针对高比表面积碳材料作为锂电池负极应用中面临的首次库伦效率低、放电电位高、循环稳定性差等问题，本项目提出以单层石墨烯构建模型研究体系，综合利用理论模拟和原位光谱手段，深入研究薄层碳材料储锂过程中涉及的锂碳相互作用机理和相关界面问题。本项目在前期的研究基础上，将基于对石墨烯晶畴、缺陷和掺杂、层间堆叠方式和层间距的精确调控，利用电化学表征过程中的原位拉曼、原位红外、原位同步辐射等手段，结合第一性原理和分子动力学计算，理解影响石墨烯表面上锂的吸附、沉积以及固体电解质界面形成过程中的碳电极结构因素、电解质因素和测试方法因素，深入认识决定锂吸脱附电位、吸附容量和迁移扩散速率的科学机制，形成结构-界面-过程之间的关联关系。本研究可望为相关碳负极材料的合理应用提供有效参考和指导，促进可实用化、新型碳负极材料与技术的进一步发展。

High-specific-surface-area carbons (HSSACs) have been intensively investigated in the anodes of Li-ion batteries but encountered problems such as low initial Coulombic efficiency, high discharging potential, unstable cycling and so on. To overcome these problems, we propose to study the Li-carbon interaction and related interface for deeply understanding the mechanisms behind Li-ion storage on materials consisting of thin carbon layers, for which a combination of simulation and in-situ spectroscopy will be utilized on a model system of single layer graphene. Based on the previous results, factors such as the crystal domain size, defects and doping, stacking and the interlayer distance in graphene materials will be tuned for the research with in-situ techniques like Raman, infrared, synchrotron-based spectroscopies and computational methods like ab initial and molecular dynamics. The target of the research is to understand the adsorption and deposition of Li on graphene, the factors influencing the formation of solid electrolyte interface and the effects of measurement method in the electrochemical testing on the interface and performance. Such research will allow us to build the relationship among the structure, interface and process, which will further benefit to the design and preparation of HSSAC-related carbon anodes, for the practical applications of such carbons.