Stiffness Reinforcement in Polymer Networks Through Supramolecular Topological Linking
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 International Edition
- Published
- 2026-04-20
- DOI
- https://doi.org/10.1002/anie.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