Abstract The composition of two different categories of anode materials, i.e. layered and alloy type is the future of anode material in Li-ion batteries. In our work, using First-principles approach, we proposed multilayer heterostructure of graphene/graphite (layered type) with silicon monolayer (Si-ML) (origin is alloy type), as a potential anode material for LiB’s. The synergetic effect of the delocalized π electron of carbon and localized π electron of Si-ML plays a crucial role in maintaining the electron and ion conductivity increases the stability and specific capacity with moderate open circuit voltage. The model structures proposed in this work shows high specific capacities in the range of 748 to 438 mAh-gm−1. This indicates that we can tune the specific capacity using the different ratio of carbon and silicon layers. The localized π electron helps to restrict the volume expansion within 15% for a fully lithiated model structure. The low interlayer diffusion energy of Li-ion makes all the heterostructure as a potential anode material. The proposed study will help to understand the Li storage properties of the carbon/silicon based composite to develop the anode materials with a certain approach.

中文翻译：

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定域和离域 π 电子对 Si/C 异质结构锂存储性能的协同作用

摘要 锂离子电池负极材料的未来发展方向是层状和合金型两大类负极材料的组合。在我们的工作中，使用第一性原理方法，我们提出了石墨烯/石墨（层状）与单层硅（Si-ML）（起源于合金类型）的多层异质结构，作为 LiB 的潜在负极材料。碳的离域π电子和Si-ML的定域π电子的协同作用在维持电子和离子电导率方面起着至关重要的作用，在适度的开路电压下增加了稳定性和比容量。这项工作中提出的模型结构显示出 748 至 438 mAh-gm-1 范围内的高比容量。这表明我们可以使用不同的碳层和硅层比例来调整比容量。对于完全锂化的模型结构，局部 π 电子有助于将体积膨胀限制在 15% 以内。锂离子的低层间扩散能使所有异质结构成为潜在的负极材料。所提出的研究将有助于了解碳/硅基复合材料的锂存储特性，从而通过某种方法开发负极材料。