Hierarchically reversible crosslinking polymeric hydrogels with highly efficient self-healing, robust mechanical properties, and double-driven shape memory behavior

Shishan Xue; Yuanpeng Wu; Guanfei Liu; Meiling Guo; Yuhan Liu; Tao Zhang; Zhanhua Wang

doi:10.1039/D0TA10850B

Hierarchically reversible crosslinking polymeric hydrogels with highly efficient self-healing, robust mechanical properties, and double-driven shape memory behavior†

Shishan Xue,^ae Yuanpeng Wu,

*^ab Guanfei Liu,^a Meiling Guo,^a Yuhan Liu,

^a Tao Zhang

*^c and Zhanhua Wang

*^d

Author affiliations

* Corresponding authors

^a The Center of Functional Materials for Working Fluids of Oil and Gas Field, School of New Energy and Materials, Southwest Petroleum University, Chengdu 610500, Sichuan, China
E-mail: ypwu@swpu.edu.cn

^b State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University, Chengdu 610500, Sichuan, China

^c College of Textile and Clothing Engineering, Soochow University, Suzhou 215123, China
E-mail: zhang.tao@suda.edu.cn

^d State Key Laboratory of Polymer Materials Engineering, Polymer Research Institute, Sichuan University, Chengdu 610065, China
E-mail: zhwangpoly@scu.edu.cn

^e School of Chemistry and Chemical Engineering, Mianyang Normal University, Mianyang 62100, China

Abstract

Designing hydrogels with both excellent mechanical properties and self-healing ability has attracted significant attention because the applications of hydrogels are restricted in many fields due to their poor mechanical properties and short service life. Herein, a novel type of hierarchically reversible crosslinked hydrogel was designed and fabricated using a poly(vinyl alcohol)–borax (PVA/borax) hydrogel and poly(1-allyl-2-thiourea-co-acrylamide) (P(ATU-co-AM)), where P(ATU-co-AM) was interpenetrated in the PVA/borax network to form a semi-interpenetrating network (semi-IPN). The PVA crystalline domains generated from the freezing–thawing process served as second crosslinking points in the semi-IPN structure, further enhancing the mechanical properties of hydrogels. The obtained hydrogels exhibited excellent mechanical properties (tensile strength of 3.6 MPa), rapid self-healing procedure (10 min), high healing efficiency (over 90%), agile pH-driven shape memory behavior (recovered within 260 s) and Ca²⁺-driven shape memory behavior, which are attributed to the reversible backbones imposed by the dynamic borate bonds, abundant hydrogen bonds from PVA and P(ATU-co-AM) chains, and crystallinity of PVA through freezing–thawing cycles. Taking advantage of these fabulous performances and inspired by the bending behavior of Mimosa, a soft catcher actuator was constructed as an example to illustrate the practical applications of this hydrogel, which could catch a plastic fish in Ca²⁺ solution. Thus, due to the self-healing property, actuators with complicated architectures and excellent shape memory behavior can be fabricated by assembling different double layer hydrogels. This study provides a novel strategy to prepare robust hydrogels without sacrificing their self-healing ability and mechanical properties, hopefully promoting the research on robust self-healing hydrogels.

Journal of Materials Chemistry A

Hierarchically reversible crosslinking polymeric hydrogels with highly efficient self-healing, robust mechanical properties, and double-driven shape memory behavior†

Abstract

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Hierarchically reversible crosslinking polymeric hydrogels with highly efficient self-healing, robust mechanical properties, and double-driven shape memory behavior

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