Author: ["Gaetano Distefano","Hirohito Suzuki","Masahiko Tsujimoto","Seiji Isoda","Silvia Bracco","Angiolina Comotti","Piero Sozzani","Takashi Uemura","Susumu Kitagawa"]
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Abstract
Chain alignment can significantly influence the macroscopic properties of a polymeric material, but no general and versatile methodology has yet been reported to obtain highly ordered crystalline packing of polymer chains, with high stability. Here, we disclose a strategy that relies on ‘ordered crosslinks’ to produce polymeric materials that exhibit a crystalline arrangement. Divinyl crosslinkers (2,5-divinyl-terephthalate) were first embedded, as substitutional ligands, into the structure of a porous coordination polymer (PCP), [Cu(terephthalate)triethylenediamine0.5]n. A representative vinyl monomer, styrene, was subsequently polymerized inside the channels of the host PCP. The polystyrene chains that form within the PCP channels also crosslink with the divinyl species. This bridges together the polymer chains of adjacent channels and ensures that, on selective removal of the PCP, the polymer chains remain aligned. Indeed, the resulting material exhibits long-range order and is stable to thermal and solvent treatments, as demonstrated by X-ray powder diffraction and transmission electron microscopy. A strategy to endow vinyl polymers with pseudo-crystalline order has been devised that relies on host–guest cross-polymerization, through functionalization of the channels of a porous coordination polymer with divinyl moieties. Polymerization of vinyl monomers within the channels is accompanied with lateral crosslinking, which ensures the polymer chains remain highly ordered after removal of the host. Cite this article
Distefano, G., Suzuki, H., Tsujimoto, M. et al. Highly ordered alignment of a vinyl polymer by host–guest cross-polymerization. Nature Chem 5, 335–341 (2013). https://doi.org/10.1038/nchem.1576 