大碳笼内嵌钆氧化物团簇金属富勒烯Gd_2O@C_(88):实验和理论研究

High-carbon cage encasing gadolinium oxide cluster metallofulerene Gd_2O@C_(88):an experimental and theoretical study

利用改进的电弧放电技术合成及多步高效液相色谱(HPLC)分离方法,得到了大碳笼含钆氧化物团簇的金属富勒烯Gd_2O@C_(88).激光解吸电离碰撞诱导解离质谱/质谱的研究结果表明,氧化钆团簇位于碳笼内部.密度泛函理论计算结果表明,金属富勒烯结构为Gd_2O@D_2(35)-C_(88).内嵌团簇向碳笼转移4个电子,价态+4,碳笼-4价,金属富勒烯的电子结构表示为[Gd_2O]^(4+)@[D_2(35)-C_(88)]^(4-).

The metallofullerene Gd_2O@C_（88） with Gd_2O cluster encased in the high carbon cage C_（88） was synthesized using arc discharging and isolated to isomer pure by the multi-step HPLC method.Laser desorption ionization collisional induced dissociation MS/MS indicated the Gd_2O cluster was located inside the carbon cage.Density functional theory computation suggests that the whole structure can be depicted as Gd_2O@D_2（35）-C_（88） and a further electronic population representation[Gd_2O]^（4＋）@[D_2（35）-C_（88）]^（4-）,with 4electrons transferred from the encased cluster to the carbon cage.So the inside cluster shows ＋4valent,while the carbon cage-4.