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Poly[n]catenanes: Synthesis of molecular interlocked chains

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Science  30 Nov 2017:
eaap7675
DOI: 10.1126/science.aap7675

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Abstract

As the macromolecular version of mechanically interlocked molecules, mechanically interlocked polymers (MIPs) are intriguing candidates for creation of sophisticated molecular machines and smart soft materials. Poly[n]catenanes, where the molecular chains consist solely of interlocked macrocycles, contain one of the highest concentrations of topological bonds. We report, herein, a synthetic approach toward this unique polymer architecture in high yield (~75%) via efficient ring-closing of rationally-designed metallosupramolecular polymers (MSPs). Light-scattering, mass spectrometric, and nuclear magnetic resonance characterization of fractionated samples support assignment of the high molecular weight product (average Mn = 21.4 kDa) to a mixture of linear poly[7–26]catenanes, branched poly[13–130]catenanes and cyclic poly[4–7]catenanes. Increased hydrodynamic radius (Rh, in solution) and glass transition temperature (Tg, in bulk materials) were observed upon metallation with Zn2+.

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