Rapid synthesis of metal–organic frameworks(MOFs),especially high-valence MOFs at roomtemperature without external energy,is a challenging topic.In this work,a stable radical solution has been discovered.Various MOFs...Rapid synthesis of metal–organic frameworks(MOFs),especially high-valence MOFs at roomtemperature without external energy,is a challenging topic.In this work,a stable radical solution has been discovered.Various MOFs with versatile metal nodes and ligands were rapidly synthesized at room temperature in the absence of external energy.Especially,MOFs with conjugated ligands achieved instantaneous architecture(in less than 1 s)and quantitative yield.Radicals in the solution play a crucial role in the accelerated kinetics,and the new radical route paves a cyclic pathway for the MOF synthesis.The mechanism has been thoroughly investigated by electron paramagnetic resonance,in situ proton nuclear magnetic resonance,X-ray absorption spectra,in situ small-angle X-ray scattering-wide-angle X-ray scattering,and density functional theory calculations.展开更多
基金The authors thank the National Natural Science Foundation of China(grant no.22073104)the Beijing Natural Science Foundation(grant no.2222043)+3 种基金the National Key Research and Development Program of China(grant nos.2017YFA0403101,2017YFA0403003,and 2017YFA0403102)the National Natural Science Foundation of China(grant nos.21890761,21733011,and 21533011)the Beijing Municipal Science&Technology Commission(grant no.Z191100007219009)the Chinese Academy of Sciences(grant no.QYZDY-SSWSLH013).The XAS(1W1B)and SAXS(1W2A)measurements were performed at the Beijing Synchrotron Radiation Facility,China.
文摘Rapid synthesis of metal–organic frameworks(MOFs),especially high-valence MOFs at roomtemperature without external energy,is a challenging topic.In this work,a stable radical solution has been discovered.Various MOFs with versatile metal nodes and ligands were rapidly synthesized at room temperature in the absence of external energy.Especially,MOFs with conjugated ligands achieved instantaneous architecture(in less than 1 s)and quantitative yield.Radicals in the solution play a crucial role in the accelerated kinetics,and the new radical route paves a cyclic pathway for the MOF synthesis.The mechanism has been thoroughly investigated by electron paramagnetic resonance,in situ proton nuclear magnetic resonance,X-ray absorption spectra,in situ small-angle X-ray scattering-wide-angle X-ray scattering,and density functional theory calculations.
