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Article

Raman and XANES Spectroscopic Study of the Influence of Coordination Atomic and Molecular Environments in Biomimetic Composite Materials Integrated with Dental Tissue

1
Solid State Physics and Nanostructures Department, Voronezh State University, University sq.1, 394018 Voronezh, Russia
2
Department of Pediatric Dentistry with Orthodontia, Voronezh State Medical University, Studentcheskaya st. 11, 394006 Voronezh, Russia
3
Scientific and Educational Center, Nanomaterials and Nanotechnologies, Ural Federal University, Mir av., 620002 Yekaterinburg, Russia
*
Author to whom correspondence should be addressed.
Academic Editors: May Lei Mei, Sanjukta Deb and Sherif Elsharkawy
Nanomaterials 2021, 11(11), 3099; https://doi.org/10.3390/nano11113099
Received: 22 October 2021 / Revised: 11 November 2021 / Accepted: 15 November 2021 / Published: 16 November 2021
(This article belongs to the Special Issue Nanomaterials in Dentistry)
In this work, for the first time, the influence of the coordination environment as well as Ca and P atomic states on biomimetic composites integrated with dental tissue was investigated. Bioinspired dental composites were synthesised based on nanocrystalline calcium carbonate-substituted hydroxyapatite Ca4ICa6IIPO46xCO3x+yOH2y (nano-cHAp) obtained from a biogenic source and a set of polar amino acids that modelled the organic matrix. Biomimetic composites, as well as natural dental tissue samples, were investigated using Raman spectromicroscopy and synchrotron X-ray absorption near edge structure (XANES) spectroscopy. Molecular structure and energy structure studies revealed several important features related to the different calcium atomic environments. It was shown that biomimetic composites created in order to reproduce the physicochemical properties of dental tissue provide good imitation of molecular and electron energetic properties, including the carbonate anion CO32− and the atomic Ca/P ratio in nanocrystals. The features of the molecular structure of biomimetic composites are inherited from the nano-cHAp (to a greater extent) and the amino acid cocktail used for their creation, and are caused by the ratio between the mineral and organic components, which is similar to the composition of natural enamel and dentine. In this case, violation of the nano-cHAp stoichiometry, which is the mineral basis of the natural and bioinspired composites, as well as the inclusion of different molecular groups in the nano-cHAp lattice, do not affect the coordination environment of phosphorus atoms. The differences observed in the molecular and electron energetic structures of the natural enamel and dentine and the imitation of their properties by biomimetic materials are caused by rearrangement in the local environment of the calcium atoms in the HAp crystal lattice. The surface of the nano-cHAp crystals in the natural enamel and dentine involved in the formation of bonds with the organic matrix is characterised by the coordination environment of the calcium atom, corresponding to its location in the CaI position—that is, bound through common oxygen atoms with PO4 tetrahedrons. At the same time, on the surface of nano-cHAp crystals in bioinspired dental materials, the calcium atom is characteristically located in the CaII position, bound to the hydroxyl OH group. The features detected in the atomic and molecular coordination environment in nano-cHAp play a fundamental role in recreating a biomimetic dental composite of the natural organomineral interaction in mineralised tissue and will help to find an optimal way to integrate the dental biocomposite with natural tissue. View Full-Text
Keywords: biomimetic dental nanocomposites; mineralised tissue; enamel; dentine; Raman spectromicroscopy; XANES biomimetic dental nanocomposites; mineralised tissue; enamel; dentine; Raman spectromicroscopy; XANES
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MDPI and ACS Style

Goloshchapov, D.; Buylov, N.; Emelyanova, A.; Ippolitov, I.; Ippolitov, Y.; Kashkarov, V.; Khudyakov, Y.; Nikitkov, K.; Seredin, P. Raman and XANES Spectroscopic Study of the Influence of Coordination Atomic and Molecular Environments in Biomimetic Composite Materials Integrated with Dental Tissue. Nanomaterials 2021, 11, 3099. https://doi.org/10.3390/nano11113099

AMA Style

Goloshchapov D, Buylov N, Emelyanova A, Ippolitov I, Ippolitov Y, Kashkarov V, Khudyakov Y, Nikitkov K, Seredin P. Raman and XANES Spectroscopic Study of the Influence of Coordination Atomic and Molecular Environments in Biomimetic Composite Materials Integrated with Dental Tissue. Nanomaterials. 2021; 11(11):3099. https://doi.org/10.3390/nano11113099

Chicago/Turabian Style

Goloshchapov, Dmitry, Nikita Buylov, Anna Emelyanova, Ivan Ippolitov, Yuri Ippolitov, Vladimir Kashkarov, Yuri Khudyakov, Kirill Nikitkov, and Pavel Seredin. 2021. "Raman and XANES Spectroscopic Study of the Influence of Coordination Atomic and Molecular Environments in Biomimetic Composite Materials Integrated with Dental Tissue" Nanomaterials 11, no. 11: 3099. https://doi.org/10.3390/nano11113099

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