Reversibly growing crosslinked polymers with programmable sizes and properties

Xiaozhuang Zhou, Yijun Zheng, Haohui Zhang, Li Yang, Yubo Cui, Baiju P. Krishnan, Shihua Dong, Michael Aizenberg, Xinhong Xiong, Yuhang Hu, Joanna Aizenberg () and Jiaxi Cui ()
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Xiaozhuang Zhou: University of Electronic Science and Technology of China
Yijun Zheng: ShanghaiTech University
Haohui Zhang: Georgia Institute of Technology
Li Yang: University of Electronic Science and Technology of China
Yubo Cui: University of Electronic Science and Technology of China
Baiju P. Krishnan: INM - Leibniz Institute for New Materials
Shihua Dong: University of Electronic Science and Technology of China
Michael Aizenberg: Harvard University
Xinhong Xiong: University of Electronic Science and Technology of China
Yuhang Hu: Georgia Institute of Technology
Joanna Aizenberg: Harvard University
Jiaxi Cui: University of Electronic Science and Technology of China

Nature Communications, 2023, vol. 14, issue 1, 1-9

Abstract: Abstract Growth constitutes a powerful method to post-modulate materials’ structures and functions without compromising their mechanical performance for sustainable use, but the process is irreversible. To address this issue, we here report a growing-degrowing strategy that enables thermosetting materials to either absorb or release components for continuously changing their sizes, shapes, compositions, and a set of properties simultaneously. The strategy is based on the monomer-polymer equilibrium of networks in which supplying or removing small polymerizable components would drive the networks toward expansion or contraction. Using acid-catalyzed equilibration of siloxane as an example, we demonstrate that the size and mechanical properties of the resulting silicone materials can be significantly or finely tuned in both directions of growth and decomposition. The equilibration can be turned off to yield stable products or reactivated again. During the degrowing-growing circle, material structures are selectively varied either uniformly or heterogeneously, by the availability of fillers. Our strategy endows the materials with many appealing capabilities including environment adaptivity, self-healing, and switchability of surface morphologies, shapes, and optical properties. Since monomer-polymer equilibration exists in many polymers, we envision the expansion of the presented strategy to various systems for many applications.

Date: 2023
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DOI: 10.1038/s41467-023-38768-z

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