Tough, Stimuli‐Responsive, and Biocompatible Hydrogels with Very High Water Content

Liu, Tianqi; Lü, Shuai; Peng, Xin; Jiao, Chen; Zhang, Jianan; Han, Mei; Wang, Huiliang

doi:10.1002/marc.201800474

Cited by 13 publications

(8 citation statements)

References 31 publications

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“…Stimuli-responsive materials are used in many biomedical applications ( e.g. , tissue engineering, biosensing) and are considered potential candidates for pulsatile, site-specific, and externally stimulated On/Off drug release systems. − Among this group of materials, hydrogels have attracted wide attention due to their tunable properties, which include mechanical strength, as well as structural, chemical, and biological responses to stimuli. , One of the most studied stimuli-responsive hydrogels so far is a thermoresponsive polymer called poly( N -isopropylacrylamide) (PNIPAAm). − The PNIPAAm phase transition from coil to globule appears when the temperature exceeds the typical low critical solution temperature (LCST) and is accompanied by a loss of polymer–water hydrogen bonds and formation of intra- and interchain hydrogen bonds between the amide groups, as well as dehydration of hydrophobic groups . At temperatures above LCST, PNIPAAm shrinks due to a sharp transition from the hydrophilic to the hydrophobic state .…”

Section: Introductionmentioning

confidence: 99%

Multifunctional Platform Based on Electrospun Nanofibers and Plasmonic Hydrogel: A Smart Nanostructured Pillow for Near-Infrared Light-Driven Biomedical Applications

Nakielski

Pawłowska

Rinoldi

et al. 2020

ACS Appl. Mater. Interfaces

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Multifunctional nanomaterials with the ability to respond to near-infrared (NIR) light stimulation are vital for the development of highly efficient biomedical nanoplatforms with a polytherapeutic approach. Inspired by the mesoglea structure of jellyfish bells, a biomimetic multifunctional nanostructured pillow with fast photothermal responsiveness for NIR light-controlled on-demand drug delivery is developed. We fabricate a nanoplatform with several hierarchical levels designed to generate a series of controlled, rapid, and reversible cascade-like structural changes upon NIR light irradiation. The mechanical contraction of the nanostructured platform, resulting from the increase of temperature to 42 °C due to plasmonic hydrogel–light interaction, causes a rapid expulsion of water from the inner structure, passing through an electrospun membrane anchored onto the hydrogel core. The mutual effects of the rise in temperature and water flow stimulate the release of molecules from the nanofibers. To expand the potential applications of the biomimetic platform, the photothermal responsiveness to reach the typical temperature level for performing photothermal therapy (PTT) is designed. The on-demand drug model penetration into pig tissue demonstrates the efficiency of the nanostructured platform in the rapid and controlled release of molecules, while the high biocompatibility confirms the pillow potential for biomedical applications based on the NIR light-driven multitherapy strategy.

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Section: Introductionmentioning

confidence: 99%

Multifunctional Platform Based on Electrospun Nanofibers and Plasmonic Hydrogel: A Smart Nanostructured Pillow for Near-Infrared Light-Driven Biomedical Applications

Nakielski

Pawłowska

Rinoldi

et al. 2020

ACS Appl. Mater. Interfaces

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“…In addition, the swelling of as‐prepared hydrogels in water destroys the RSF/SDS network so that equilibrium hydrogels cannot be obtained. In contrast, if the first RSF/SDS network can be stabilized first during the swelling of hydrogels, the above drawbacks would be overcome, and the obtained hydrogels can reach equilibrium state in water …”

mentioning

confidence: 99%

Highly Stretchable and Tough Physical Silk Fibroin–Based Double Network Hydrogels

Zhao

Guan

2019

Macromol. Rapid Commun.

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a facile way to construct strong RSF hydrogels simply by adding sodium dodecyl sulfate (SDS) into high molecular weight RSF solutions. The resulting hydrogels demonstrated high tensile strength of ≈0.74 MPa and fair extensibility of 140%. [6] Shao et al. also found that ionic liquid (IL)/water mixtures could generate RSF-based gels, whose tensile strength and breaking elongation reached up to 0.4 MPa and 147%, respectively. [11] Okay et al. reported a novel strategy to design mechanically robust and stretchable silk fibroin/hyaluronic acid hydrogels with chemical cross-links and physical cross-links (β-sheet domains). [7] The hybrid hydrogels exhibited a high extensibility up to around 400% and tensile strength of 65 kPa after equilibrium swelling. Okay also described a directional freezing/cryogelation method to produce high-strength silk fibroin cryogels with a degree of mechanical anisotropy. The compressive modulus of cryogels formed at 16.7 wt% RSF concentration was 45 MPa, but the tensile properties were not shown. [12] Consequently, achieving highly stretchable RSF hydrogels for wide-range applications [13] is still in its infancy.An alternative strategy to prepare strong and tough hydrogels is the double network (DN) hydrogel, which introduces a flexible and stretchable second network. These DN hydrogels demonstrated high fracture strength (0.1-10 MPa) and high water content (60-90%). [14][15][16][17][18][19] A series of DN gels using biomacromolecules (agar, cellulose) had been developed. [20,21] Chen et al. developed RSF-based DN hydrogels via introducing a hydrophobically associated gel of polyacrylamide (HPAAm) as the second network. [10] The DN hydrogels were conveniently synthesized by the one-pot method coupled with photo-polymerization, and the resultant RSF/HPAAm DN gels showed a tensile strength of ≈1.17 MPa, and breaking elongation of ≈1900%, but non-equilibrium RSF/HPAAm DN gels contained excessive residual monomers. It is notable that although the RSF gels could be rapidly achieved via introducing SDS, the gelation that takes only a few minutes is difficult to control. It is quite difficult to achieve uniform mixing between SDS micelles and the hydrophobic monomers via the one-step method, which often resulted in poor homogeneity of the gels. In addition, the swelling of as-prepared hydrogels in water destroys the RSF/SDS network so that equilibrium hydrogels cannot be obtained. In contrast, if the first RSF/SDS network can be stabilized first during the swelling of hydrogels, the Regenerated silk fibroin (RSF) is a promising biomedical material, but the poor mechanical properties of RSF hydrogels may hinder the use as structural components. Herein, an equilibrium RSF hydrogel is prepared and optimized based on the double network (DN) concept. After sufficient soaking in water and removal of small molecules, the equilibrium RSF DN hydrogels prove stable in water, strong, highly extensible, and tough with 0.26-0.44 MPa tensile strength, 500-900% elongation, and 2 MJ m −3 work of extension. The...

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“…In general, high water content is common in hydrogel due to its biomimicry property [44]. However, hydrogel with a water content greater than 90% is very weak and has a limited practical application in tissue engineering [45]. Due to this reason, a suitable formulation is crucial to balance between sufficient water content and mechanical strength.…”

Section: Swelling Properties Of Cnc/alg/pegda Constructsmentioning

confidence: 99%

Preparation and Characterisation of Cellulose Nanocrystal/Alginate/Polyethylene Glycol Diacrylate (CNC/Alg/PEGDA) Hydrogel Using Double Network Crosslinking Technique for Bioprinting Application

et al. 2022

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In this study, we aimed to prepare and characterise hydrogel formulations using cellulose nanocrystals (CNCs), alginate (Alg), and polyethylene glycol diacrylate (PEGDA). The CNC/Alg/PEGDA formulations were formed using a double network crosslinking approach. Firstly, CNC was extracted from oil palm trunk, and the size and morphology of the CNCs were characterised using TEM analysis. Secondly, different formulations were prepared using CNCs, Alg, and PEGDA. The mixtures were crosslinked with Ca2+ ions and manually extruded using a syringe before being subjected to UV irradiation at 365 nm. The shear-thinning properties of the formulations were tested prior to any crosslinking, while the determination of storage and loss modulus was conducted post extrusion after the Ca2+ ion crosslink using a rheometer. For the analysis of swelling behaviour, the constructs treated with UV were immersed in PBS solution (pH 7.4) for 48 h. The morphology of the UV crosslinked construct was analysed using SEM imaging. The extracted CNC exhibited rod-like structures with an average diameter and length of around 7 ± 2.4 and 113 ± 20.7 nm, respectively. Almost all CNC/Alg/PEGDA formulations (pre-gel formulation) displayed shear-thinning behaviour with the power-law index η < 1, and the behaviour was more prominent in the 1% [w/v] Alg formulations. The CNC/Alg/PEGDA with 2.5% and 4% [w/v] Alg displayed a storage modulus dominance over loss modulus (G′ > G″) which suggests good shape fidelity. After the hydrogel constructs were subjected to UV treatment at 365 nm, only the F8 construct [4% CNC: 4% Alg: 40% PEGDA] demonstrated tough and flexible characteristics that possibly mimic the native articular cartilage property due to a similar water content percentage (79.5%). In addition, the small swelling ratio of 4.877 might contribute to a minimal change of the 3D construct’s geometry. The hydrogel revealed a rough and wavy surface, and the pore size ranged from 3 to 20 µm. Overall, the presence of CNCs in the double network hydrogel demonstrated importance and showed positive effects towards the fabrication of a potentially ideal 3D bioprinted scaffold.

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Tough, Stimuli‐Responsive, and Biocompatible Hydrogels with Very High Water Content

Cited by 13 publications

References 31 publications

Multifunctional Platform Based on Electrospun Nanofibers and Plasmonic Hydrogel: A Smart Nanostructured Pillow for Near-Infrared Light-Driven Biomedical Applications

Multifunctional Platform Based on Electrospun Nanofibers and Plasmonic Hydrogel: A Smart Nanostructured Pillow for Near-Infrared Light-Driven Biomedical Applications

Highly Stretchable and Tough Physical Silk Fibroin–Based Double Network Hydrogels

Preparation and Characterisation of Cellulose Nanocrystal/Alginate/Polyethylene Glycol Diacrylate (CNC/Alg/PEGDA) Hydrogel Using Double Network Crosslinking Technique for Bioprinting Application

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