Origin of micro-scale heterogeneity in polymerisation of photo-activated resin composites

Slobodan Sirovica; Johanne H. Solheim; Maximilian W. A. Skoda; Carol J. Hirschmugl; Eric C. Mattson; Ebrahim Aboualizadeh; Yilan Guo; Xiaohui Chen; Achim Kohler; Dan L. Romanyk; Scott M. Rosendahl; Suzanne Morsch; Richard A. Martin; Owen Addison

doi:10.1038/s41467-020-15669-z

Origin of micro-scale heterogeneity in polymerisation of photo-activated resin composites

Slobodan Sirovica, Johanne H. Solheim, Maximilian W. A. Skoda, Carol J. Hirschmugl, Eric C. Mattson, Ebrahim Aboualizadeh, Yilan Guo, Xiaohui Chen, Achim Kohler, Dan L. Romanyk, Scott M. Rosendahl, Suzanne Morsch, Richard A. Martin, Owen Addison^*

^*Corresponding author for this work

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

Abstract

Photo-activated resin composites are widely used in industry and medicine. Despite extensive chemical characterisation, the micro-scale pattern of resin matrix reactive group conversion between filler particles is not fully understood. Using an advanced synchrotron-based wide-field IR imaging system and state-of-the-art Mie scattering corrections, we observe how the presence of monodispersed silica filler particles in a methacrylate based resin reduces local conversion and chemical bond strain in the polymer phase. Here we show that heterogeneity originates from a lower converted and reduced bond strain boundary layer encapsulating each particle, whilst at larger inter-particulate distances light attenuation and monomer mobility predominantly influence conversion. Increased conversion corresponds to greater bond strain, however, strain generation appears sensitive to differences in conversion rate and implies subtle distinctions in the final polymer structure. We expect these findings to inform current predictive models of mechanical behaviour in polymer-composite materials, particularly at the resin-filler interface.

Original language	English
Article number	1849
Journal	Nature Communications
Volume	11
Issue number	1
DOIs	https://doi.org/10.1038/s41467-020-15669-z
Publication status	Published - 15 Apr 2020

Bibliographical note

This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.

Funding: S.S. was funded by the Global Challenges Studentship from the Science and Technology Facilities Council (award no. ST/L502510/1).

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Origin of micro-scale heterogeneity
This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.
Final published version, 1.69 MBLicence: CC BY 3.0

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Sirovica, S., Solheim, J. H., Skoda, M. W. A., Hirschmugl, C. J., Mattson, E. C., Aboualizadeh, E., Guo, Y., Chen, X., Kohler, A., Romanyk, D. L., Rosendahl, S. M., Morsch, S., Martin, R. A., & Addison, O. (2020). Origin of micro-scale heterogeneity in polymerisation of photo-activated resin composites. Nature Communications, 11(1), Article 1849. https://doi.org/10.1038/s41467-020-15669-z

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abstract = "Photo-activated resin composites are widely used in industry and medicine. Despite extensive chemical characterisation, the micro-scale pattern of resin matrix reactive group conversion between filler particles is not fully understood. Using an advanced synchrotron-based wide-field IR imaging system and state-of-the-art Mie scattering corrections, we observe how the presence of monodispersed silica filler particles in a methacrylate based resin reduces local conversion and chemical bond strain in the polymer phase. Here we show that heterogeneity originates from a lower converted and reduced bond strain boundary layer encapsulating each particle, whilst at larger inter-particulate distances light attenuation and monomer mobility predominantly influence conversion. Increased conversion corresponds to greater bond strain, however, strain generation appears sensitive to differences in conversion rate and implies subtle distinctions in the final polymer structure. We expect these findings to inform current predictive models of mechanical behaviour in polymer-composite materials, particularly at the resin-filler interface.",

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Origin of micro-scale heterogeneity in polymerisation of photo-activated resin composites

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