Solution-processable and functionalizable ultra-high molecular weight polymers via topochemical synthesis

Christopher L. Anderson, He Li, Christopher G. Jones, Simon J. Teat, Nicholas S. Settineri, Eric A. Dailing, Jiatao Liang, Haiyan Mao, Chongqing Yang, Liana M. Klivansky, Xinle Li, Jeffrey A. Reimer, Hosea M. Nelson () and Yi Liu ()
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Christopher L. Anderson: Lawrence Berkeley National Laboratory
He Li: Lawrence Berkeley National Laboratory
Christopher G. Jones: University of California, Los Angeles
Simon J. Teat: Lawrence Berkeley National Laboratory
Nicholas S. Settineri: University of California, Berkeley
Eric A. Dailing: Lawrence Berkeley National Laboratory
Jiatao Liang: Lawrence Berkeley National Laboratory
Haiyan Mao: University of California, Berkeley
Chongqing Yang: Lawrence Berkeley National Laboratory
Liana M. Klivansky: Lawrence Berkeley National Laboratory
Xinle Li: Lawrence Berkeley National Laboratory
Jeffrey A. Reimer: University of California, Berkeley
Hosea M. Nelson: University of California, Los Angeles
Yi Liu: Lawrence Berkeley National Laboratory

Nature Communications, 2021, vol. 12, issue 1, 1-8

Abstract: Abstract Topochemical polymerization reactions hold the promise of producing ultra-high molecular weight crystalline polymers. However, the totality of topochemical polymerization reactions has failed to produce ultra-high molecular weight polymers that are both soluble and display variable functionality, which are restrained by the crystal-packing and reactivity requirements on their respective monomers in the solid state. Herein, we demonstrate the topochemical polymerization reaction of a family of para-azaquinodimethane compounds that undergo facile visible light and thermally initiated polymerization in the solid state, allowing for the first determination of a topochemical polymer crystal structure resolved via the cryoelectron microscopy technique of microcrystal electron diffraction. The topochemical polymerization reaction also displays excellent functional group tolerance, accommodating both solubilizing side chains and reactive groups that allow for post-polymerization functionalization. The thus-produced soluble ultra-high molecular weight polymers display superior capacitive energy storage properties. This study overcomes several synthetic and characterization challenges amongst topochemical polymerization reactions, representing a critical step toward their broader application.

Date: 2021
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DOI: 10.1038/s41467-021-27090-1

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