Stiffness Reinforcement in Polymer Networks Through Supramolecular Topological Linking

B Bohang Wu (Key Laboratory of Polymer Chemistry and Physics of Ministry of Education School of Materials Science and Engineering Peking University Beijing China) J Junting Huang C Chengyu Zeng (Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore 117543, Republic of Singapore) M Mingxin Zhong (Research School of Polymeric Materials, School of Materials Science and Engineering Jiangsu University Zhenjiang China) Q Qin Ding (Key Laboratory of Polymer Chemistry and Physics of Ministry of Education School of Materials Science and Engineering Peking University Beijing China) D Du Wang J Jingzhou Wang (Discovery Chemistry, Merck & Co., Inc., 213 E Grand Ave, South San Francisco, California 94080, United States) Z Zixiang Zhou (Hubei Key Laboratory of Low Dimensional Optoelectronic Materials and Devices) T Tong Wu X Xinling Wang H Hui Li D Dan Xing J Jianhao Lin (Arthritis Clinical and Research Center Peking University People's Hospital Beijing P. R. China) Y Yiheng Wu (State Key Laboratory of Advanced Metallurgy) Y Yuwei Gu S Shixian Lv Y Yuchong Yang (Yusuf Hamied Department of Chemistry) Y Yang Jiao G Guanglu Wu (State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry) J Jasper van der Gucht M Martien A. Cohen Stuart (Laboratory of Physical Chemistry and Soft Matter Wageningen University & Research Wageningen the Netherlands) T Tongfan Hao (Research School of Polymeric Materials, School of Materials Science and Engineering Jiangsu University Zhenjiang China) Z Zehuan Huang (Melville Laboratory for Polymer Synthesis, Yusuf Hamied Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, U.K.)

Abstract

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.

Article Details

Volume / Issue Vol. 65, Issue 23
Published June 01, 2026
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (23)

B

Bohang Wu

Key Laboratory of Polymer Chemistry and Physics of Ministry of Education School of Materials Science and Engineering Peking University Beijing China

J

Junting Huang

C

Chengyu Zeng

Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore 117543, Republic of Singapore

M

Mingxin Zhong

Research School of Polymeric Materials, School of Materials Science and Engineering Jiangsu University Zhenjiang China

Q

Qin Ding

Key Laboratory of Polymer Chemistry and Physics of Ministry of Education School of Materials Science and Engineering Peking University Beijing China

D

Du Wang

J

Jingzhou Wang

Discovery Chemistry, Merck & Co., Inc., 213 E Grand Ave, South San Francisco, California 94080, United States

Z

Zixiang Zhou

Hubei Key Laboratory of Low Dimensional Optoelectronic Materials and Devices

T

Tong Wu

X

Xinling Wang

H

Hui Li

D

Dan Xing

J

Jianhao Lin

Arthritis Clinical and Research Center Peking University People's Hospital Beijing P. R. China

Y

Yiheng Wu

State Key Laboratory of Advanced Metallurgy

Y

Yuwei Gu

S

Shixian Lv

Y

Yuchong Yang

Yusuf Hamied Department of Chemistry

Y

Yang Jiao

G

Guanglu Wu

State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry

J

Jasper van der Gucht

M

Martien A. Cohen Stuart

Laboratory of Physical Chemistry and Soft Matter Wageningen University & Research Wageningen the Netherlands

T

Tongfan Hao

Research School of Polymeric Materials, School of Materials Science and Engineering Jiangsu University Zhenjiang China

Z

Zehuan Huang

Melville Laboratory for Polymer Synthesis, Yusuf Hamied Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, U.K.