium
dendrites in solid-state polymer lithium batteries [Figure 10D-F] ; in other words, their lithium dendrite
[98]
growth model incorporates both mechanical stress and the thermal field. The research showed that high
temperature, high electrolyte modulus, and external stress slow lithium dendrite growth and reduce long