Polycyclic aromatic hydrocarbons(PAHs)play an important role in the industry,and the development of new materials for the selective separation of PAHs is of great significance.In this work,we report a hexahedral metal...Polycyclic aromatic hydrocarbons(PAHs)play an important role in the industry,and the development of new materials for the selective separation of PAHs is of great significance.In this work,we report a hexahedral metal-organic cage with low symmetry by subcomponent self-assembly.In this cage,the eight ZnII centers adopt an interestin∧∧/△△△△△△or∧∧∧∧∧∧/△△configuration.This cage with a cavity volume of 520˚A3 can bind anthracene,phenanthrene,and pyrene to form 1:1 host-guest complexes,while the bigger triphenylene,chrysene,perylene,and coronene cannot be encapsulated.The binding constant Ka of pyrene is about 1.110×10^(3)(mol/L)^(−1),which is more than an order of magnitude larger than that of anthracene and phenanthrene(111(mol/L)^(−1),277(mol/L)^(−1),respectively).X-ray structure studies reveal that the pyrene is located in the cavity and stabilized by multiple C–H…πinteractions.After separation from a mixture of PAHs,pyrene with>96.1%purity can be obtained.This work provides a useful method for the first time for the selective separation of pyrene from PAHs mixture by utilizing a metal-organic cage as the material,making it a useful tool for purifying and separating specific compounds from complex mixtures.展开更多
基金the National Natural Science Foundation of China(Nos.22171106,21731002,21975104,21871172 and 22201101)the Guangdong Major Project of Basic and Applied Research(No.2019B030302009)+3 种基金Guangdong Natural Science Foundation(No.2022A1515011937)the Guangzhou Science and Technology Program(No.202002030411)the Fundamental Research Funds for the Central Universities(No.21622103)the China Postdoctoral Science Foundation(No.2022M711327),and Jinan University.
文摘Polycyclic aromatic hydrocarbons(PAHs)play an important role in the industry,and the development of new materials for the selective separation of PAHs is of great significance.In this work,we report a hexahedral metal-organic cage with low symmetry by subcomponent self-assembly.In this cage,the eight ZnII centers adopt an interestin∧∧/△△△△△△or∧∧∧∧∧∧/△△configuration.This cage with a cavity volume of 520˚A3 can bind anthracene,phenanthrene,and pyrene to form 1:1 host-guest complexes,while the bigger triphenylene,chrysene,perylene,and coronene cannot be encapsulated.The binding constant Ka of pyrene is about 1.110×10^(3)(mol/L)^(−1),which is more than an order of magnitude larger than that of anthracene and phenanthrene(111(mol/L)^(−1),277(mol/L)^(−1),respectively).X-ray structure studies reveal that the pyrene is located in the cavity and stabilized by multiple C–H…πinteractions.After separation from a mixture of PAHs,pyrene with>96.1%purity can be obtained.This work provides a useful method for the first time for the selective separation of pyrene from PAHs mixture by utilizing a metal-organic cage as the material,making it a useful tool for purifying and separating specific compounds from complex mixtures.