A High Modulus, Multi‐Stimuli Responsive, Interwoven Protein Network With Topologically Confined Micro‐Association
Abstract
Abstract All‐protein‐based materials are attractive for their genetic encodability, precise structure, and versatile functions, yet integrating mechanical strength, dynamic adaptability, and functional activity in one system remains challenging. Herein, we report a multi‐stimuli‐responsive, self‐healing, all‐protein‐based network with an interwoven network topology, whose mechanics can be further reinforced by topologically confined micro‐association upon tempering. The network was constructed by polymerizing pseudo[2]catenanes—which employ p53dim for entanglement and SpyTag(DA)‐SpyCatcher complex for physical cyclization—that are opened into a star‐like conformation. Network formation can be triggered by increasing concentration, calmodulin (CaM) binding, or light irradiation (when azoswitch‐modified CaM is used). Subsequent tempering unfolds the SpyTag/SpyCatcher complex, inducing micro‐association that acts as additional crosslinks within the topologically confined network. While the entangled architecture minimizes chain slippage, the micro‐associations enhance crosslinking and stress dissipation, collectively improving mechanical properties and long‐term stability. We further demonstrate its practical utility in controlled release and enzyme immobilization, establishing topological proteins as a versatile platform for designing genetically programmable, mechanically tunable, stimuli‐responsive biomaterials.
Article Details
Authors (10)
Tingjie Xu
Yibin Sun
Jilin University , , ,
Yu‐Xiang Wang
Beijing National Laboratory for Molecular Sciences Key Laboratory of Polymer Chemistry & Physics of Ministry of Education Center for Soft Matter Science and Engineering College of Chemistry and Molecular Engineering Peking University Beijing 100871 P.R. China
Fengyi Jiang
Bo Hou
School of Chemistry and Molecular Engineering
Ziyi Meng
Beijing National Laboratory for Molecular Sciences Key Laboratory of Polymer Chemistry & Physics of Ministry of Education Center for Soft Matter Science and Engineering College of Chemistry and Molecular Engineering Peking University Beijing 100871 P.R. China
Lianjie Xu
Beijing National Laboratory for Molecular Sciences, Key Laboratory of Polymer Chemistry & Physics of Ministry of Education, Center for Soft Matter Science and Engineering, College of Chemistry and Molecular Engineering, Peking University
Yajie Liu
Center for Retrovirus Research, The Ohio State University
Wen‐Hao Wu
Beijing National Laboratory for Molecular Sciences Key Laboratory of Polymer Chemistry & Physics of Ministry of Education Center for Soft Matter Science and Engineering College of Chemistry and Molecular Engineering Peking University Beijing 100871 P.R. China
Wen‐Bin Zhang
Beijing National Laboratory for Molecular Sciences Key Laboratory of Polymer Chemistry & Physics of Ministry of Education Center for Soft Matter Science and Engineering College of Chemistry and Molecular Engineering Peking University Beijing 100871 P.R. China