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Molecular and kinetic design for the expanded control of molecular weights in ring-opening metathesis polymerization of norbornene-substituted polyhedral oligomeric silsesquioxanes

Abstract

Cube-like polyhedral oligomeric silsesquioxane (POSS) is a promising candidate of isotropically bulky pendants to expand the dimensional limit of polymer main chains. This paper presents molecular and kinetic insights into the controlled synthesis of rod-like POSS-containing polynorbornenes. Ring-opening metathesis polymerization (ROMP) was performed on three norbornene-substituted POSS monomers with different spacers. For monomers possessing non- and amide functionalities at the spacers, ROMP at the maximum concentration ([M]0 = 0.4 M) led to 100% conversion, predictable molecular weights (Mn ≤ 1236 kDa) and low dispersities (Ɖ ≤ 1.20) in homopolymers. Scaling analysis for POSS-containing polynorbornenes revealed an unusual finding, namely, that the periodic clustering of POSS pendants favored by long flex-ible spacers (16-atom chains) enhanced the rigidity of polynorbornene main chains, leading to their rod-like conformation. Kinetically optimized ROMP allowed the subsequent addition of a macromonomer to create POSS-bottlebrush copolymers (POSSBBCPs). These POSSBBCPs self-assembled into thin films to form ordered nanostructures with diverse morphologies and periodicities greater than 100 nm.

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Publication details

The article was received on 12 Jun 2018, accepted on 14 Sep 2018 and first published on 14 Sep 2018


Article type: Paper
DOI: 10.1039/C8PY00870A
Citation: Polym. Chem., 2018, Accepted Manuscript
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    Molecular and kinetic design for the expanded control of molecular weights in ring-opening metathesis polymerization of norbornene-substituted polyhedral oligomeric silsesquioxanes

    C. Chae, Y. Yu, H. Seo, M. Kim, M. Y. L. N. Kishore and J. Lee, Polym. Chem., 2018, Accepted Manuscript , DOI: 10.1039/C8PY00870A

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