Engineering of a Biomimetic Interface between a Native Dental Tissue and Restorative Composite and Its Study Using Synchrotron FTIR Microscopic Mapping

Seredin, P. V.; Goloshchapov, D. L.; Ippolitov, Yuri; Vongsvivut, Jitraporn

doi:10.3390/ijms22126510

Cited by 15 publications

(31 citation statements)

References 51 publications

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“…In addition, as it is noted in [ 43 , 45 , 46 , 47 ], the activity of amino acid side chains can be determined from their vibrational spectra and they represent the conformational changes of molecules in different environments. Therefore, the use of FTIR spectroscopy, sensitive to molecular transformations, is to study the mechanisms of conjugation of proteins and mineral components in biocomposites to be optimal [ 40 , 48 , 49 ].…”

Section: Resultsmentioning

confidence: 99%

“…FTIR absorption spectra of the composites in the range 4500–400 cm −1 . and spectral resolution of 2 cm −1 were recorded at the Infrared Microspectroscopy (IRM) beamline (Australian synchrotron, Clayton, VIC, Australia) using a Bruker Vertex 80v spectrometer coupled with a Hyperion 2000 FTIR microscope and a liquid nitrogen-cooled narrow-band mercury cadmium telluride (MCT) detector (Bruker Optik, Germany) [ 38 , 39 , 40 ]. Blackman-Harris 3-term apodization, Mertz phase correction, and a zero-filling factor of 2 were set as default acquisition parameters using the OPUS 7.2 software suite (Bruker Optik, Germany).…”

Section: Methodsmentioning

confidence: 99%

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Investigation of the Effect of Nanocrystalline Calcium Carbonate-Substituted Hydroxyapatite and L-Lysine and L-Arginine Surface Interactions on the Molecular Properties of Dental Biomimetic Composites

et al. 2021

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Differences in the surface interactions of non-stoichiometric nanocrystalline B-type carbonate-substituted hydroxyapatite (n-cHAp) with the amino acids L-Lysine hydrochloride (L-LysHCl) and L-Arginine hydrochloride (L-ArgHCl) in acidic and alkaline media were determined using structural and spectroscopic analysis methods. The obtained data confirm that hydroxyapatite synthesized using our technique, which was used to develop the n-cHAp/L-LysHCl and n-cHAp/L-ArgHCl composites, is nanocrystalline. Studies of molecular composition of the samples by Fourier transform infrared spectroscopy under the change in the charge state of L-Lysine in environments with different alkalinity are consistent with the results of X-ray diffraction analysis, as evidenced by the redistribution of the modes’ intensities in the spectra that is correlated with the side chains, i.e., amide and carboxyl groups, of the amino acid. During the formation of a biomimetic composite containing L-Lysine hydrochloride and n-cHAp, the interaction occurred through bonding of the L-Lysine side chain and the hydroxyl groups of hydroxyapatite, which created an anionic form of L-Lysine at pH ≤ 5. In contrast, in biocomposites based on L-Arginine and n-cHAp, the interaction only slightly depends on pH value, and it proceeds by molecular orientation mechanisms. The X-ray diffraction and infrared spectroscopy results confirm that changes in the molecular composition of n-cHAp/L-ArgHCl biomimetic composites are caused by the electrostatic interaction between the L-ArgHCl molecule and the carbonate-substituted calcium hydroxyapatite. In this case, the bond formation was detected by Fourier transform infrared (FTIR) spectroscopy; the vibrational modes attributed to the main carbon chain and the guanidine group of L-Arginine are shifted during the interaction. The discovered interaction mechanisms between nanocrystalline carbonate-substituted hydroxyapatite that has physicochemical properties characteristic of the apatite in human dental enamel and specific amino acids are important for selecting the formation conditions of biomimetic composites and their integration with the natural dental tissue.

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Section: Resultsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Investigation of the Effect of Nanocrystalline Calcium Carbonate-Substituted Hydroxyapatite and L-Lysine and L-Arginine Surface Interactions on the Molecular Properties of Dental Biomimetic Composites

et al. 2021

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“…The speed was reduced when the dentine was reached. The cavity formed in the tooth was treated according to the technique described in our previous work [5]. Then, the C D composite was applied to the dentine with universal adhesive, covering the entire area up to the visible edge of the dentin-enamel border and pre-cured with photopolymerisation.…”

Section: Integration Of Natural Dental Tissue and Biomimetic Composites (Treatment)mentioning

confidence: 99%

“…The study of the structure of biologically and artificially formed mineralised tissue has been developed extensively due to the relevance and importance of these data for medicine [1][2][3]. However, advances in restorative and regenerative dentistry, as well as the emergence of the biomimetic approach as a driving force for applied materials science, sometimes require the study of the properties of mineralised human hard tissue at the molecular and atomic level [4,5]. With respect to current medical technologies for dental hard tissue regeneration, it should be noted that despite the tremendous efforts that have been made to restore enamel using a variety of biomedical strategies and biocomposite materials, this task remains difficult [3,6].…”

Section: Introductionmentioning

confidence: 99%

“…With respect to current medical technologies for dental hard tissue regeneration, it should be noted that despite the tremendous efforts that have been made to restore enamel using a variety of biomedical strategies and biocomposite materials, this task remains difficult [3,6]. The solution to enamel restoration involves understanding the molecular mechanisms of organisation and integration of artificial bioinspired materials based on nanocrystalline calcium carbonate-substituted hydroxyapatite (nano-cHAp) and natural tissue; finding the relationship between the inorganic mineral component and the organic matrix within which it was formed; and establishing the atomic ordering at the integration interface [3,5].…”

Section: Introductionmentioning

confidence: 99%

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

et al. 2021

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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 Ca4ICa6IIPO46−xCO3x+yOH2−y (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.

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Probing the micro- and nanoscopic properties of dental materials using infrared spectroscopy: A proof-of-principle study

Beddoe,

Gölz,

Barkey

et al. 2023

Acta Biomaterialia

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Engineering of a Biomimetic Interface between a Native Dental Tissue and Restorative Composite and Its Study Using Synchrotron FTIR Microscopic Mapping

Cited by 15 publications

References 51 publications

Investigation of the Effect of Nanocrystalline Calcium Carbonate-Substituted Hydroxyapatite and L-Lysine and L-Arginine Surface Interactions on the Molecular Properties of Dental Biomimetic Composites

Investigation of the Effect of Nanocrystalline Calcium Carbonate-Substituted Hydroxyapatite and L-Lysine and L-Arginine Surface Interactions on the Molecular Properties of Dental Biomimetic Composites

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

Probing the micro- and nanoscopic properties of dental materials using infrared spectroscopy: A proof-of-principle study

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