论文部分内容阅读
两个金属硫化物富勒烯Sc2S@C82-Cs(6)和Sc2S@C82-C3v(8)的结构已经通过单晶X射线衍射验证,但对于其形成机理却知之甚少.本文通过密度泛函理论方法计算研究了Sc2S@C82的不同异构体的热力学和动力学稳定性.结合封闭网络增长模型,研究了Sc2S@C82的形成机理.计算表明,该金属富勒烯是在Sc2S@C80-D5h(31923)的基础上通过C2增长而来,且增长路径是通过中间体Sc2S@C82-Cs(39704)而不是通常认为的Sc2S@C82-Cs(39663);此外,证实了异构体Sc2S@C82-Cs(6)和Sc2S@C82-C3v(8)的相互转化是一个可逆过程;碳催化的Stone-Wales旋转可以大大降低反应的能垒.这些结果对其他金属富勒烯的形成机理具有参考意义.
The structures of the two metal-sulfide fullerenes Sc2S @ C82-Cs (6) and Sc2S @ C82-C3v (8) have been verified by single crystal X-ray diffraction but little is known about their formation mechanism. Functional theory method was used to study the thermodynamic and kinetic stability of different isomers of Sc2S @ C82. The formation mechanism of Sc2S @ C82 was studied in combination with the closed network growth model. The calculations show that the metal fullerenes are stable in Sc2S @ C80 -D5h (31923), and the growth pathway is through the intermediate Sc2S @ C82-Cs (39704) rather than Sc2S @ C82-Cs (39663), which is generally recognized; in addition, it was confirmed that isomers The interconversion of Sc2S @ C82-Cs (6) to Sc2S @ C82-C3v (8) is a reversible process; the carbon-catalyzed Stone-Wales rotation can greatly reduce the energy barrier of the reaction.These results suggest the formation of other metal fullerenes Mechanism has reference value.