Fabrication of mechanically tough and self-recoverable nanocomposite hydrogels from polyacrylamide grafted cellulose nanocrystal and poly(acrylic acid)

Li, Bengang; Zhang, Yandan; Wu, Chao; Guo, Bin; Luo, Zhenyang

doi:10.1016/j.carbpol.2018.06.047

Cited by 68 publications

(23 citation statements)

References 25 publications

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“…This leads to a higher chance of fracture, unlike more elastic polymers such as polyurethane, where the swelling of the composite would result in no fractures (Frost and Foster, 2019). As well, the drying and reswelling properties themselves showed novelty compared to typical CNC hydrogels found in literature (Yin et al, 2014; Li et al, 2018; Jayaramudu et al, 2019). Usual trends observe that as CNC content within the scaffolds increases, specifically above 5 wt.%, the swelling properties drastically decrease and lead to further embrittlement (Yin et al, 2014; Li et al, 2018; Jayaramudu et al, 2019).…”

Section: Resultsmentioning

confidence: 79%

Gradient Poly(ethylene glycol) Diacrylate and Cellulose Nanocrystals Tissue Engineering Composite Scaffolds via Extrusion Bioprinting

Frost¹,

Sutliff²,

Thayer

et al. 2019

Front. Bioeng. Biotechnol.

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Bioprinting has advanced drastically in the last decade, leading to many new biomedical applications for tissue engineering and regenerative medicine. However, there are still a myriad of challenges to overcome, with vast amounts of research going into bioprinter technology, biomaterials, cell sources, vascularization, innervation, maturation, and complex 4D functionalization. Currently, stereolithographic bioprinting is the primary technique for polymer resin bioinks. However, it lacks the ability to print multiple cell types and multiple materials, control directionality of materials, and place fillers, cells, and other biological components in specific locations among the scaffolds. This study sought to create bioinks from a typical polymer resin, poly(ethylene glycol) diacrylate (PEGDA), for use in extrusion bioprinting to fabricate gradient scaffolds for complex tissue engineering applications. Bioinks were created by adding cellulose nanocrystals (CNCs) into the PEGDA resin at ratios from 95/5 to 60/40 w/w PEGDA/CNCs, in order to reach the viscosities needed for extrusion printing. The bioinks were cast, as well as printed into single-material and multiple-material (gradient) scaffolds using a CELLINK BIOX printer, and crosslinked using lithium phenyl-2,4,6-trimethylbenzoylphosphinate as the photoinitiator. Thermal and mechanical characterizations were performed on the bioinks and scaffolds using thermogravimetric analysis, rheology, and dynamic mechanical analysis. The 95/5 w/w composition lacked the required viscosity to print, while the 60/40 w/w composition displayed extreme brittleness after crosslinking, making both CNC compositions non-ideal. Therefore, only the bioink compositions of 90/10, 80/20, and 70/30 w/w were used to produce gradient scaffolds. The gradient scaffolds were printed successfully and embodied unique mechanical properties, utilizing the benefits of each composition to increase mechanical properties of the scaffold as a whole. The bioinks and gradient scaffolds successfully demonstrated tunability of their mechanical properties by varying CNC content within the bioink composition and the compositions used in the gradient scaffolds. Although stereolithographic bioprinting currently dominates the printing of PEGDA resins, extrusion bioprinting will allow for controlled directionality, cell placement, and increased complexity of materials and cell types, improving the reliability and functionality of the scaffolds for tissue engineering applications.

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Section: Resultsmentioning

confidence: 79%

Gradient Poly(ethylene glycol) Diacrylate and Cellulose Nanocrystals Tissue Engineering Composite Scaffolds via Extrusion Bioprinting

Frost¹,

Sutliff²,

Thayer

et al. 2019

Front. Bioeng. Biotechnol.

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“…When the AM‐MCC content was less than 2 wt%, the breaking elongation together with the breaking stress improved simultaneously, which have been observed in hydrogels reinforced with cellulose nanofibers or nanocrystals [15a,18] . The results mean that there would be strong interactions between the AM‐MCC particles and the PAA matrix of the gel, including filler‐polymer interaction, [3e] functional groups‐metallic ion interaction, [15a,19] and hydrogen bonding . These kinds of abundant and reversible interactions not only contribute to the improvement in mechanical strength of the hydrogel, but also restrain the crack propagation during the stressing processes [15a] .…”

Section: Resultsmentioning

confidence: 84%

“…Besides, the composite hydrogels containing AM‐MCC particles display still much higher breaking stress and elongation after healing. It suggests that part of the interactions between the hydrogel matrix of PAA/Fe 3+ and the AM‐MCC particles could be also re‐built during the self‐healing process and then contribute to the mechanical strength of the healed hydrogel network [10,15a,19,20] . The inset indicates that Gel‐3 (3 wt% AM‐MCC content) is the strongest after self‐healing.…”

Section: Resultsmentioning

confidence: 99%

Reinforcement of Self‐Healing Polyacrylic Acid Hydrogel with Acrylamide Modified Microcrystalline Cellulose^†

2020

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of main observation and conclusion Self-healing hydrogel such as polyacrylic acid (PAA) hydrogel has attracted increasing attention based on its promising potential applications. However, it usually suffers from low strength especially as mechanical device. Herein, a commercial microcrystalline cellulose (MCC) was modified with acrylamide to graft polyacrylamide (PAM) chains on the particle surface. The acrylamide-modified MCC (AM-MCC) was then dispersed in monomer solution of acrylic acid to prepare composite hydrogel. The mechanical properties of the obtained composite hydrogels and the self-healed hydrogels were carefully measured by compressive and tensile tests, and by dynamic mechanical analysis. Our results demonstrate that introduction of a small amount of AM-MCC such as 3 wt% can not only reinforce the original hydrogel and the healed hydrogel markedly, but also improve self-healing efficiency obviously. The analyses indicate that in addition to the reversible multi-interactions such as hydrogen bonding and ionic interactions, the entanglements between the PAA chains of the hydrogel matrix and the PAM chains grafted on the MCC particles have also played an important role on the improvement in mechanical performances and the healing ability of the hydrogel. Moreover, the responsiveness to exterior ion has been tested to indicate potential application of the composite hydrogel as self-healable sensor.

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“…Improved neural differentiation and oxygen metabolism were observed upon embedding neural stem cells (Cheng et al, 2019). In other study by Li et al (2018) polyacrylamide grafted cellulose nanocrystals (CNC-g-PAM), as physical crosslinkers and interfacial compatible nanofillers, were incorporated into poly(acrylic acid) to develop NC hydrogels. NC hydrogels showed significant improvement in tensile properties and self-recovery ability compared to the pure poly(acrylic acid) hydrogel.…”

Section: Nano-scaled Cellulose: a Robust Nanomaterialsmentioning

confidence: 99%

Insight Into the Current Directions in Functionalized Nanocomposite Hydrogels

et al. 2020

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Since the introduction of tissue engineering as an encouraging method for the repair and regeneration of injured tissue, there have been many attempts by researchers to construct bio-mimetic scaffolds which mimic the native extracellular matrix, with the aim of promoting cell growth, cell proliferation, and restoration of the tissue's native functionality. Among the different materials and methods of scaffold fabrication, one particularly promising class of materials, hydrogels, has been extensively studied, with the inclusion of nano-scaled materials into hydrogels leading to the creation of an exciting new generation of nanocomposites, known as nanocomposite hydrogels. To closely mimic the native tissue behavior, scientists have recently focused on the functionalization of incorporated nanomaterials via chiral biomolecules, with reported results showing great potential. The current article aims to introduce a perspective of nano-scaled cellulose as a promising nanomaterial which can be multi-functionalized for the fabrication of nanocomposite hydrogels with applications in tissue engineering and drug delivery systems. This article also briefly reviews the recently reported literature on nanocomposite hydrogels incorporated with chiral functionalized nanomaterials. Such knowledge paves the path for the development of tailored hydrogels toward practical applications.

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Fabrication of mechanically tough and self-recoverable nanocomposite hydrogels from polyacrylamide grafted cellulose nanocrystal and poly(acrylic acid)

Cited by 68 publications

References 25 publications

Gradient Poly(ethylene glycol) Diacrylate and Cellulose Nanocrystals Tissue Engineering Composite Scaffolds via Extrusion Bioprinting

Gradient Poly(ethylene glycol) Diacrylate and Cellulose Nanocrystals Tissue Engineering Composite Scaffolds via Extrusion Bioprinting

Reinforcement of Self‐Healing Polyacrylic Acid Hydrogel with Acrylamide Modified Microcrystalline Cellulose^†

Insight Into the Current Directions in Functionalized Nanocomposite Hydrogels

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Fabrication of mechanically tough and self-recoverable nanocomposite hydrogels from polyacrylamide grafted cellulose nanocrystal and poly(acrylic acid)

Cited by 68 publications

References 25 publications

Gradient Poly(ethylene glycol) Diacrylate and Cellulose Nanocrystals Tissue Engineering Composite Scaffolds via Extrusion Bioprinting

Gradient Poly(ethylene glycol) Diacrylate and Cellulose Nanocrystals Tissue Engineering Composite Scaffolds via Extrusion Bioprinting

Reinforcement of Self‐Healing Polyacrylic Acid Hydrogel with Acrylamide Modified Microcrystalline Cellulose†

Insight Into the Current Directions in Functionalized Nanocomposite Hydrogels

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Product

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Reinforcement of Self‐Healing Polyacrylic Acid Hydrogel with Acrylamide Modified Microcrystalline Cellulose^†