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Peer-reviewedCC BYACS macro letters

Dynamic Covalent Lewis Pair Grafting Enables Spontaneous Linear-to-Bottlebrush Polymer Assembly and Adaptive Elastomers.

  • Edip Ajvazi1
  • Verena Schinegger1,2
  • Milan Kracalik3
  • Oliver Brüggemann1
  • Ingrid Graz2,4
  • Uwe Monkowius5,2
  • Ian Teasdale1
5 affiliations
  1. 1Institute of Polymer Chemistry, Johannes Kepler University Linz, Altenberger Straße 69, 4040Linz, Austria.
  2. 2School of Education, STEM Education, Johannes Kepler University Linz, Altenberger Straße 69, 4040Linz, Austria.
  3. 3Institute of Polymer Science, Johannes Kepler University Linz, Altenberger Straße 69, 4040Linz, Austria.
  4. 4Institute of Biophysics, Life Science Center, Johannes Kepler Universität Linz, Gruberstrasse 40, 4020Linz, Austria.
  5. 5Institute of Inorganic Chemistry, Johannes Kepler University Linz, Altenberger Straße 69, 4040Linz, Austria.
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Abstract

Bottlebrush and comb-graft polymers, macromolecules with densely grafted side chains along a central backbone, exhibit distinctive conformational, rheological, and self-assembly behaviors. Although these architectures are widely used to tune mechanical responses, most reported systems rely on stable covalent carbon frameworks, or fragile supramolecular assemblies, while dynamic covalent chemistries remain largely unexplored. Herein, we harness Lewis acid-base pairs whose directional coordinate bonds drive the spontaneous assembly of graft architectures by simply mixing Lewis acid-terminated polydimethylsiloxane (PDMS) oligomers with the polymeric Lewis base poly(4-vinylpyridine) (P4VP). The PDMS-oligomers efficiently graft to the P4VP backbone. 11B and 1H NMR studies revealing a dynamic-covalent equilibrium, with rapid kinetics. Upon addition of a difunctional boronate cross-linker, the dynamically grafted polymers form stretchable elastomeric networks that can be thermally reprocessed and undergo autonomous self-healing. This Lewis-pair strategy expands bottlebrush polymer chemistry beyond static covalent and fragile supramolecular designs, with a simple, tunable route to recyclable covalent adaptable networks of soft and elastic materials.

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Cite

BibTeXRIS
BibTeX
@article{ajvazi2026dynamic,
  title = {{Dynamic Covalent Lewis Pair Grafting Enables Spontaneous Linear-to-Bottlebrush Polymer Assembly and Adaptive Elastomers.}},
  author = {Edip Ajvazi and Verena Schinegger and Milan Kracalik and Oliver Brüggemann and Ingrid Graz and Uwe Monkowius and Ian Teasdale},
  journal = {ACS macro letters},
  year = {2026},
  month = oct,
  doi = {10.1021/acsmacrolett.6c00433},
  url = {https://europepmc.org/article/MED/42899739},
  note = {CC BY},
}
RIS
TY  - JOUR
TI  - Dynamic Covalent Lewis Pair Grafting Enables Spontaneous Linear-to-Bottlebrush Polymer Assembly and Adaptive Elastomers.
AU  - Edip Ajvazi
AU  - Verena Schinegger
AU  - Milan Kracalik
AU  - Oliver Brüggemann
AU  - Ingrid Graz
AU  - Uwe Monkowius
AU  - Ian Teasdale
PY  - 2026
DA  - 2026/10/01
JO  - ACS macro letters
DO  - 10.1021/acsmacrolett.6c00433
UR  - https://europepmc.org/article/MED/42899739
AB  - Bottlebrush and comb-graft polymers, macromolecules with densely grafted side chains along a central backbone, exhibit distinctive conformational, rheological, and self-assembly behaviors. Although these architectures are widely used to tune mechanical responses, most reported systems rely on stable covalent carbon frameworks, or fragile supramolecular assemblies, while dynamic covalent chemistries remain largely unexplored. Herein, we harness Lewis acid-base pairs whose directional coordinate bonds drive the spontaneous assembly of graft architectures by simply mixing Lewis acid-terminated polydimethylsiloxane (PDMS) oligomers with the polymeric Lewis base poly(4-vinylpyridine) (P4VP). The PDMS-oligomers efficiently graft to the P4VP backbone. 11B and 1H NMR studies revealing a dynamic-covalent equilibrium, with rapid kinetics. Upon addition of a difunctional boronate cross-linker, the dynamically grafted polymers form stretchable elastomeric networks that can be thermally reprocessed and undergo autonomous self-healing. This Lewis-pair strategy expands bottlebrush polymer chemistry beyond static covalent and fragile supramolecular designs, with a simple, tunable route to recyclable covalent adaptable networks of soft and elastic materials.
SN  - 2161-1653
ER  -