Polymers with low ceiling temperatures (Tc) are highly desirable as they can depolymerize under mild conditions, but they typically suffer from demanding synthetic conditions and poor stability. We envision that this challenge can be addressed by developing high-Tc polymers that can be converted into low-Tc polymers on demand. Here, we demonstrate the mechanochemical generation of a low-Tc polymer, poly(2,5-dihydrofuran) (PDHF), from an unsaturated polyether that contains cyclobutane-fused THF in each repeat unit. Upon mechanically induced cycloreversion of cyclobutane, each repeat unit generates three repeat units of PDHF. The resulting PDHF completely depolymerizes into 2,5-dihydrofuran in the presence of a ruthenium catalyst. The mechanochemical generation of the otherwise difficult-to-synthesize PDHF highlights the power of polymer mechanochemistry in accessing elusive structures. The concept of mechanochemically regulating the Tc of polymers can be applied to develop next-generation sustainable plastics.
A new analog of 1,3-bis(pyridylimino)isoindoline with bridging CCN groups can be produced via a one-step reaction. This ligand can bind metal ions and exhibits significantly red shifted absorption properties.
Transition metal-catalyzed copolymerization of CO and ethylene has a strong inherent propensity to produce the strictly alternating copolymer. In this work, nickel catalysts capable of both homopolymerization of ethylene and alternating copolymerization of CO and ethylene are developed to explore the possibility of non-alternating copolymerization of CO and ethylene under the assumption that comonomer incorporation in the polymer chain can be adjusted by the concentrations of the comonomers. Both polyketones with slightly more than 50 % ethylene and "polyethylenes" with a small amount of CO incorporation are obtained but only under carefully controlled conditions and in low yields.
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