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| Applying reticular synthesis to the design of Cu-based MOFs with mechanically interlocked linkers | |
| 作者姓名： | Alexander J.Stirk Benjamin H.Wilson Christopher A.O’Keefe Hazem Amame Kelong Zhu Robert W.Schurko Stephen J.Loeb |
| 作者单位： | Department of Chemistry and Biochemistry;Department of Chemistry;School of Chemistry;Department of Chemistry and Biochemistry |
| 基金项目： | S.J.L.acknowledges the Natural Sciences and Engineering Research Council of Canada for support of a Discovery Grant(101694)and a Canada Research Chair.R.W.S.is also grateful for support from NSERC,the Canadian Foundation for Innovation,the Ontario Innovation Trust,the University of Windsor for the development and maintenance of the SSNMR centre,and for funding from the Florida State University and the National High Magnetic Field Laboratory(NHMFL),which is funded by the National Science Foundation Cooperative Agreement(DM R-1644779)and by the State of Florida.The authors acknowledge M.Revington for technical assistance with solution NM Rspectroscopy and J.Auld for technical assistance with high resolution mass spectrometry. |
| 摘 要： | The concept of“robust dynamics”describes the incorporation of mechanically interlocked molecules(MIMs)into metal-organic framework(MOF)materials such that large amplitude motions(e.g.,rotation or translation of a macrocycle)can occur inside the free volume pore of the MOF.To aid in the preparation of such materials,reticular synthesis was used herein to design rigid molecular building blocks with predetermined ordered structures starting from the well-known MOF NOTT-101.New linkers were synthesized that have a T-shape,based on a triphenylene tetra-carboxylate strut,and their incorporation into Cu(II)-based MOFs was investigated.The single-crystal structures of three new MOFs,UWCM-12(fof),β-UWCM-13(loz),UWCM-14(lil),with naked T-shaped linkers were determined;β-UWCM-13 is the first reported example of the loz topology.A fourth MOF,UWDM-14(lil)is analogous to UWCM-14(lil)but contains a2]rotaxane linker.Variable-temperature,2H solid-state NMR was used to probe the dynamics of a 24-membered macrocycle threaded onto the MOF skeleton. |
| 关 键 词： | reticular chemistry metal-organic frameworks mechanically interlocked molecules ROTAXANE |
Applying reticular synthesis to the design of Cu-based MOFs with mechanically interlocked linkers |
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| Stirk,Alexander J.,Wilson,Benjamin H.,O’Keefe,Christopher A.,Amarne,Hazem,Zhu,Kelong,Schurko,Robert W.,Loeb,Stephen J..Applying reticular synthesis to the design of Cu-based MOFs with mechanically interlocked linkers[J].Nano Research,2021,14(2):417-422. | |
| Authors: | Stirk Alexander J Wilson Benjamin H O’Keefe Christopher A Amarne Hazem Zhu Kelong Schurko Robert W Loeb Stephen J |
| Affiliation: | 1.Department of Chemistry and Biochemistry, University of Windsor, Windsor, Ontario, N9B 3B4, Canada ;2.Department of Chemistry, The University of Jordan, Amman, 11942, Jordan ;3.School of Chemistry, Sun Yat-Sen University, Guangzhou, 510275, China ;4.Department of Chemistry and Biochemistry, Florida State University, Tallahassee, Florida, 32306-4390, USA ; |
| Abstract: | The concept of “robust dynamics” describes the incorporation of mechanically interlocked molecules (MIMs) into metal-organic framework (MOF) materials such that large amplitude motions (e.g., rotation or translation of a macrocycle) can occur inside the free volume pore of the MOF. To aid in the preparation of such materials, reticular synthesis was used herein to design rigid molecular building blocks with predetermined ordered structures starting from the well-known MOF NOTT-101. New linkers were synthesized that have a T-shape, based on a triphenylene tetra-carboxylate strut, and their incorporation into Cu(II)-based MOFs was investigated. The single-crystal structures of three new MOFs, UWCM-12 (fof), β-UWCM-13 (loz), UWCM-14 (lil), with naked T-shaped linkers were determined; β-UWCM-13 is the first reported example of the loz topology. A fourth MOF, UWDM-14 (lil) is analogous to UWCM-14 (lil) but contains a 2]rotaxane linker. Variable-temperature, 2H solid-state NMR was used to probe the dynamics of a 24-membered macrocycle threaded onto the MOF skeleton.  |
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