Polymer architecture dictates multiple relaxation processes in soft networks with two orthogonal dynamic bonds

Abstract

Materials with tunable modulus, viscosity, and complex viscoelastic spectra are crucial in applications such as self-healing, additive manufacturing, and energy damping. It is still challenging to predictively design polymer networks with hierarchical relaxation processes, as many competing factors affect dynamics. Here, networks with both pendant and telechelic architecture are synthesized with mixed orthogonal dynamic bonds to understand how the network connectivity and bond exchange mechanisms govern the overall relaxation spectrum. A hydrogen-bonding group and a vitrimeric dynamic crosslinker are combined into the same network, and multimodal relaxation is observed in both pendant and telechelic networks. This is in stark contrast to similar networks where two dynamic bonds share the same exchange mechanism. With the incorporation of orthogonal dynamic bonds, the mixed network also demonstrates excellent damping and improved mechanical properties. In addition, two relaxation processes arise when only hydrogen-bond exchange is present, and both modes are retained in the mixed dynamic networks. This work provides molecular insights for the predictive design of hierarchical dynamics in soft materials.

Document Details

Document Type
Pub Defense Publication
Publication Date
Nov 09, 2023
Source ID
10.1038/s41467-023-43073-w

Entities

People

  • Christopher M Evans
  • Sirui Ge
  • Yu-hsuan Tsao

Organizations

  • Air Force Office of Scientific Research
  • National Science Foundation

Tags

Readers

  • Computational Modeling and Simulation
  • Materials Science and Engineering.
  • Quantum Chemistry