Free-Standing, Single-Monomer-Thick Two-Dimensional Polymers through Covalent Self-Assembly in Solution
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- Free-Standing, Single-Monomer-Thick Two-Dimensional Polymers through Covalent Self-Assembly in Solution
- Kangkyun Baek; Gyeongwon Yun; Kim, Youngkook; Kim, Dongwoo; Hota, Raghunandan; Ilha Hwang; Dan Xu; Young Ho Ko; Gu, Gil Ho; Suh, Ju Hyung; Park, Chan Gyung; Sung, Bong June; Ki Moon Kim
- JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, v.135, no.17, pp.6523 - 6528
- AMER CHEMICAL SOC
- The design and synthesis of two-dimensional
(2D) polymers is a challenging task, hitherto achieved in
solution only through the aid of a solid surface “template” or
preorganization of the building blocks in a 2D con!ned space.
We present a novel approach for synthesizing free-standing,
covalently bonded, single-monomer-thick 2D polymers in
solution without any preorganization of building blocks on
solid surfaces or interfaces by employing shape-directed
covalent self-assembly of rigid, disk-shaped building blocks
having laterally predisposed reactive groups on their periphery. We demonstrate our strategy through a thiol−ene “click” reaction
between (allyloxy)12CB, a cucurbituril (CB) derivative with 12 laterally predisposed reactive alkene groups, and 1,2-
ethanedithiol to synthesize a robust and readily transferable 2D polymer. We can take advantage of the high binding a"nity of
fully protonated spermine (positive charges on both ends) to CB to keep each individual polymer sheet separated from one
another by electrostatic repulsion during synthesis, obtaining, for the !rst-time ever, a single-monomer-thick 2D polymer in
solution. The arrangement of CB repeating units in the resulting 2D polymer has been characterized using gold nanoparticle
labeling and scanning transmission electron microscopy. Furthermore, we have con!rmed the generality of our synthetic
approach by applying it to di#erent monomers to generate 2D polymers. Novel 2D polymers, such as our CB derived
polymer, may be useful in selective transport, controlled drug delivery, and chemical sensing and may even serve as well-de!ned
2D sca#olds for ordered functionalization and platforms for bottom-up 3D construction.
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