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A kinetic approach to the mechanism of formation of mesoporous silica nanoparticles

  • Invited Paper: Nano-structured materials (particles, fibers, colloids, composites, etc.)
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Abstract

The synthesis of mesoporous silica nanoparticles (MSNs), widely investigated for application in nanomedicine, depends on many experimental factors and lacks reproducibility. Furthermore, its mechanism is not fully understood, in particular for the chemistry of the hydrolysis and condensation of tetraethoxysilane (TEOS). We coupled simple pH measurements with light diffusion monitoring directly within the reaction vessel in order to understand the early stages of the synthesis until the formation of nanoparticles. We found that two regimes of hydrolysis can be detected before the nanoparticles are formed. At the turning point, only 28% of the TEOS molecules are singly hydrolyzed and the condensation reaction only starts after the aggregation of the silicate-surfactant micelles. Experimental factors such as stirring strength or presence of carbonates of sodium hydroxide exert a strong influence on the kinetics of MSNs formation and on their size, and must be carefully controlled for reproducibility. Based on all our experimental evidence and on previous literature reports, a formation mechanism was proposed in order to highlight the importance of the interplay between chemical and physicochemical processes in such a complex system.

Graphical Abstract

The synthesis of mesoporous silica nanoparticles was investigated by pH monitoring, which gives valuable complementary information to the currently accepted mechanism.

Highlights

  • pH monitoring coupled with light scattering measurements enable an understanding of the early stages of the synthesis of mesoporous silica nanoparticles promoted by sodium hydroxide.

  • The nucleation of the nanoparticles, the determining step to control their size, occurs within a minute after the initial tetraethoxysilane addition under basic conditions.

  • Two regimes of hydrolysis are observed initially, while the condensation reaction only starts after the nucleation of NPs.

  • Experimental factors such as stirring strength or presence of carbonates in sodium hydroxide must be carefully controlled for reproducibility.

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Acknowledgements

Sabine Douillet and Dr. Jérôme Kieffer (ESRF) are gratefully acknowledged for their help.

Funding

This work was supported by the Agence Nationale de la Recherche (ANR-20-CE09-0017-03).

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Authors and Affiliations

  1. Univ. Grenoble Alpes, CNRS, Grenoble INP, Institut Néel, 38000, Grenoble, France

    Ricardo Alvarado Meza, Tom Santori & Xavier Cattoën

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  1. Ricardo Alvarado Meza
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  2. Tom Santori
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  3. Xavier Cattoën
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Contributions

All authors contributed to the study conception and design. Material preparation, data collection, and analysis were performed by RAM, TS, and XC. The first draft of the manuscript was written by XC and all authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.

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Correspondence to Xavier Cattoën.

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Alvarado Meza, R., Santori, T. & Cattoën, X. A kinetic approach to the mechanism of formation of mesoporous silica nanoparticles. J Sol-Gel Sci Technol (2023). https://doi.org/10.1007/s10971-023-06130-w

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