Monovalent Salt and pH-Induced Gelation of Oxidised Cellulose Nanofibrils and Starch Networks: Combining Rheology and Small-Angle X-ray Scattering

Water quality parameters such as salt content and various pH environments can alter the stability of gels as well as their rheological properties. Here, we investigated the effect of various concentrations of NaCl and different pH environments on the rheological properties of TEMPO-oxidised cellulos...

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Main Authors: Kazi M. Zakir Hossain, Vincenzo Calabrese, Marcelo A. da Silva, Saffron J. Bryant, Julien Schmitt, Jennifer H. Ahn-Jarvis, Frederick J. Warren, Yaroslav Z. Khimyak, Janet L. Scott, Karen J. Edler
Format: Article
Language:English
Published: MDPI AG 2021-03-01
Series:Polymers
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Online Access:https://www.mdpi.com/2073-4360/13/6/951
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author Kazi M. Zakir Hossain
Vincenzo Calabrese
Marcelo A. da Silva
Saffron J. Bryant
Julien Schmitt
Jennifer H. Ahn-Jarvis
Frederick J. Warren
Yaroslav Z. Khimyak
Janet L. Scott
Karen J. Edler
author_facet Kazi M. Zakir Hossain
Vincenzo Calabrese
Marcelo A. da Silva
Saffron J. Bryant
Julien Schmitt
Jennifer H. Ahn-Jarvis
Frederick J. Warren
Yaroslav Z. Khimyak
Janet L. Scott
Karen J. Edler
author_sort Kazi M. Zakir Hossain
collection DOAJ
description Water quality parameters such as salt content and various pH environments can alter the stability of gels as well as their rheological properties. Here, we investigated the effect of various concentrations of NaCl and different pH environments on the rheological properties of TEMPO-oxidised cellulose nanofibril (OCNF) and starch-based hydrogels. Addition of NaCl caused an increased stiffness of the OCNF:starch (1:1 wt%) blend gels, where salt played an important role in reducing the repulsive OCNF fibrillar interactions. The rheological properties of these hydrogels were unchanged at pH 5.0 to 9.0. However, at lower pH (4.0), the stiffness and viscosity of the OCNF and OCNF:starch gels appeared to increase due to proton-induced fibrillar interactions. In contrast, at higher pH (11.5), syneresis was observed due to the formation of denser and aggregated gel networks. Interactions as well as aggregation behaviour of these hydrogels were explored via ζ-potential measurements. Furthermore, the nanostructure of the OCNF gels was probed using small-angle X-ray scattering (SAXS), where the SAXS patterns showed an increase of slope in the low-q region with increasing salt concentration arising from aggregation due to the screening of the surface charge of the fibrils.
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spelling doaj.art-2e115ee35b6c4bea83e0c381ce37088e2023-11-21T11:13:32ZengMDPI AGPolymers2073-43602021-03-0113695110.3390/polym13060951Monovalent Salt and pH-Induced Gelation of Oxidised Cellulose Nanofibrils and Starch Networks: Combining Rheology and Small-Angle X-ray ScatteringKazi M. Zakir Hossain0Vincenzo Calabrese1Marcelo A. da Silva2Saffron J. Bryant3Julien Schmitt4Jennifer H. Ahn-Jarvis5Frederick J. Warren6Yaroslav Z. Khimyak7Janet L. Scott8Karen J. Edler9Department of Chemistry, University of Bath, Claverton Down, Bath BA2 7AY, UKDepartment of Chemistry, University of Bath, Claverton Down, Bath BA2 7AY, UKDepartment of Chemistry, University of Bath, Claverton Down, Bath BA2 7AY, UKDepartment of Chemistry, University of Bath, Claverton Down, Bath BA2 7AY, UKDepartment of Chemistry, University of Bath, Claverton Down, Bath BA2 7AY, UKFood Innovation and Health, Quadram Institute Bioscience, Norwich Research Park, Norwich NR4 7UQ, UKFood Innovation and Health, Quadram Institute Bioscience, Norwich Research Park, Norwich NR4 7UQ, UKSchool of Pharmacy, University of East Anglia, Norwich NR4 7TJ, UKDepartment of Chemistry, University of Bath, Claverton Down, Bath BA2 7AY, UKDepartment of Chemistry, University of Bath, Claverton Down, Bath BA2 7AY, UKWater quality parameters such as salt content and various pH environments can alter the stability of gels as well as their rheological properties. Here, we investigated the effect of various concentrations of NaCl and different pH environments on the rheological properties of TEMPO-oxidised cellulose nanofibril (OCNF) and starch-based hydrogels. Addition of NaCl caused an increased stiffness of the OCNF:starch (1:1 wt%) blend gels, where salt played an important role in reducing the repulsive OCNF fibrillar interactions. The rheological properties of these hydrogels were unchanged at pH 5.0 to 9.0. However, at lower pH (4.0), the stiffness and viscosity of the OCNF and OCNF:starch gels appeared to increase due to proton-induced fibrillar interactions. In contrast, at higher pH (11.5), syneresis was observed due to the formation of denser and aggregated gel networks. Interactions as well as aggregation behaviour of these hydrogels were explored via ζ-potential measurements. Furthermore, the nanostructure of the OCNF gels was probed using small-angle X-ray scattering (SAXS), where the SAXS patterns showed an increase of slope in the low-q region with increasing salt concentration arising from aggregation due to the screening of the surface charge of the fibrils.https://www.mdpi.com/2073-4360/13/6/951cellulose nanofibrilsstarchrheologySAXSsaltpH
spellingShingle Kazi M. Zakir Hossain
Vincenzo Calabrese
Marcelo A. da Silva
Saffron J. Bryant
Julien Schmitt
Jennifer H. Ahn-Jarvis
Frederick J. Warren
Yaroslav Z. Khimyak
Janet L. Scott
Karen J. Edler
Monovalent Salt and pH-Induced Gelation of Oxidised Cellulose Nanofibrils and Starch Networks: Combining Rheology and Small-Angle X-ray Scattering
Polymers
cellulose nanofibrils
starch
rheology
SAXS
salt
pH
title Monovalent Salt and pH-Induced Gelation of Oxidised Cellulose Nanofibrils and Starch Networks: Combining Rheology and Small-Angle X-ray Scattering
title_full Monovalent Salt and pH-Induced Gelation of Oxidised Cellulose Nanofibrils and Starch Networks: Combining Rheology and Small-Angle X-ray Scattering
title_fullStr Monovalent Salt and pH-Induced Gelation of Oxidised Cellulose Nanofibrils and Starch Networks: Combining Rheology and Small-Angle X-ray Scattering
title_full_unstemmed Monovalent Salt and pH-Induced Gelation of Oxidised Cellulose Nanofibrils and Starch Networks: Combining Rheology and Small-Angle X-ray Scattering
title_short Monovalent Salt and pH-Induced Gelation of Oxidised Cellulose Nanofibrils and Starch Networks: Combining Rheology and Small-Angle X-ray Scattering
title_sort monovalent salt and ph induced gelation of oxidised cellulose nanofibrils and starch networks combining rheology and small angle x ray scattering
topic cellulose nanofibrils
starch
rheology
SAXS
salt
pH
url https://www.mdpi.com/2073-4360/13/6/951
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