Dual physically crosslinked nanocomposite hydrogels reinforced by poly(N-vinylpyrrolidone) grafted cellulose nanocrystal
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ORIGINAL RESEARCH
Dual physically crosslinked nanocomposite hydrogels reinforced by poly(N-vinylpyrrolidone) grafted cellulose nanocrystal with high strength, toughness, and rapid selfrecovery Bengang Li
. Yuanfeng Han . Yandan Zhang . Xuzhi Cao . Zhenyang Luo
Received: 2 July 2020 / Accepted: 22 September 2020 Ó Springer Nature B.V. 2020
Abstract It remains challenging to develop hydrogels with comprehensive mechanical properties including ultrahigh strength, toughness and rapid self-recovery. Herein, dual physical crosslinking strategy was used to develop novel nanocomposite hydrogels reinforced by poly(N-vinylpyrrolidone) grafted cellulose nanocrystal (CNC-g-PVP). The hydrogels were fabricated via in situ copolymerization of acrylic acid (AA) and acrylamide (AM) in presence of CNC-g-PVP and subsequent introduction of Fe3? ions. CNC-g-PVP induced the first crosslinking through strong cooperative hydrogen bonds existing between PVP chains grafted onto CNCs and amide
groups from P(AM-co-AA) chains. Fe3? triggered the second crosslinking by forming coordination bonds with –COO- groups. The cooperative hydrogen bonds enhanced the interfacial compatibility between CNCg-PVP nanofillers and hydrogel matrix, and served as fast recoverable sacrificial bonds. As a result, the hydrogels exhibited high tensile strength (1.89–2.51 MPa), remarkable toughness (6.01–6.81 MJ/m3), rapid self-recovery (83.4–97.8% recovery of hysteresis loop within 5 min) and favourable fatigue resistance.
Electronic supplementary material The online version of this article (https://doi.org/10.1007/s10570-020-03487-x) contains supplementary material, which is available to authorized users. B. Li (&) Y. Han Y. Zhang X. Cao Z. Luo (&) College of Science, Nanjing Forestry University, Nanjing 210037, People’s Republic of China e-mail: [email protected] Z. Luo e-mail: [email protected]
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Cellulose
Graphic abstract
Keywords Nanocomposite hydrogel Cellulose nanocrystals Mechanical properties Cooperative hydrogen bonds Coordination bonds
Introduction Hydrogels are chemically or physically crosslinked polymer networks capable of absorbing large amounts of water. As promising soft and wet materials, hydrogels have been utilized in numerous fields, such as drug delivery (Secret et al. 2014), tissue engineering (Torres-Rendon et al. 2015), soft electronics (Lin et al. 2016), sensors (Jing et al. 2018), and so on. However, the conventional hydrogels usually exhibit poor mechanical performance due to their intrinsic structural inhomogeneity and lacking of effective energy dissipation (Zhao 2014; Gong 2010), which severely hinders their practical application in load-bearing fields such as artificial muscles and soft actuators. To address this problem, tremendous efforts have been devoted to develop mechanically strong and tough hydrogels with novel microstructures and toughening mechanisms, including tetra-arm PEG hydrogels (Shibayama et al. 2019), nanocomposite hydrogels (Chen
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