锕系金属团簇内嵌富勒烯的合成，团簇结构与磁性研究

Actinide metallic endohedral fullerenes are novel fullerene compound. Our recent study on these compounds showed that fullerene cage are capable of catching and stabilizing novel actinide metallic clusters, containing actinide metallic bonds which haven’t been obtained via conventional actinide synthetic methods. On the other hand, the encapsulated actinide metal can stabilize novel fullerene cages which has never been observed before. These research results revealed that this family of compounds resemble neither conventional fullerene compound nor conventional actinide compound and have unique molecular structures and physiochemical properties. The in-depth research on these compound will bring new understanding into both fullerene formation mechanism and actinide chemical bond, which are significant for both fullerene chemistry and actinide chemistry research. Thus, the overall goal of the present proposal is to synthesize a series of novel actinide cluster fullerenes and carry a systematic study on their molecular structure, bonding character and molecular magnetism. This project will focus on fundamental scientific questions such as the structure and bonding motif of the novel actinide clusters which were stabilized only by fullerene cages , the correlation between the unique structure of actinide clusters and the molecular magnetism. This project aims at the ‘exploring the novel clusters’ and ‘understanding the structure and the function of clusters’, which are main objectives of the key project. The successful implementation of this project will also establish theoretical foundation for potential application of fullerene cluster materials on biomedicine, magnetic materials and nuclear sciences.

锕系金属内嵌富勒烯是一类新型的富勒烯化合物。我们对这类化合物的初步研究表明，富勒烯碳笼可捕获并稳定新型锕系金属团簇，团簇中包含通过传统锕系合成化学中尚无法获得的锕系化学键，而锕系金属也可稳定此前无法获得的新结构富勒烯团簇。此类团簇化合物不同于传统的富勒烯与锕系化合物，具有独特的团簇结构和物化性质，对其深入研究可能带来对富勒烯形成机理和锕系化学键的新的认知。基于此，本项目拟合成一系列新型锕系金属团簇内嵌富勒烯，对其团簇结构，价键和分子磁性进行系统研究。重点探讨这些新结构的锕系金属团簇与富勒烯团簇的相互稳定机理，深入研究锕系金属团簇的价键结构，团簇结构与分子磁性的关联等关键科学问题。本项目聚焦于重大项目提出的‘发展新型团簇’以及‘理解团簇结构与功能’的总体目标，其成功实施也将为该富勒烯团簇材料在生物医学，磁性材料和核材料方面的潜在应用奠定理论基础。

锕系金属内嵌富勒烯是一类新型的富勒烯化合物。此类团簇化合物不同于传统的富勒烯与锕系化合物，具有独特的团簇结构和物化性质，对其深入研究可能带来对富勒烯形成机理和锕系化学键的新的认知。基于此，本项目深入研究锕系金属团簇的价键结构，团簇结构与分子磁性的关联等关键科学问题，取得了系列研究成果：合成获得了U2C@C2n，U2N@C80, UCN@C82, UN@C82, Th2@C80，ThC2@C82等一系列新型锕系金属团簇富勒烯，并对其团簇结构，价键和分子磁性进行系统研究。研究表明，内嵌的锕系金属团簇具有独特的价键结构，U，Th在内嵌的金属团簇中均显示出特殊的配位行为。揭示了在碳笼的限域化学环境下，U与CN，Th与C2形成的罕见的三角形团簇和η2配位结构。发现了富勒烯碳笼内的配位环境能够有效的稳定UN团簇等含有特殊锕系金属多重键的价键结构。在国际上率先获得了含有Th-Th金属键的分子化合物Th2@C80，并研究了其电子结构与分子磁性之间的相互关系。本项目聚焦于重大项目提出的‘发展新型团簇’以及‘理解团簇结构与功能’的总体目标，揭示了富勒烯团簇与锕系金属团簇相互稳定的机理，并发现了这一作用能够有效的稳定目前在分子化合物中尚难以获得锕系金属多重键和锕系金属键，这一系列研究成果为富勒烯与锕系金属团簇研究提供了新的思路。

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