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Synthesis of Information-bearing Peptoids and their Sequence-directed Dynamic Covalent Self-assembly
Published on: February 6, 2020
Spontaneous Long-Range Order and Alignment in Phase-Separated Dynamic Covalent Networks Using Discrete Siloxanes
Stefan J D Maessen1, Tymen M L van der Leede1, Anne B Spoelstra2
1Department of Chemical Engineering & Chemistry and Institute for Complex Molecular Systems, Eindhoven University of Technology, Eindhoven, the Netherlands.
Angewandte Chemie (International Ed. in English)
|July 31, 2026
Summary
Researchers created dynamic covalent networks with spontaneous hexagonal ordering using siloxane linkers. This self-assembly improves mechanical properties and simplifies actuator fabrication.
Area of Science:
- Materials Science
- Polymer Chemistry
- Supramolecular Chemistry
Background:
- Dynamic covalent networks (DCNs) offer tunable properties but achieving long-range order remains challenging.
- Hydrogen bonding interactions are key in directing network self-assembly.
- Controlling network architecture is crucial for advanced material functionalities.
Purpose of the Study:
- To develop DCNs exhibiting spontaneous alignment and hexagonal columnar ordering.
- To investigate the role of siloxane linkers in network self-assembly.
- To enhance the (thermo)mechanical properties and dynamics of DCNs.
Main Methods:
- Preparation of DCNs using discrete siloxane linkers and acylsemicarbazide bonds.
- Solvent evaporation technique for inducing network ordering and homeotropic alignment.
- Characterization using transmission electron microscopy (TEM) and grazing incidence small-angle X-ray scattering (GISAXS).
Main Results:
- Achieved spontaneous alignment and long-range hexagonal columnar ordering in DCNs.
- Demonstrated the critical role of discrete siloxane linker length in achieving order.
- Observed improved (thermo)mechanical properties, enhanced creep resistance, and slower dynamics in ordered networks.
Conclusions:
- Discrete siloxane linkers enable self-assembly of ordered DCNs via phase separation and hydrogen bonding.
- Simple solvent evaporation facilitates near-perfect homeotropic alignment.
- Ordered DCNs exhibit superior properties and enable simplified fabrication of actuators.
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