Journal
INORGANIC CHEMISTRY
Volume 57, Issue 21, Pages 13513-13523Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.8b02126
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Funding
- Science Challenge Project [TZ2016004]
- National Natural Science Foundation of China [21671191, 21577144, 11405186]
- Major Program of National Natural Science Foundation of China [21790373]
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As an emerging type of actinide hybrid material, uranyl rotaxane coordination polymers (URCPs) with new coordination patterns and topological structures are still desired. In this work, we propose a new strategy to construct URCPs by promoting the simultaneous coordination of both the wheel and axle moieties in pseudorotaxane linkers with metal nodes. Starting from a series of cucurbit[6]uril (CB[6])based pseudorotaxane ligands, CnBPCA@CB[6] [CnBPCA = 1,1-(alpha,omega-diyObis[4-(ethoxycarbonyl)pyridin-1-ium] bromides, where n = 5-8] with slightly deformed CB[6], four new URCPs (URCP1, URCP3, URCP4, and URCPS) with interwoven network structures, as well as another noninterwoven polymer(URCP2), have been successfully prepared. According to single-crystal structure analysis, we attribute the interwoven structures of the URCPs to the distortion of CB[6] in pseudorotaxane ligands with shorter or longer spacers (CS, C7, and C8). This indicates that the deformation could effectively diminish the steric hindrance around the portals, thus endowing the inert CB[6] host with coordination ability like the string molecule. Besides, the participation of water molecules and sulfate anions in the uranyl coordination sphere is also found to have a great influence on the final structures of the obtained URCPs. The successful preparation of interwoven URCPs in this work gives some new insights into the metal coordination of supramolecular entities and could facilitate other new applications of CB[6]-based pseudorotaxane ligands. Most importantly, the strategy proposed in this work provides some hints in the controllable design of metal organic rotaxane frameworks with unique topologies.
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