The sol-gel transition of ultra-low solid content TEMPO-cellulose nanofibril/mixed-linkage β-glucan bionanocomposite gels

Suvi Arola, Mahmoud Ansari, Antti Oksanen, Elias Retulainen, Savvas G. Hatzikiriakos, Harry Brumer (Corresponding Author)

Research output: Contribution to journalArticleScientificpeer-review

Abstract

We present the preparation, morphological analysis, and rheological characterization of ultra-low solid content gels prepared by physically cross-linking TEMPO-oxidized cellulose nanofibrils (TEMPO-CNF) with the soluble plant-cell-wall polysaccharide, mixed-linkage β-glucan (MLG). Of particular note, gel formation was rapidly induced by very small amounts of MLG (e.g. 0.125% w/v) at extremely low TEMPO-CNF concentration (0.05% w/v), which independently were otherwise fluid and thus easily handled. Rheology of these bionanocomposite gel systems as a function of MLG and TEMPO-CNF concentrations revealed that the critical gel concentration of MLG and TEMPO-CNF followed a power-law relation of the concentration of the other component. Surprisingly, these systems also exhibited an additional transition to thick gels at high TEMPO-CNF and MLG concentrations that was visible only at low frequencies. Cryogenic scanning electron microscopy (cryo-SEM) imaging of admixture solutions and gels revealed increased network crowding with increasing MLG amounts. The data are consistent with the hypothesis that non-covalent cellulose-MLG interactions, analogous to those occurring within plant cell walls, drive gel formation. The ability to tune gel physical properties simply by controlling CNF (a promising forest bioproduct) and MLG (a readily available agricultural polysaccharide) fractions at very low solid and polymer content opens new possibilities for material applications in diverse industries.

Original languageEnglish
Pages (from-to)9393-9401
Number of pages9
JournalSoft Matter
Volume14
Issue number46
DOIs
Publication statusPublished - 28 Nov 2018
MoE publication typeNot Eligible

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Glucans
cellulose
linkages
oxidized cellulose
Cellulose
Sol-gels
Gels
gels
polysaccharides
Polysaccharides
crowding
TEMPO
admixtures
Rheology
rheology
Cryogenics
cryogenics
Polymers
Physical properties
physical properties

Cite this

@article{541dad7bd79740978e22a7fc6fe0a63e,
title = "The sol-gel transition of ultra-low solid content TEMPO-cellulose nanofibril/mixed-linkage β-glucan bionanocomposite gels",
abstract = "We present the preparation, morphological analysis, and rheological characterization of ultra-low solid content gels prepared by physically cross-linking TEMPO-oxidized cellulose nanofibrils (TEMPO-CNF) with the soluble plant-cell-wall polysaccharide, mixed-linkage β-glucan (MLG). Of particular note, gel formation was rapidly induced by very small amounts of MLG (e.g. 0.125{\%} w/v) at extremely low TEMPO-CNF concentration (0.05{\%} w/v), which independently were otherwise fluid and thus easily handled. Rheology of these bionanocomposite gel systems as a function of MLG and TEMPO-CNF concentrations revealed that the critical gel concentration of MLG and TEMPO-CNF followed a power-law relation of the concentration of the other component. Surprisingly, these systems also exhibited an additional transition to thick gels at high TEMPO-CNF and MLG concentrations that was visible only at low frequencies. Cryogenic scanning electron microscopy (cryo-SEM) imaging of admixture solutions and gels revealed increased network crowding with increasing MLG amounts. The data are consistent with the hypothesis that non-covalent cellulose-MLG interactions, analogous to those occurring within plant cell walls, drive gel formation. The ability to tune gel physical properties simply by controlling CNF (a promising forest bioproduct) and MLG (a readily available agricultural polysaccharide) fractions at very low solid and polymer content opens new possibilities for material applications in diverse industries.",
author = "Suvi Arola and Mahmoud Ansari and Antti Oksanen and Elias Retulainen and Hatzikiriakos, {Savvas G.} and Harry Brumer",
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The sol-gel transition of ultra-low solid content TEMPO-cellulose nanofibril/mixed-linkage β-glucan bionanocomposite gels. / Arola, Suvi; Ansari, Mahmoud; Oksanen, Antti; Retulainen, Elias; Hatzikiriakos, Savvas G.; Brumer, Harry (Corresponding Author).

In: Soft Matter, Vol. 14, No. 46, 28.11.2018, p. 9393-9401.

Research output: Contribution to journalArticleScientificpeer-review

TY - JOUR

T1 - The sol-gel transition of ultra-low solid content TEMPO-cellulose nanofibril/mixed-linkage β-glucan bionanocomposite gels

AU - Arola, Suvi

AU - Ansari, Mahmoud

AU - Oksanen, Antti

AU - Retulainen, Elias

AU - Hatzikiriakos, Savvas G.

AU - Brumer, Harry

PY - 2018/11/28

Y1 - 2018/11/28

N2 - We present the preparation, morphological analysis, and rheological characterization of ultra-low solid content gels prepared by physically cross-linking TEMPO-oxidized cellulose nanofibrils (TEMPO-CNF) with the soluble plant-cell-wall polysaccharide, mixed-linkage β-glucan (MLG). Of particular note, gel formation was rapidly induced by very small amounts of MLG (e.g. 0.125% w/v) at extremely low TEMPO-CNF concentration (0.05% w/v), which independently were otherwise fluid and thus easily handled. Rheology of these bionanocomposite gel systems as a function of MLG and TEMPO-CNF concentrations revealed that the critical gel concentration of MLG and TEMPO-CNF followed a power-law relation of the concentration of the other component. Surprisingly, these systems also exhibited an additional transition to thick gels at high TEMPO-CNF and MLG concentrations that was visible only at low frequencies. Cryogenic scanning electron microscopy (cryo-SEM) imaging of admixture solutions and gels revealed increased network crowding with increasing MLG amounts. The data are consistent with the hypothesis that non-covalent cellulose-MLG interactions, analogous to those occurring within plant cell walls, drive gel formation. The ability to tune gel physical properties simply by controlling CNF (a promising forest bioproduct) and MLG (a readily available agricultural polysaccharide) fractions at very low solid and polymer content opens new possibilities for material applications in diverse industries.

AB - We present the preparation, morphological analysis, and rheological characterization of ultra-low solid content gels prepared by physically cross-linking TEMPO-oxidized cellulose nanofibrils (TEMPO-CNF) with the soluble plant-cell-wall polysaccharide, mixed-linkage β-glucan (MLG). Of particular note, gel formation was rapidly induced by very small amounts of MLG (e.g. 0.125% w/v) at extremely low TEMPO-CNF concentration (0.05% w/v), which independently were otherwise fluid and thus easily handled. Rheology of these bionanocomposite gel systems as a function of MLG and TEMPO-CNF concentrations revealed that the critical gel concentration of MLG and TEMPO-CNF followed a power-law relation of the concentration of the other component. Surprisingly, these systems also exhibited an additional transition to thick gels at high TEMPO-CNF and MLG concentrations that was visible only at low frequencies. Cryogenic scanning electron microscopy (cryo-SEM) imaging of admixture solutions and gels revealed increased network crowding with increasing MLG amounts. The data are consistent with the hypothesis that non-covalent cellulose-MLG interactions, analogous to those occurring within plant cell walls, drive gel formation. The ability to tune gel physical properties simply by controlling CNF (a promising forest bioproduct) and MLG (a readily available agricultural polysaccharide) fractions at very low solid and polymer content opens new possibilities for material applications in diverse industries.

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