Understanding heat driven gelation of anionic cellulose nanofibrils: Combining Saturation Transfer Difference (STD) NMR, Small Angle X-ray Scattering (SAXS) and rheology

Vincenzo Calabrese; Juan C. Muñoz-García; Julien Schmitt; Marcelo A. da Silva; Janet L. Scott; Jesús Angulo; Yaroslav Z. Khimyak; Karen J. Edler

doi:10.1016/j.jcis.2018.09.085

Understanding heat driven gelation of anionic cellulose nanofibrils: Combining Saturation Transfer Difference (STD) NMR, Small Angle X-ray Scattering (SAXS) and rheology

Vincenzo Calabrese, Juan C. Muñoz-García, Julien Schmitt, Marcelo A. da Silva, Janet L. Scott, Jesús Angulo, Yaroslav Z. Khimyak, Karen J. Edler

Pharmaceutical Materials and Soft Matter

Research output: Contribution to journal › Article › peer-review

32 Citations (Scopus)

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Abstract

A novel mechanism of heat-triggered gelation for oxidised cellulose nanofibrils (OCNF) is reported. We demonstrate that a synergistic approach combining rheology, small-angle X-ray scattering (SAXS) and saturation transfer difference NMR (STD NMR) experiments enables a detailed characterisation of gelation at different length scales. OCNF dispersions experience an increase in solid-like behaviour upon heating as evidenced by rheological studies, associated with enhanced interfibrillar interactions measured using SAXS. Interactions result in an increased fibrillar overlap and increased population of confined water molecules monitored by STD NMR. In comparison, cationic cellulose nanofibrils (produced by reaction of cellulose with trimethylglycidylammonium chloride) were found to be heat-unresponsive.

Original language	English
Pages (from-to)	205-213
Number of pages	9
Journal	Journal of Colloid and Interface Science
Volume	535
Early online date	25 Sep 2018
DOIs	https://doi.org/10.1016/j.jcis.2018.09.085
Publication status	Published - 1 Feb 2019

Keywords

Water confinement
hydrogel
TEMPO oxidised cellulose
heat induced gelation
saturation transfer difference NMR
SAXS
rheology

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10.1016/j.jcis.2018.09.085Licence: CC BY

Accepted manuscriptAccepted author manuscript, 1.5 MBLicence: CC BY-NC-ND
Calabrese_etal_JColloidInterfaceSciFinal published version, 1.21 MBLicence: CC BY

https://linkinghub.elsevier.com/retrieve/pii/S0021979718311603Licence: CC BY

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Calabrese, V., Muñoz-García, J. C., Schmitt, J., da Silva, M. A., Scott, J. L., Angulo, J., Khimyak, Y. Z., & Edler, K. J. (2019). Understanding heat driven gelation of anionic cellulose nanofibrils: Combining Saturation Transfer Difference (STD) NMR, Small Angle X-ray Scattering (SAXS) and rheology. Journal of Colloid and Interface Science, 535, 205-213. https://doi.org/10.1016/j.jcis.2018.09.085

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abstract = "A novel mechanism of heat-triggered gelation for oxidised cellulose nanofibrils (OCNF) is reported. We demonstrate that a synergistic approach combining rheology, small-angle X-ray scattering (SAXS) and saturation transfer difference NMR (STD NMR) experiments enables a detailed characterisation of gelation at different length scales. OCNF dispersions experience an increase in solid-like behaviour upon heating as evidenced by rheological studies, associated with enhanced interfibrillar interactions measured using SAXS. Interactions result in an increased fibrillar overlap and increased population of confined water molecules monitored by STD NMR. In comparison, cationic cellulose nanofibrils (produced by reaction of cellulose with trimethylglycidylammonium chloride) were found to be heat-unresponsive.",

keywords = "Water confinement, hydrogel, TEMPO oxidised cellulose, heat induced gelation, saturation transfer difference NMR, SAXS, rheology",

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Calabrese, V, Muñoz-García, JC, Schmitt, J, da Silva, MA, Scott, JL, Angulo, J , Khimyak, YZ & Edler, KJ 2019, 'Understanding heat driven gelation of anionic cellulose nanofibrils: Combining Saturation Transfer Difference (STD) NMR, Small Angle X-ray Scattering (SAXS) and rheology', Journal of Colloid and Interface Science, vol. 535, pp. 205-213. https://doi.org/10.1016/j.jcis.2018.09.085

Understanding heat driven gelation of anionic cellulose nanofibrils: Combining Saturation Transfer Difference (STD) NMR, Small Angle X-ray Scattering (SAXS) and rheology. / Calabrese, Vincenzo; Muñoz-García, Juan C.; Schmitt, Julien et al.

In: Journal of Colloid and Interface Science, Vol. 535, 01.02.2019, p. 205-213.

Research output: Contribution to journal › Article › peer-review

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AU - Schmitt, Julien

AU - da Silva, Marcelo A.

AU - Scott, Janet L.

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AU - Khimyak, Yaroslav Z.

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AB - A novel mechanism of heat-triggered gelation for oxidised cellulose nanofibrils (OCNF) is reported. We demonstrate that a synergistic approach combining rheology, small-angle X-ray scattering (SAXS) and saturation transfer difference NMR (STD NMR) experiments enables a detailed characterisation of gelation at different length scales. OCNF dispersions experience an increase in solid-like behaviour upon heating as evidenced by rheological studies, associated with enhanced interfibrillar interactions measured using SAXS. Interactions result in an increased fibrillar overlap and increased population of confined water molecules monitored by STD NMR. In comparison, cationic cellulose nanofibrils (produced by reaction of cellulose with trimethylglycidylammonium chloride) were found to be heat-unresponsive.

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Understanding heat driven gelation of anionic cellulose nanofibrils: Combining Saturation Transfer Difference (STD) NMR, Small Angle X-ray Scattering (SAXS) and rheology

Abstract

Keywords

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Jesus Angulo

Yaroslav Khimyak

Data for: Understanding heat driven gelation of anionic cellulose nanofibrils: Combining saturation transfer difference (STD) NMR, small angle X-ray scattering (SAXS) and rheology

Cite this

Understanding heat driven gelation of anionic cellulose nanofibrils: Combining Saturation Transfer Difference (STD) NMR, Small Angle X-ray Scattering (SAXS) and rheology

Abstract

Keywords

Access to Document

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Jesus Angulo

Yaroslav Khimyak

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Data for: Understanding heat driven gelation of anionic cellulose nanofibrils: Combining saturation transfer difference (STD) NMR, small angle X-ray scattering (SAXS) and rheology

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