基于X-射线光谱模拟的硼杂笼富勒烯功能材料的结构与性能研究

Boron-doped fullerene is a kind of important novel functional materials which possess unique physical and chemical properties, and thus could remedy the disadvantage of traditional fullerene. But as far as our knowledge concerns, the large numbers of isomers which own very similar energies could not be distinguished effectively. Based on the sensitivity of x-ray spectrum to chemical environment, our item refers to a method to identify the isomers of boron-doped fullerene. Making use of the density functional theory (DFT) method, the near-edge x-ray absorption fine structure (NEXAFS), x-ray photoelectron (XPS) and x-ray emission (XES) spectra of different kinds of novel boron-doped fullerene have been simulated and analyzed systemically. The different isomers can be well distinguished according to the strong isomer-dependent “fingerprints” in the spectra. By discussing the relationship of the x-ray spectrum, the geometry configuration and the electronic structures, the forming mechanisms of the spectra are elaborately explained. Furthermore, the connection in the spectrum, the structures and the relative contents is abstracted to summarize the rules of isomers discriminance and also obtain the corresponding parameters. Knowledge acquired in this item could provide a criterion for identifying the isomers of boron-doped fullerene, and could help to illustrate their spectrum properties. This item could be regard as a significant research which can provide valuable theoretical information for further industrial manufacture and purification of these novel functional materials.

硼杂笼富勒烯具有独特的物理和化学性质，作为弥补传统富勒烯不足的重要新型功能材料，迄今仍面临着尚无法有效分辨其所存在大量能量相近异构体的难题。本项目提出一种基于X射线光谱对化学环境的敏感性来鉴别指认硼杂笼富勒烯的方法。通过采用密度泛函理论系统模拟并分析不同类型硼杂笼富勒烯体系的各种X射线光谱(包括XPS、NEXAFS及XES)，深入探讨X射线光谱与几何构型、电子结构的内在关系，阐释谱图微观成因，并凝炼谱图信息与异构体特定结构及其相对含量之间的对应关系，进而总结出判别指认硼杂笼富勒烯异构体的规律并获得相应指标。本项目将为硼杂笼富勒烯异构体的辨别指认提供判断标准和依据，有助于明确其谱学性质，并为该类功能材料的工业化制备与提纯提供可靠的理论依据。

本项目按照原定研究计划，提出了一种基于X射线光谱对化学环境的敏感性来鉴别指认硼杂笼富勒烯的方法。通过采用密度泛函理论系统模拟并分析不同类型硼杂笼富勒烯体系的各种X射线光谱(包括XPS、NEXAFS及XES)，深入探讨了X射线光谱与几何构型、电子结构的内在关系，阐释了谱图微观成因，并凝炼出谱图信息与异构体特定结构及其相对含量之间的对应关系，进而总结出判别指认硼杂笼富勒烯异构体的规律并获得相应指标。本项目的研究成果可为硼杂笼富勒烯异构体的辨别指认提供判断标准和依据，有助于明确其谱学性质，并为该类功能材料的工业化制备与提纯提供可靠的理论依据。