CAJ | 학술논문

采用密度泛函理论(DFT)中的广义梯度近似(GGA)方法对C_(56)X_(10)(X=F,Cl,Br,I)的结构稳定性和电子性质进行了计算研究.结构稳定性计算表明:对于C_(56)X_(10)(X=F,Cl,Br,I),能隙、反应热、最大振动频率和最小振动频率都随着X原子序数的增加而减小,表明C_(56)X_(10)(X=F,Cl,Br,I)的稳定性随着X原子序数的增加而逐渐降低,其中C_(56)F_(10)最为稳定.前人在实验上已成功合成出C_(56)Cl_(10),因此,我们推测C_(56)F_(10)有望在实验上成功合成.前线轨道计算发现,C_(56)相邻的五边形公共顶点以及两个六边形-五边形-六边形公共顶点是笼子中化学活性最强的部位,有利于卤族元素的外部吸附.此外,计算结果还显示,C_(56)X_(10)(X=F,Cl,Br,I)的电负性随着X原子序数的增大而逐渐减弱,C-X基团的电负性因位置的不同而不同.
채용밀도범함이론(DFT)중적엄의제도근사(GGA)방법대C_(56)X_(10)(X=F,Cl,Br,I)적결구은정성화전자성질진행료계산연구.결구은정성계산표명:대우C_(56)X_(10)(X=F,Cl,Br,I),능극、반응열、최대진동빈솔화최소진동빈솔도수착X원자서수적증가이감소,표명C_(56)X_(10)(X=F,Cl,Br,I)적은정성수착X원자서수적증가이축점강저,기중C_(56)F_(10)최위은정.전인재실험상이성공합성출C_(56)Cl_(10),인차,아문추측C_(56)F_(10)유망재실험상성공합성.전선궤도계산발현,C_(56)상린적오변형공공정점이급량개륙변형-오변형-륙변형공공정점시롱자중화학활성최강적부위,유리우서족원소적외부흡부.차외,계산결과환현시,C_(56)X_(10)(X=F,Cl,Br,I)적전부성수착X원자서수적증대이축점감약,C-X기단적전부성인위치적불동이불동.
The generalized gradient approximation (GGA) method based on density functional theory (DFT) was used to analyze the structural stability and electronic properties of the unconventional carbon halogen fullerenes C_(56)X_(10)(X=F, Cl, Br, I). The investigation of structural stability indicates that the evolution of energy gaps, the reactive heat (△E), the maximal vibration frequencies, and the minimal vibration frequencies of C_(56)X_(10)(X=F, Cl, Br, I) all decrease with an increase in the atomic number of X. This indicates that the stabilities should decrease from C_(56)F_(10) to C_(56)I_(10). C_(56)F_(10) is the most stable molecule among the four molecules and we predict that it can be isolated and synthesized because of the successful isolation of C_(56)Cl_(10). From the analysis of the frontier orbitals of C_(56) and C_(56)X_(10)(X=F, Cl, Br, I), the C atoms axe located at the abutting pentagon sites and both the hexagon-hexagon-pentagon vertex functions are the most active sites on C_(56) and this is suitable for halogen atom attachment. Our calculations also show that the electronegativity of C_(56)X_(10)(X=F, Cl, Br, I) cluster molecules decrease with an increase in the atomic number of X. However, the electronegativity of the C-X fragment in the molecules is affected by its location.