MOF-177对金属富勒烯的吸附选择性研究  

Research for adsorption selectivity of MOF-177 to metallofullerenes

作　　者：张玉荣 张捷 余春燕[2] 贾伟[2] 张竹霞[3,4] 崔鹏 ZHANG Yu-rong;ZHANG Jie;YU Chun-yan;JIA Wei;ZHANG Zhu-xia;CUI Peng(Shanxi Economic and Trade School,Taiyuan 030000,China;Key Laboratory of Interface Science and Engineering in Advanced Materials,Taiyuan University of Technology,Taiyuan 030024,China;College of Aeronautics and Astronautics,Taiyuan University of Technology,Taiyuan 030024,China;Key Laboratory of Magnetic Molecules and Magnetic Information Materials,Ministry of Eduacation,Linfen 041004,China;School of Information,Guizhou University of Finance and Economics,Guiyang 550025,China)

机构地区：[1]山西省经贸学校,山西太原030000 [2]太原理工大学,新材料界面科学与工程教育部重点实验室,山西太原030024 [3]太原理工大学航空航天学院,山西太原030024 [4]磁性分子与磁信息材料教育部重点实验室,山西临汾041004 [5]贵州财经大学信息学院,贵州贵阳550025

出　　处：《分子科学学报》2021年第3期237-242,共6页Journal of Molecular Science

基　　金：固体表面物理化学国家重点实验室(厦门大学)开放课题(201928);山西省自然科学基金资助项项目(201901D111109,201801D121101);山西省重点研发计划(201903D111009);地区科学基金资助项目(21963004)。

摘　　要：采用电弧放电法制备了3种金属富勒烯Sc_(3)N@C_(78)-D3 h,Sc_(3)N@C_(80)-Ih和Sc_(2)_C_(2)@C_(82)-Cs,并用溶剂热法合成了金属-有机骨架材料MOF-177.利用紫外-可见分光光度计和高效液相色谱对甲苯溶液中MOF-177吸附金属富勒烯的过程进行了观察和表征.通过比较其紫外-可见吸光强度和色谱图,发现MOF-177对Sc_(2)_C_(2)@C_(82)的吸附速率最快,结合能力更强.对比计算优化后的3种金属富勒烯的结构图和MOF-177腔体的结构图可以看出,MOF-177与不同尺寸大小和形状的金属富勒烯有着不同的主客体相互作用.Three metallofullerene Sc_(3)N@C_(78)-D3h,Sc_(3)N@C_(80)-Ih and Sc_(2)_C_(2)@C_(82)-Cs were prepared by arc discharge method and the metal-organic framework materials(MOFs)of MOF-177 was synthesized by solvent-thermal method.As a porous crystalline material,MOFs are widely used for adsorption and separation.MOF-177 have aromatic frameworks and large pores(above 1.08 nm),which can effectively adsorb some organic guest molecules and fullerenes.MOF-177 is a porous material whose structure consists of octahedral zinc nitrate hexahydrate(Zn_(4)O(-COO)_(6))and triangular planar aromatic 1,3,5-tri-4-carboxylbenzene(H3BTB)units.MOF-177 have cage-like pores and H3BTB units in two sets of parallel quasi-planar units with a minimum distance of about 1.399 nm.It can be seen that MOF-177 have suitable pore size for metallofullerenes and have been found to adsorb and disperse Sc3C2@C80,DySc2N@C80 and [e-mail],we chose MOF-177 to adsorb Sc_(3)N@C_(78)-D3h,Sc_(3)N@C_(80)-Ih and Sc_(2)_C_(2)@C_(82)-Cs with different carbon cage sizes.Subsequently,the adsorption process of metallofullerenes by MOF-177 in toluene solution was observed and characterized by UV-Vis absorption spectroscopy.By comparing their light absorption intensity,it was found that in the presence of MOF-177 in toluene solution,the absorbance of Sc_(2)_C_(2)@C_(82) has the fastest decrease,and the absorbance of Sc_(3)N@C_(78) and Sc_(3)N@C_(80) have slower decreases.thus MOF-177 has stronger adsorption ability to the Sc_(2)_C_(2)@C_(82).By comparing the structures of the three theoretically optimized metallofullerenes and the MOF-177 cavity,it can be seen that MOF-177 has different host-guest interactions with different sizes and shapes of metallofullerenes.Size will directly affect the adsorption capacity of MOF-177.Fullerene size too large into the MOF channel will be more difficult,too small into the MOF channel is not easy to be captured stably.The shape of the Sc_(2)_C_(2)@C_(82) metallofullerene carbon cage is similar to that of the spindle,which coi

关 键 词：金属富勒烯 金属有机骨架 MOF-177 主客体作用 吸附选择性 

分 类 号：O643[理学—物理化学]