TY - JOUR
T1 - Polymer architecture dictates multiple relaxation processes in soft networks with two orthogonal dynamic bonds
AU - Ge, Sirui
AU - Tsao, Yu Hsuan
AU - Evans, Christopher M.
N1 - The authors gratefully acknowledge support from the Air Force Office of Scientific Research (AFOSR) under support provided by the Organic Materials Chemistry Program (grant FA9550-20-1-0262 to S.G. and C.M.E.). Portions of the work were also supported by the National Science Foundation through award CBET-2029928 (X-ray scattering of vitrimers, to Y.T. and C.M.E.). Aspects of this work were performed at the Materials Research Laboratory and School of Chemical Sciences facilities in UIUC.
The authors gratefully acknowledge support from the Air Force Office of Scientific Research (AFOSR) under support provided by the Organic Materials Chemistry Program (grant FA9550-20-1-0262 to S.G. and C.M.E.). Portions of the work were also supported by the National Science Foundation through award CBET-2029928 (X-ray scattering of vitrimers, to Y.T. and C.M.E.). Aspects of this work were performed at the Materials Research Laboratory and School of Chemical Sciences facilities in UIUC.
PY - 2023/12
Y1 - 2023/12
N2 - 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.
AB - 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.
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U2 - 10.1038/s41467-023-43073-w
DO - 10.1038/s41467-023-43073-w
M3 - Article
C2 - 37945556
AN - SCOPUS:85176150889
SN - 2041-1723
VL - 14
JO - Nature communications
JF - Nature communications
IS - 1
M1 - 7244
ER -