4.8 Article

An Orthogonal Dynamic Covalent Polymer Network with Distinctive Topology Transformations for Shape- and Molecular Architecture Reconfiguration

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 11, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202109941

Keywords

Bottlebrush Polymer; Orthogonal Dynamic Covalent Bonds; Topological Transformation

Funding

  1. National Natural Science Foundation of China [52033009, 52003232, 21625402]
  2. China National Postdoctoral Program for Innovative Talents [BX20190294]
  3. China Postdoctoral Science Foundation [2020M681821]

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The designed dynamic covalent network can undergo two orthogonal topological transformations, allowing independent control of macroscopic shape and molecular architecture. The network design enables shape reconfigurability and spatially definable mechanical properties of the material.
Bond exchange in a typical dynamic covalent polymer network allows access to macroscopic shape reconfigurability, but the network architecture is not altered. An alternative possibility is that the network architecture can be designed to switch to various topological states corresponding to different material properties. Achieving both in one network can expand the material scope, but their intrinsically conflicting mechanisms make it challenging. We design a dynamic covalent network that can undergo two orthogonal topological transformations, namely transesterification on the branched chains and olefin metathesis on the mainframe. This allows independent control of the macroscopic shape and molecular architecture. With this design, we illustrate a bottlebrush network with programmable shape and spatially definable mechanical properties. Our strategy paves a way to on-demand regulation of network polymers.

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