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. 2024 Mar 21;10(3):212.
doi: 10.3390/gels10030212.

Tailoring Hydrogel Structures: Investigating the Effects of Multistep Cellulose Defibrillation on Polyvinyl Alcohol Composites

Gabriel Goetten de Lima  1   2 , Bruno Bernardi Aggio  3 , Alessandra Cristina Pedro  3 , Tielidy A de M de Lima  1 , Washington Luiz Esteves Magalhães  3
Affiliations

Tailoring Hydrogel Structures: Investigating the Effects of Multistep Cellulose Defibrillation on Polyvinyl Alcohol Composites

Gabriel Goetten de Lima et al. Gels. .

Abstract

Defibrillating cellulose through various grinding steps and incorporating it into hydrogels introduces unique properties that warrant thorough exploration. This study investigates cellulose defibrillation at different steps (15-120) using an ultra-fine friction grinder, blended with high-molecular-weight polyvinyl alcohol (PVA), and crosslinked via freeze-thawing. A critical discovery is the influence of defibrillation on the hydrogel structure, as evidenced by reduced crystallinity, thermal degradation, and the enhanced swelling of PVA chains. Despite an increased elastic modulus of up to 120 steps, the synthesized material maintains remarkable strength under hydrated conditions, holding significant promise in biomaterial applications.

Keywords: PVA; composite hydrogels; freeze–thawing; kraft process; nanofibrillated cellulose.

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Conflict of interest statement

The authors declare no conflicts of interest.

Figures

Figure 1
Figure 1
Surface morphology performed by SEM for PVA hydrogels samples containing cellulose defibrillated at different steps: (a) 15, (b) 30, (c) 60, and (d) 120.
Figure 2
Figure 2
Cross-section (a–d) and processed colourmap (e–h) images for samples studied of PVA hydrogels with cellulose defibrillated at 15 (a,e), 30 (b,f), 60 (c,g), and 120 (d,h) steps.
Figure 3
Figure 3
FTIR of PVA hydrogels and also containing cellulose defibrillated at different steps: 30, 60, and 120. Regions were assigned as to the most different profiles seen; the numbers on each assigned band mean that there is a perceived difference for that specific condition.
Figure 4
Figure 4
PM-IRRAS for the bulk signal of PVA hydrogels containing cellulose defibrillated at different steps, where (a) corresponds to the whole spectra region and purple circle indicates the region where a zoom with smoothing spectra was performed in (b).
Figure 5
Figure 5
DMA tensile stress–strain mode for dried (a) and fully swollen (c) PVA+NFC hydrogels, containing cellulose defibrillated at different steps. (b,d) The elastic modulus calculated as the slope in stress–strain curves. (*) Statistically significant different by HSD Tukey test (p < 0.05).
Figure 6
Figure 6
(a) Thermogravimetric analysis and its derivative for pure NFC films defibrillated at different steps (a,c) and PVA hydrogel samples blended with cellulose defibrillated at different steps (b,d). Arrows indicate the direction in which the main peak is shifting at increased defibrillation steps.
Figure 7
Figure 7
Swelling ratio of the studied PVA hydrogels containing defibrillated cellulose at different steps.
Figure 8
Figure 8
Diagram to illustrate the hypothesis of this work in which cellulose bundles are defibrillated by the mechanical forces; depending on the degree of defibrillation, the interaction between PVA by physical crosslinking changes. A saturation fn the interaction occurs at 60 steps, and at 120 steps, PVA is aggregated around the overdefibrillated fibres.
See this image and copyright information in PMC

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