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Erosion-Driven Enamel Crystallite Growth Phenomenon at the Tooth Surface In Vitro

  • Kang Rae Cho*
    Kang Rae Cho
    Institute of Tissue Regeneration Engineering, Dankook University, Cheonan 31116, Chungnam, Republic of Korea
    Department of Chemical and Biological Engineering, College of Engineering, Sookmyung Women’s University, Seoul 04310, Republic of Korea
    Department of Energy Engineering/KENTECH Institute for Environmental and Climate Technology, Korea Institute of Energy Technology (KENTECH), Naju 58330, Republic of Korea
    *Email: [email protected]
    More by Kang Rae Cho
  • Seung Bin Jo
    Seung Bin Jo
    Institute of Tissue Regeneration Engineering, Dankook University, Cheonan 31116, Chungnam, Republic of Korea
    More by Seung Bin Jo
  • Bupmo Kim
    Bupmo Kim
    Department of Chemical Engineering & Division of Environmental Science and Engineering, Pohang University of Science and Technology, Pohang 37673, Gyeongbuk, Republic of Korea
    More by Bupmo Kim
  • Wooyul Kim
    Wooyul Kim
    Department of Energy Engineering/KENTECH Institute for Environmental and Climate Technology, Korea Institute of Energy Technology (KENTECH), Naju 58330, Republic of Korea
    More by Wooyul Kim
  • Jeung Hun Park
    Jeung Hun Park
    Andlinger Center for Energy and the Environment, and Department of Chemical and Biological Engineering, Princeton University, Princeton, New Jersey 08544, United States
    Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States
    Department of Chemical Engineering, Columbia University, New York, New York 10027, United States
  • Yunseong Ji
    Yunseong Ji
    Institute of Tissue Regeneration Engineering, Dankook University, Cheonan 31116, Chungnam, Republic of Korea
    Fuel Cell Laboratory, Korea Institute of Energy Research, Daejeon 34129, Republic of Korea
    More by Yunseong Ji
  • Yu Jin Kim
    Yu Jin Kim
    Department of Nanobiomedical Science and BK21 PLUS NBM Global Research Center for Regenerative Medicine, Dankook University, Cheonan 31116, Chungnam, Republic of Korea
    More by Yu Jin Kim
  • Rajendra Kumar Singh
    Rajendra Kumar Singh
    Institute of Tissue Regeneration Engineering, Dankook University, Cheonan 31116, Chungnam, Republic of Korea
  • Jung-Hwan Lee
    Jung-Hwan Lee
    Institute of Tissue Regeneration Engineering, Dankook University, Cheonan 31116, Chungnam, Republic of Korea
    Department of Nanobiomedical Science and BK21 PLUS NBM Global Research Center for Regenerative Medicine, Dankook University, Cheonan 31116, Chungnam, Republic of Korea
    Department of Biomateials Science, College of Dentistry, Dankook University, Cheonan 31116, Chungnam, Republic of Korea
  • , and 
  • Hae-Won Kim*
    Hae-Won Kim
    Institute of Tissue Regeneration Engineering, Dankook University, Cheonan 31116, Chungnam, Republic of Korea
    Department of Nanobiomedical Science and BK21 PLUS NBM Global Research Center for Regenerative Medicine, Dankook University, Cheonan 31116, Chungnam, Republic of Korea
    Department of Biomateials Science, College of Dentistry, Dankook University, Cheonan 31116, Chungnam, Republic of Korea
    *Email: [email protected]
    More by Hae-Won Kim
Cite this: ACS Appl. Bio Mater. 2022, 5, 8, 3753–3765
Publication Date (Web):August 1, 2022
https://doi.org/10.1021/acsabm.2c00247
Copyright © 2022 American Chemical Society

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    Abstract

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    The erosion of tooth enamel is a common oral disease. The erosion pattern and location and the effects of nanoscale chemical composition on the erosion susceptibility of enamel have been well documented. However, the enamel remineralization accompanied by erosion and its underlying physicochemical mechanisms still remain poorly understood. Here, using rat molars selected for its good relevancy to human teeth, we investigated the remineralization behavior of the outermost enamel surface at the nanoscale level during erosion in diluted hydrochloric acid solutions. While particles on the outermost enamel surface that represent the termination of crystallites protruding to the surface from the near-surface core eroded by acid-attack, the lateral-growth of the particles (i.e., the main remineralization picture of the surface enamel) occurred concurrently. Ionic analyses indicate that the particle growth is driven by the local increase in pH near the eroding enamel surface as a result of the combination of the PO43– and CO32– released from the enamel surface with H+. As the pH increases eventually to the equilibrium pH level (∼5.5), a local supersaturation of solute ions is induced, resulting in particle growth. A simple growth model based on the experimental results together with an assumption that the particle growth is a diffusional process suggests that the particle growth rate is controlled by the degree of supersaturation and accommodation site for solute ions, which are affected by the pH of solution eroding the enamel surface. The remineralization mechanism presented by our study can explain how the enamel on being acid-exposed or tooth decay progress by beverage or food can naturally remineralize in the oral cavity and how remineralization can foster different surface topology at the nanoscale, depending on the pH value of etchant before the dental filling material is applied.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsabm.2c00247.

    • Supporting Discussion (Discussion S1), Tables S1 and S2 and Figures S1–S18 explaining the simulated results about the equilibrium species forming from the ionic species dissolved from enamel in the HCl solutions at various pH values (from 1.78 to 5.5) by Visual MINTEQ; optical micrographs of the enamel surfaces of the rat molar exposed to HCl solution of initial pH 1.78 according to etching time; SEM images of the structure of the near-surface core of the rat molar; EDX data of the eroded outermost enamel surfaces of the rat molar; methods to obtain the mean size of enamel particles and groove percentage on the outermost enamel surfaces; sequential liquid-phase AFM images of the enamel surfaces of the rat molar in the HCl solution at pH 4.1 and pH 3.07; optical micrographs and SEM images of the enamel surfaces of the rat molar etched by 18.4 wt % phosphoric acid (H3PO4) solution; SEM images showing the surface nucleation on the template of the enamel surface of rat molars; SEM images of the enamel surfaces of the rat molars in the HCl solutions of initial pH 2.13 and 2.8 with respect to etching time; estimation of the pH of etching solutions containing tooth samples after specific etching time by the pH paper (PDF)

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