Predictive design of vip-responsive frameworks on the molecular level is still a major challenge for experimental and theoretical chemists.The isoreticular approach is one of the most promising approaches for design...Predictive design of vip-responsive frameworks on the molecular level is still a major challenge for experimental and theoretical chemists.The isoreticular approach is one of the most promising approaches for designing MOFs with desired textural properties and framework topology.In this work we successfully applied the isoreticular approach for the design of the new flexible frameworks DUT-180 and DUT-190,constructed by square planar or octahedral metal nodes and a tetracarboxylate ligand.The flexibility mechanism in DUT-190 was explored using in situ PXRD and NMR in parallel to physisorption of subcritical gases such as nitrogen(77 K),carbon dioxide(195 K)and xenon(206 K).Methane physisorption experiments,conducted in a broad temperature range indicate a softening of the DUT-190 framework compared to its analogue DUT-13.These experimental and computational findings can be used as a roadmap for discovery of new flexible frameworks with desired micromechanical properties.展开更多
基金the European Research Council(ERC)under the European Union’s Horizon 2020 research and innovation program(grant agreement No.742743)support by the Federal Ministry of Education and Research(Project TIMESWITCH No 05K21OD1)support by the Graduate Academy of the Technical University Dresden.E.B.and S.K.gratefully acknowledge financial support from DFG(FOR 2433).
文摘Predictive design of vip-responsive frameworks on the molecular level is still a major challenge for experimental and theoretical chemists.The isoreticular approach is one of the most promising approaches for designing MOFs with desired textural properties and framework topology.In this work we successfully applied the isoreticular approach for the design of the new flexible frameworks DUT-180 and DUT-190,constructed by square planar or octahedral metal nodes and a tetracarboxylate ligand.The flexibility mechanism in DUT-190 was explored using in situ PXRD and NMR in parallel to physisorption of subcritical gases such as nitrogen(77 K),carbon dioxide(195 K)and xenon(206 K).Methane physisorption experiments,conducted in a broad temperature range indicate a softening of the DUT-190 framework compared to its analogue DUT-13.These experimental and computational findings can be used as a roadmap for discovery of new flexible frameworks with desired micromechanical properties.
