Stiffness Reinforcement in Polymer Networks Through Supramolecular Topological Linking
ABSTRACT Polymer networks possess numerous elastically defective and isolated loops, which do not contribute to mechanical stiffness. In this report, we introduce a strategy of supramolecular topological linking to access stiffer‐yet‐ductile polymeric materials through incorporation of supramolecular tetravalent crosslinkers. Dynamic dissociation/re‐association between these high‐functionality crosslinks enables the formation of topologically‐linked loops that serve as elastic springs to stiffen the networks. An exceptional scaling exponent of 2.05 for Young's modulus versus crosslinker concentration is obtained, exceeding most reported randomly‐crosslinked polymeric systems. Compared to conventional analogs, the mechanical properties of the resultant materials are enhanced: Young's modulus (2‐fold), elongation at break (8‐fold), and work of fracture (100‐fold). Uplifting modulus scalings through supramolecular topological linking paves a new path to the design of stiffness‐reinforced soft materials, holding substantial promise in load‐bearing application scenarios such as tissue implants, bioelectronic interfaces, and soft robotics.
Authors
- Bohang Wu (ORCID: https://orcid.org/0000-0002-0101-6034)
- Yiheng Wu (ORCID: https://orcid.org/0009-0001-0524-7251)
- Yuwei Gu (ORCID: https://orcid.org/0000-0002-9604-7764)
- Guanglu Wu (ORCID: https://orcid.org/0000-0002-9690-5992)
- Tongfan Hao (ORCID: https://orcid.org/0000-0003-0093-4922)
- Qin Ding (ORCID: https://orcid.org/0000-0002-8902-795X)
- X Wang
- Hui Li (ORCID: https://orcid.org/0000-0001-9198-3951)
- Jasper van der Gucht (ORCID: https://orcid.org/0000-0001-5525-8322)
- Martien A. Cohen Stuart (ORCID: https://orcid.org/0000-0001-6880-7861)
- Shixian Lv (ORCID: https://orcid.org/0000-0001-5623-7224)
- Jingzhou Wang (ORCID: https://orcid.org/0000-0001-8142-2202)
- Zehuan Huang (ORCID: https://orcid.org/0000-0003-4111-7064)
- Jie Yang (ORCID: https://orcid.org/0000-0003-4801-7162)
- Junting Huang
- Yuchong Yang (ORCID: https://orcid.org/0000-0001-9733-3255)
- Dan Xing (ORCID: https://orcid.org/0000-0001-6966-3134)
- Du Wang
- Zixiang Zhou
- Chengyu Zeng
- Jianhao Lin
- Tong Wu
- Mingxin Zhong
Institutions
- Rutgers, The State University of New Jersey (US)
- Jiangsu University (CN)
- Jilin University (CN)
- Peking University (CN)
- University of Cambridge (GB)
- University of Chicago (US)
- Ministry of Education (RO)
- Ministry of Education (IR)
- Peking University People's Hospital (CN)
- Ministry of Education and Child Care (CA)
- State Key Laboratory of Supramolecular Structure and Materials
- Wageningen University & Research (NL)
Publication Details
- Journal
- Angewandte Chemie
- Published
- 2026-04-21
- DOI
- https://doi.org/10.1002/ange.7480690
- Primary Topic
- Polymer composites and self-healing
- Type
- article
- Field-Weighted Citation Impact
- 0.00
Funders
- National Natural Science Foundation of China
- Natural Science Foundation of Beijing Municipality