Tough and Healable Shape‐Memory Elastomers Enabled by Dynamic Hyperbranched Topological Networks

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Main Authors: Zhao Xu, Juan Chen, Haili Qin, Jiang‐Qi Feng, Pan Guo, Hong Chen, Huai‐Ping Cong
Format: Artículo Open Access
Published: Wiley 2026
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author Zhao Xu
Juan Chen
Haili Qin
Jiang‐Qi Feng
Pan Guo
Hong Chen
Huai‐Ping Cong
author_facet Zhao Xu
Juan Chen
Haili Qin
Jiang‐Qi Feng
Pan Guo
Hong Chen
Huai‐Ping Cong
Zhao Xu
Juan Chen
Haili Qin
Jiang‐Qi Feng
Pan Guo
Hong Chen
Huai‐Ping Cong
collection Wiley Open Access
contents Tough and Healable Shape‐Memory Elastomers Enabled by Dynamic Hyperbranched Topological Networks Zhao Xu Juan Chen Haili Qin Jiang‐Qi Feng Pan Guo Hong Chen Huai‐Ping Cong Advanced Materials ABSTRACT Integrating rapid self‐healability and shape memory into tough polyurethane elastomers is highly desirable for applications of artificial muscles and soft actuators. However, this combination is fundamentally limited by an inherent structural trade‐off between strong phase separation and dynamic interactions. Herein, we develop a dynamic hyperbranched topology strategy to engineer gold nanoparticle‐crosslinked polyurethane elastomers featuring a hierarchical structure that includes dynamic topological networks, enhanced hard domains with strong hydrogen bonds, and nano‐assemblies phase‐separated from an amorphous matrix in which soft segments are prepacked for ultrasensitive strain‐induced crystallization (SIC). Reversible dissociation/combination of dynamic bonds and progressive rupture of hard domains and assemblies contribute to energy dissipation, while ultrasensitive SIC enables network self‐reinforcement, affording a high strength of 53 MPa, a toughness of 483.3 MJ m −3 , and a fracture energy of 352.5 kJ m −2 . Meanwhile, abundant dynamic bonds enable rapid self‐healability of the elastomer with a healing efficiency of 93.5% upon 2‐min near‑infrared  irradiation. Accompanied by sensitive SIC‐induced network fixation, these elastomers show remarkable shape memory with a shape fixation ratio of 91% and a shape recovery ratio of 94.7%. Based on the unprecedented combinational properties, this work establishes a design paradigm for hierarchically structured elastomers that reconcile high mechanical performance with smart stimulus responsiveness. 10.1002/adma.73541 http://onlinelibrary.wiley.com/termsAndConditions#vor
doi_str_mv 10.1002/adma.73541
format Artículo Open Access
id wiley_oa_10_1002_adma_73541
institution Wiley Open Access
license_str_mv http://onlinelibrary.wiley.com/termsAndConditions#vor
publishDate 2026
publisher Wiley
record_format wiley_oa
spellingShingle Tough and Healable Shape‐Memory Elastomers Enabled by Dynamic Hyperbranched Topological Networks
Zhao Xu
Juan Chen
Haili Qin
Jiang‐Qi Feng
Pan Guo
Hong Chen
Huai‐Ping Cong
Advanced Materials
Tough and Healable Shape‐Memory Elastomers Enabled by Dynamic Hyperbranched Topological Networks Zhao Xu Juan Chen Haili Qin Jiang‐Qi Feng Pan Guo Hong Chen Huai‐Ping Cong Advanced Materials ABSTRACT Integrating rapid self‐healability and shape memory into tough polyurethane elastomers is highly desirable for applications of artificial muscles and soft actuators. However, this combination is fundamentally limited by an inherent structural trade‐off between strong phase separation and dynamic interactions. Herein, we develop a dynamic hyperbranched topology strategy to engineer gold nanoparticle‐crosslinked polyurethane elastomers featuring a hierarchical structure that includes dynamic topological networks, enhanced hard domains with strong hydrogen bonds, and nano‐assemblies phase‐separated from an amorphous matrix in which soft segments are prepacked for ultrasensitive strain‐induced crystallization (SIC). Reversible dissociation/combination of dynamic bonds and progressive rupture of hard domains and assemblies contribute to energy dissipation, while ultrasensitive SIC enables network self‐reinforcement, affording a high strength of 53 MPa, a toughness of 483.3 MJ m −3 , and a fracture energy of 352.5 kJ m −2 . Meanwhile, abundant dynamic bonds enable rapid self‐healability of the elastomer with a healing efficiency of 93.5% upon 2‐min near‑infrared  irradiation. Accompanied by sensitive SIC‐induced network fixation, these elastomers show remarkable shape memory with a shape fixation ratio of 91% and a shape recovery ratio of 94.7%. Based on the unprecedented combinational properties, this work establishes a design paradigm for hierarchically structured elastomers that reconcile high mechanical performance with smart stimulus responsiveness. 10.1002/adma.73541 http://onlinelibrary.wiley.com/termsAndConditions#vor
title Tough and Healable Shape‐Memory Elastomers Enabled by Dynamic Hyperbranched Topological Networks
topic Advanced Materials
url https://advanced.onlinelibrary.wiley.com/doi/10.1002/adma.73541