To achieve zero carbon emissions, the transition to renewable energy heavily depends on energy storage systems with high energy density, such as anode-free Li-metal batteries (AFLMBs). However, AFLMBs face challenges such as active Li loss and uneven Li deposition, making the stabilization of the solid electrolyte interphase (SEI) crucial for enhanced battery performance. We employed density functional theory (DFT) calculations and ab initio molecular dynamics (AIMD) simulations to investigate the potential decomposition mechanisms of a high-performance gel polymer electrolyte (FN-GPE) on a Li/Cu anode surface. The FN-GPE consists of PVDF-co-HFP, FEC, DME, LiPF₆, and LiNO₃. The decomposition products include organic compounds such as alkoxides (C_xH_yO_z) and unsaturated carbon chains, alongside inorganic compounds like LiF, Li₂O, Li₃N, and Li₃P. The atomic charge distribution in the FN-GPE@Li/Cu system aligns well with experimental X-ray photoelectron spectroscopy (XPS). This computational study demonstrates the efficiency of the combined DFT-AIMD method in exploring potential SEI components of the FN-GPE and offers insights for designing electrolytes to construct multi-component hybrid organic-inorganic SEIs.

中文翻译：

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揭示凝胶聚合物电解质中多组分杂化有机-无机SEI的形成：一项计算研究


为了实现零碳排放，向可再生能源的过渡在很大程度上取决于具有高能量密度的储能系统，例如无阳极锂金属电池 （AFLMB）。然而，AFLMB 面临主动锂损失和锂沉积不均匀等挑战，这使得固体电解质界面 （SEI） 的稳定对于增强电池性能至关重要。我们采用密度泛函理论 （DFT） 计算和从头计算分子动力学 （AIMD） 模拟来研究高性能凝胶聚合物电解质 （FN-GPE） 在 Li/Cu 阳极表面的潜在分解机制。FN-GPE 由 PVDF-co-HFP、FEC、DME、LiPF₆ 和 LiNO₃ 组成。分解产物包括有机化合物，如醇盐 （C_xH_yO_z） 和不饱和碳链，以及无机化合物，如 LiF、Li₂O、Li₃N 和 Li₃P。FN-GPE@Li/Cu 系统中的原子电荷分布与实验 X 射线光电子能谱 （XPS） 非常吻合。这项计算研究证明了 DFT-AIMD 组合方法在探索 FN-GPE 的潜在 SEI 组分方面的效率，并为设计电解质以构建多组分杂化有机-无机 SEI 提供了见解。