Wetting of alginate aerogels, from mesoporous solids to hydrogels: a small-angle scattering analysis

aerogels; Boolean models; gels; scattering data analysis; small-angle scattering; Alginate aerogels; Boolean modeling; Mesoporous solid; Mesoporous structures; Scattering analysis; Scattering data; Scattering data analyse; Small angle scattering; Small-angle neutron scattering; Small-angle scattering; Biochemistry, Genetics and Molecular Biology (all)

Abstract :

[en] Mesoporous polysaccharide aerogels are versatile functional materials for drug delivery and wound dressing devices. The hydration and wetting of these aerogels control their application-related performance, e.g. the release of encapsulated drugs. Reported here is a detailed small-angle neutron scattering (SANS) analysis of the hydration mechanism of a calcium alginate aerogel, based on mathematical modelling of the scattering. The model accounts for the hierarchical structure of the material comprising a mesoporous structure, the solid skeleton of which is made up of water-swollen polymers. At large scale, the mesoporous structure is modelled as a random collection of elongated cylinders, which grow in size as they absorb water and aggregate. The small-scale inner structure of the skeleton is described as a Boolean model of polymer coils, which captures the progressive transition from a dense dry polymer to a fully hydrated gel. Using known physico-chemical characteristics of the alginate, the SANS data are fitted using the size of the cylinders as the only adjustable parameter. The alginate aerogel maintains a nanometre-scale, albeit altered, structure for low water contents but it collapses into micrometre-sized structures when the water content approaches one gram of water per gram of alginate. In addition to the wetting of aerogels, the model might be useful for the small-angle scattering analysis of the supercritical drying of gels.

Disciplines :

Physics
Materials science & engineering
Chemistry

Author, co-author :

Balogh, Zoltán ; HUN-REN-DE Mechanisms of Complex Homogeneous and Heterogeneous Chemical Reactions Research Group, Department of Inorganic Chemistry, University of Debrecen, Debrecen, Hungary ; Doctoral School of Chemistry, University of Debrecen, Debrecen, Hungary ; Neutron Spectroscopy Department, HUN-REN Centre for Energy Research, Budapest, Hungary

Kalmár, József; HUN-REN-DE Mechanisms of Complex Homogeneous and Heterogeneous Chemical Reactions Research Group, Department of Inorganic Chemistry, University of Debrecen, Debrecen, Hungary

Gommes, Cédric ; Université de Liège - ULiège > Department of Chemical Engineering

Language :

English

Title :

Wetting of alginate aerogels, from mesoporous solids to hydrogels: a small-angle scattering analysis

Publication date :

April 2024

Journal title :

Journal of Applied Crystallography

ISSN :

0021-8898

eISSN :

1600-5767

Publisher :

International Union of Crystallography

Volume :

Issue :

Pt 2

Pages :

369 - 379

Peer reviewed :

Peer Reviewed verified by ORBi

Additional URL :

https://journals.iucr.org/j/issues/2024/02/00/jl5081/jl5081.pdf

Funders :

COST - European Cooperation in Science and Technology
F.R.S.-FNRS - Fonds de la Recherche Scientifique

Funding text :

C. J. Gommes is grateful to the Fonds de la Recherche Scientifique (FRS\u2013FNRS, Belgium) for a Research Associate Position and for supporting this work through grant PDR T.0100.22. Part of this work is based on work from AERoGELS COST Action (ref. CA18125) supported by COST (European Cooperation in Science and Technology), in particular through a stay of Z. Balogh in Li\u00E8ge.

Available on ORBi :

since 30 January 2025

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Bibliography

Almásy, L. (2021). J. Surf. Investig. 15, 527–531.
Banerjee, A., De, R. & Das, B. (2022). Carbohydr. Polym. 277, 118855.
Budtova, T. (2023). Springer Handbook of Aerogels, pp. 677–705. Heidelberg: Springer.
Burchard, W. (1977). Macromolecules, 10, 919–927.
Ciccariello, S., Goodisman, J. & Brumberger, H. (1988). J. Appl. Cryst. 21, 117–128.
Debye, P. (1947). J. Phys. Chem. 51, 18–32.
Debye, P., Anderson, H. Jr & Brumberger, H. (1957). J. Appl. Phys. 28, 679–683.
Depta, P. N., Gurikov, P., Schroeter, B., Forgács, A., Kalmár, J., Paul, G., Marchese, L., Heinrich, S. & Dosta, M. (2022). J. Chem. Inf. Model. 62, 49–70.
Dirac, P. A. M. (1943). Approximate Rate of Neutron Multiplication for a Solid of Arbitrary Shape and Uniform Density. Declassified British Report MSD 5/PI. Harwell: UKAEA.
Fanova, A., Sotiropoulos, K., Radulescu, A. & Papagiannopoulos, A. (2024). Polymers, 16, 490.
Feigin, L. & Svergun, D. (1987). Structure Analysis by Small-Angle X-ray and Neutron Scattering. Berlin: Springer.
Forgács, A., Papp, V., Paul, G., Marchese, L., Len, A., Dudás, Z., Fábián, I., Gurikov, P. & Kalmár, J. (2021). Appl. Mater. Interfaces, 13, 2997–3010.
Ganesan, K., Budtova, T., Ratke, L., Gurikov, P., Baudron, V., Preibisch, I., Niemeyer, P., Smirnova, I. & Milow, B. (2018). Materials, 11, 2144.
García-González, C. A., Budtova, T., Durães, L., Erkey, C., Del Gaudio, P., Gurikov, P., Koebel, M., Liebner, F., Neagu, M. & Smirnova, I. (2019). Molecules, 24, 1815.
García-González, C. A., Sosnik, A., Kalmár, J., De Marco, I., Erkey, C., Concheiro, A. & Alvarez-Lorenzo, C. (2021). J. Controlled Release, 332, 40–63.
Gille, W. (2011). Comput. Struct. 89, 2309–2315.
Glatter, O. (2018). Scattering Methods and their Application in Colloid and Interface Science. Amsterdam: Elsevier.
Glatter, O. & Kratky, O. (1982). Small Angle X-ray Scattering. New York: Academic Press.
Gommes, C. J. (2013). J. Appl. Cryst. 46, 493–504.
Gommes, C. J. (2018). Microporous Mesoporous Mater. 257, 62–78.
Gommes, C. J., Jaksch, S. & Frielinghaus, H. (2021). J. Appl. Cryst. 54, 1832–1843.
Gommes, C. J., Jiao, Y., Roberts, A. P. & Jeulin, D. (2020). J. Appl. Cryst. 53, 127–132.
Gommes, C. J., Prieto, G. & de Jongh, P. E. (2016). J. Phys. Chem. C, 120, 1488–1506.
Gommes, C. J. & Roberts, A. P. (2008). Phys. Rev. E, 77, 041409.
Hammouda, B. (2016). J. Res. Natl Inst. Standards, 121, 139.
Hermida-Merino, D., Portale, G., Fields, P., Wilson, R., Bassett, S. P., Jennings, J., Dellar, M., Gommes, C., Howdle, S. M., Vrolijk, B. C. M. & Bras, W. (2014). Rev. Sci. Instrum. 85, 093905.
Herrera, F., Rumi, G., Steinberg, P. Y., Wolosiuk, A. & Angelomé, P. C. (2023). ChemCatChem, 15, e202300490.
Jeulin, D. (2021). Morphological Models of Random Structures. Cham: Springer.
Külcü, I. D. & Rege, A. (2021). Soft Matter, 17, 5278–5283.
Lantuéjoul, C. (2002). Geostatistical Simulations. Berlin: Springer.
Lighthill, M. J. (1958). An Introduction to Fourier Analysis and Generalised Functions, Cambridge Monographs on Mechanics. Cambridge University Press.
Maleki, H., Montes, S., Hayati-Roodbari, N., Putz, F. & Huesing, N. (2018). Appl. Mater. Interfaces, 10, 22718–22730.
Matheron, G. (1967). Éléments pour une Théorie des Milieux Poreux. Paris: Masson.
Mollica, G., Ziarelli, F., Lack, S., Brunel, F. & Viel, S. (2012). Carbohydr. Polym. 87, 383–391.
Ohser, J. & Mücklich, M. (2000). Statistical Analysis of Micro-structures in Materials Science. New York: Springer.
Paraskevopoulou, P., Smirnova, I., Athamneh, T., Papastergiou, M., Chriti, D., Mali, G., Čendak, T., Raptopoulos, G. & Gurikov, P. (2020). RSC Adv. 10, 40843–40852.
Paul, G., Bisio, C., Braschi, I., Cossi, M., Gatti, G., Gianotti, E. & Marchese, L. (2018). Chem. Soc. Rev. 47, 5684–5739.
Pedersen, J. S. (1997). Adv. Colloid Interf. Sci. 70, 171–210.
Pedersen, J. S. & Schurtenberger, P. (1996). Macromolecules, 29, 7602–7612.
Petersen, H. & Weidenthaler, C. (2022). Inorg. Chem. Front. 9, 4244–4271.
Preibisch, I., Niemeyer, P., Yusufoglu, Y., Gurikov, P., Milow, B. & Smirnova, I. (2018). Materials, 11, 1287.
Ratke, L. & Gurikov, P. (2021). The Chemistry and Physics of Aerogels. Cambridge University Press.
Rege, A., Ratke, L., Külcü, D. & Gurikov, P. (2020). J. Non-Cryst. Solids, 531, 119859.
Robinson, A. (2018). Nature, 557, 30.
Salomonsen, T., Jensen, H. M., Larsen, F. H., Steuernagel, S. & Engelsen, S. B. (2009). Food Hydrocolloids, 23, 1579–1586.
Seiffert, S. & Sprakel, J. (2012). Chem. Soc. Rev. 41, 909–930.
Serra, J. (1982). Image Analysis and Mathematical Morphology, Vol. 1. London: Academic Press.
Shibayama, M. (2011). Polym. J. 43, 18–34.
Sivia, D. S. (2011). Elementary Scattering Theory for X-ray and Neutron Users. New York: Oxford University Press.
Smirnova, I., García-González, C. A. & Gurikov, P. (2023). Springer Handbook of Aerogels, pp. 1489–1504. Heidelberg: Springer.
Sonntag, U., Stoyan, D. & Hermann, H. (1981). Phys. Status Solidi A, 68, 281–288.
Sorbier, L., Moreaud, M. & Humbert, S. (2019). J. Appl. Cryst. 52, 1348–1357.
Sperger, D. M., Fu, S., Block, L. H. & Munson, E. J. (2011). J. Pharm. Sci. 100, 3441–3452.
Takeshita, S., Sadeghpour, A., Malfait, W. J., Konishi, A., Otake, K. & Yoda, S. (2019). Biomacromolecules, 20, 2051–2057.
Teixeira, J. (1988). J. Appl. Cryst. 21, 781–785.
Torquato, S. (2002). Random Heterogeneous Materials. New York: Springer.
Wei, Y. & Hore, M. J. A. (2021). J. Appl. Phys. 129, 171101.