An Orthogonal Dynamic Covalent Polymer Network with Distinctive Topology Transformations for Shape‐ and Molecular Architecture Reconfiguration

• Published in: Angewandte Chemie Vol. 134; no. 11
• Main Authors: Miao, Wusha, Yang, Bo, Jin, Binjie, Ni, Chujun, Feng, Haijun, Xue, Yaoting, Zheng, Ning, Zhao, Qian, Shen, Youqing, Xie, Tao
• Format: Journal Article
• Language: English
• Published: Weinheim Wiley Subscription Services, Inc 07.03.2022
• Subjects: Bottlebrush Polymer; Chain branching; Chemical bonds; Chemistry; Computer architecture; Covalence; Mainframes; Material properties; Mechanical properties; Metathesis; Molecular structure; Orthogonal Dynamic Covalent Bonds; Polymers; Reconfiguration; Topological Transformation; Topology; Transesterification
• ISSN: 0044-8249; 1521-3757
• DOI: 10.1002/ange.202109941

Bond exchange in a typical dynamic covalent polymer network allows access to macroscopic shape reconfigurability, but the network architecture is not altered. An alternative possibility is that the network architecture can be designed to switch to various topological states corresponding to different material properties. Achieving both in one network can expand the material scope, but their intrinsically conflicting mechanisms make it challenging. We design a dynamic covalent network that can undergo two orthogonal topological transformations, namely transesterification on the branched chains and olefin metathesis on the mainframe. This allows independent control of the macroscopic shape and molecular architecture. With this design, we illustrate a bottlebrush network with programmable shape and spatially definable mechanical properties. Our strategy paves a way to on‐demand regulation of network polymers. A dynamic covalent polymer network was designed to allow independent programming of the macroscopic shape and mechanical properties via two orthogonal topological transformations.