Jellyfish‐Inspired Polyurea Ionogel with Mechanical Robustness, Self‐Healing, and Fluorescence Enabled by Hyperbranched Cluster Aggregates

Author:

Zhang Zhipeng1,Qian Lu2,Zhang Bin1,Ma Chunfeng1ORCID,Zhang Guangzhao1

Affiliation:

1. Faculty of Materials Science and Engineering South China University of Technology Guangzhou 510640 China

2. Science and Technology Innovation Center Guangzhou University of Chinese Medicine Guangzhou 510006 China

Abstract

AbstractIonogels are promising for soft iontronics, with their network structure playing a pivotal role in determining their performance and potential applications. However, simultaneously achieving mechanical toughness, low hysteresis, self‐healing, and fluorescence using existing network structures is challenging. Drawing inspiration from jellyfish, we propose a novel hierarchical crosslinking network structure design for in situ formation of hyperbranched cluster aggregates (HCA) to fabricate polyurea ionogels to overcome these challenges. Leveraging the disparate reactivity of isocyanate groups, we induce the in situ formation of HCA through competing reactions, enhancing toughness and imparting the clustering‐triggered emission of ionogel. This synergy between supramolecular interactions in the network and plasticizing effect in ionic liquid leads to reduced hysteresis of the ionogel. Furthermore, the incorporation of NCO‐terminated prepolymer with dynamic oxime–urethane bonds (NPU) enables self‐healing and enhances stretchability. Our investigations highlight the significant influence of HCA on ionogel performance, showcasing mechanical robustness including high strength (3.5 MPa), exceptional toughness (5.5 MJ m−3), resistance to puncture, and low hysteresis, self‐healing, as well as fluorescence, surpassing conventional dynamic crosslinking approaches. This network design strategy is versatile and can meet the various demands of flexible electronics applications.

Funder

National Key Research and Development Program of China

National Natural Science Foundation of China

Basic and Applied Basic Research Foundation of Guangdong Province

Publisher

Wiley

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