Effect of fluoride concentration in pH 4.3 and pH 7.0 supersaturated solutions on the crystal growth of hydroxyapatite

Haneol Shin; Sung-Ho Park; Jeong-Won Park; Chan-Young Lee

doi:10.5395/rde.2012.37.1.16

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Research Article Effect of fluoride concentration in pH 4.3 and pH 7.0 supersaturated solutions on the crystal growth of hydroxyapatite: Haneol Shin, DDS¹, Sung-Ho Park, DDS, MSD, PhD¹, Jeong-Won Park, DDS, MSD, PhD², Chan-Young Lee, DDS, MSD, DDSc¹; 2012;37(1):-23.
DOI: https://doi.org/10.5395/rde.2012.37.1.16
Published online: March 2, 2012

¹Department of Conservative Dentistry, Yonsei University College of Dentistry, Seoul, Korea.

²Department of Conservative Dentistry, Gangnam Severance Hospital, Yonsei University College of Dentistry, Seoul, Korea.

Correspondence to Chan-Young Lee, DDS, MSD, DDSc. Professor, Department of Conservative Dentistry, Yonsei University College of Dentistry, 50 Yonsei-ro, Seodaemun-gu, Seoul, Korea 120-752. TEL, +82-2-2228-8701; FAX, +82-2-313-7575; chanyoungl@yuhs.ac

• Received: December 17, 2011 • Revised: January 13, 2012 • Accepted: January 20, 2012

©Copyights 2012. The Korean Academy of Conservative Dentistry.

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Abstract
REFERENCES

Abstract

Objectives
Present study was undertaken to investigate the crystal growth onto synthetic hydroxyapatite (HA) seeds in pH 4.3 and pH 7.0 supersaturated solutions with different fluoride concentrations.
Materials and Methods
8 groups of pH 4.3 and 7.0 calcium phosphate supersaturated solutions were prepared with different fluoride concentrations (0, 1, 2 and 4 ppm). Calcium phosphate precipitates yield crystal growth onto the HA seed surface while solutions flow. For evaluation of crystallizing process, the changes of Ca²⁺, PO₄^3-, F^- concentrations of the inlet and outlet solutions were determined. The recovered solid samples were weighed to assess the amount of minerals precipitated, and finally determined their composition to deduce characteristics of crystals.
Results
During the seeded crystal growth, there were significantly more consumption of Ca²⁺, PO₄^3-, F^- in pH 4.3 solutions than pH 7.0 (p < 0.05). As fluoride concentration increased in pH 4.3 solution, Ca²⁺, PO₄^3-, F^- consumption in experimental solutions, weight increment of HA seed, and fluoride ratio in crystallized samples were increased. There were significant differences among the groups (p < 0.05). But in pH 7.0 solution, these phenomena were not significant. In pH 7.0 solutions, analyses of crystallized samples showed higher Ca/P ratio in higher fluoride concentration. There were significant differences among the groups (p < 0.05). But in pH 4.3 solution, there were not significant differences in Ca/P ratio.
Conclusions
Crystal growth in pH 4.3 solutions was superior to that in pH 7.0 solutions. In pH 4.3 solutions, crystal growth increased with showed in higher fluoride concentration up to 4 ppm.
Keywords: Fluoride concentration; Hydroxyapatite; pH; Seeded crystal growth

Figure 1

Schematic illustration of experimental set-up.

Figure 2

Schematic illustrations of calculating the amounts of crystal growth. (a) Amounts of seed crystals oriinally placed in the reaction column; (b) Weighed amounts of solid sampe recovered at the end of experiment; (b)-(a) Difference between (b) and (a), amounts of crystal growth.

Table 1

Initial composition of experimental solutions

Table 2

Changes in compositions of the experimental solution after experiments (Mean ± SD, n = 10)

SD, standard deviation; NM, not measurable, no fluoride was added to the experimental solutions.

Different letters denote statistically different (p < 0.05).

Table 3

Weight increments of the HA seed after crystal growth (Mean ± SD, n = 10)

SD, standard deviation.

Different letters denote statistically different (p < 0.05).

Table 4

Molecular ratio in crystallized samples (Mean ± SD, n = 10)

SD, standard deviation.

^*1 sample is missed in two groups (groups 6 and 8, n = 9).

Different letters denote statistically different (p < 0.05).

REFERENCES

1. Margolis HC, Moreno EC. Kinetic and thermodynamic aspects of enamel demineralization. Caries Res. 1985;19: 22-35.Article PubMed
2. Aoba T. Solubility properties of human tooth mineral and pathogenesis of dental caries. Oral Dis. 2004;10: 249-257.Article PubMed
3. Robinson C, Brookes SJ, Bonass WA, Shore RC, Kirkham J. Enamel maturation. Ciba Found Symp. 1997;205: 156-170.Article PubMed
4. Nancollas GH, Mohan MS. The growth of hydroxyapatite crystals. Arch Oral Biol. 1970;15: 731-745.Article PubMed
5. Aoba T, Moreno EC. Preparation of hydroxyapatite crystals and their behavior as seeds for crystal growth. J Dent Res. 1984;63: 874-880.Article PubMed PDF
6. Barone JP, Nancollas GH, Tomson M. The seeded growth of calcium phosphates. The kinetics of growth of dicalcium phosphate dihydrate on hydroxyapatite. Calcif Tissue Res. 1976;21: 171-182.Article PubMed PDF
7. Eanes ED. The influence of fluoride on the seeded growth of apatite from stable supersaturated solutions at pH 7.4. J Dent Res. 1980;59: 144-150.Article PubMed PDF
8. Mura-Galelli MJ, Narusawa H, Shimada T, Iijima M, Aoba T. Effects of fluoride on precipitation and hydrolysis of octacalcium phosphate in an experimental model simulating enamel mineralization during amelogenesis. Cells Mater. 1992;2: 221-230.
9. Kwun JW, Kim KY, Lee SJ, Jung IY, Lee CY. The effect of the supersaturated solutions containing high concentrations of fluoride on seeded crystal growth. J Korean Acad Conserv Dent. 1999;24: 330-336.
10. Lee CY, Aoba T. Seeded crystal growth onto enamal mineral and synthetic hydroxyapatite in dilute supersaturated solutions containing low concentration of fluoride. J Korean Acad Conserv Dent. 1995;20: 818-826.
11. Oh SY, Jung IY, Kum KY, Lee CY. Effects of fluoride concentration and seed material on seeded crystal growth. J Korean Acad Conserv Dent. 1997;22: 560-574.
12. Iijima M, Moradian-Oldak J. Control of apatite crystal growth in a fluoride containing amelogenin-rich matrix. Biomaterials. 2005;26: 1595-1603.Article PubMed
13. Fan Y, Nelson JR, Alvarez JR, Hagan J, Berrier A, Xu X. Amelogenin-assisted ex vivo remineralization of human enamel: effects of supersaturation degree and fluoride concentration. Acta Biomater. 2011;7: 2293-2302.PubMed PMC
14. Matsumoto T, Okazaki M, Inoue M, Sasaki J, Hamada Y, Takahashi J. Role of acidic amino acid for regulating hydroxyapatite crystal growth. Dent Mater J. 2006;25: 360-364.Article PubMed
15. Iijima M, Tohda H, Suzuki H, Yanagisawa T, Moriwaki Y. Effects of F- on apatite-octacalcium phosphate intergrowth and crystal morphology in a model system of tooth enamel formation. Calcif Tissue Int. 1992;50: 357-361.Article PubMed PDF
16. Aoba T. The effect of fluoride on apatite structure and growth. Crit Rev Oral Biol Med. 1997;8: 136-153.Article PubMed PDF
17. Elliot JC. Studies in inorganic chemistry: structure and chemistry of the apatites and other calcium orthophosphates. 1994;Amsterdam: Elsevier; 111.
18. Robinson C, Connell S, Kirkham J, Brookes SJ, Shore RC, Smith AM. The effect of fluoride on the developing tooth. Caries Res. 2004;38: 268-276.PubMed
19. Yanagisawa T, Takuma S, Tohda H, Fejerskov O, Fearnhead RW. High resolution electron microscopy of enamel crystals in cases of human dental fluorosis. J Electron Microsc (Tokyo). 1989;38: 441-448.PubMed
20. Amjad Z, Nancollas GH. Effect of fluoride on the growth of hydroxyapatite and human dental enamel. Caries Res. 1979;13: 250-258.Article PubMed
21. Cate JM, Arends J. Remineralization of artificial enamel lesions in vitro. Caries Res. 1977;11: 277-286.Article PubMed
22. Han WS, Kum KY, Lee CY. The influence of fluoride on remineralization of artificial dental caries. J Korean Acad Conserv Dent. 1996;21: 161-173.
23. Lammers PC, Borggreven JM, Driessens FC. Influence of fluoride on in vitro remineralization of artificial subsurface lesions determined with a sandwich technique. Caries Res. 1990;24: 81-85.Article PubMed
24. Feagin F, Patel PR, Koulourides T, Pigman W. Study of the effect of calcium, phosphate, fluoride and hydrogen ion concentrations on the remineralization of partially demineralized human and bovine enamel surfaces. Arch Oral Biol. 1971;16: 535-548.Article PubMed
25. Featherstone JD, Rodgers BE, Smith MW. Physicochemical requirements for rapid remineralization of early carious lesions. Caries Res. 1981;15: 221-235.Article PubMed
26. Kim MK, Kum KY, Lee CY. The influence of pH on remineralization of artificial dental caries. J Korean Acad Conserv Dent. 1997;22: 193-208.
27. Kwon JW, Suh DG, Song YJ, Lee Y, Lee CY. The effect of lactic acid concentration and pH of lactic acid buffer solutions on enamel remineralization. J Korean Acad Conserv Dent. 2008;33: 507-517.Article
28. Yamazaki H, Margolis HC. Enhanced enamel remineralization under acidic conditions in vitro. J Dent Res. 2008;87: 569-574.Article PubMed PDF
29. Song YJ. Development of diffusion pathway in the initial enamel caries lesion. 2009;Graduate School of Yonsei University; Doctoral Dissertation.
30. Song SC. Effect of fluoride on remineralization of artificial enamel caries in pH 4.3 and pH 7.0 remineralized solution. 2011;Graduate School of Yonsei University; Doctoral Dissertation.
31. Kwak YJ, Kim ES, Park SH, Gong HK, Lee Y, Lee CY. The remineralizing features of pH 5.5 solutions of different degree of saturations on artifically demineralized enamel. J Korean Acad Conserv Dent. 2008;33: 481-492.Article
32. Yi JS, Roh BD, Shin SJ, Lee Y, Kong HK, Lee CY. The dynamic change of artificially demineralized enamel by degree of saturation of remineralization soultion at pH 4.3. J Korean Acad Conserv Dent. 2009;34: 20-29.
33. Park JS, Park SH, Park JW, Lee CY. The remineralization aspect of enamel according to change of the degree of saturation of the organic acid buffering solution in pH 5.5. J Korean Acad Conserv Dent. 2010;35: 96-105.Article
34. Eanes ED, Meyer JL. The influence of fluoride on apatite formation from unstable supersaturated solutions at pH 7.4. J Dent Res. 1978;57: 617-624.Article PubMed PDF
35. LeGeros RZ. Calcium phosphates in oral biology and medicine. Monogr Oral Sci. 1991;15: 1-201.PubMed
36. Nelson DG, Featherstone JD, Duncan JF, Cutress TW. Effect of carbonate and fluoride on the dissolution behaviour of synthetic apatites. Caries Res. 1983;17: 200-211.PubMed
37. Wu W, Nancollas GH. Determination of interfacial tension from crystallization and dissolution data: a comparison with other methods. Adv Colloid Interface Sci. 1999;79: 229-279.Article PubMed
38. Barone JP, Nancollas GH. The growth of calcium phosphates on hydroxyapatite crystals. The effect of fluoride and phosphonate. J Dent Res. 1978;57: 735-742.Article PubMed PDF

Tables & Figures

Figure 1

Schematic illustration of experimental set-up.

Figure 2

Table 1

Initial composition of experimental solutions

Table 2

Changes in compositions of the experimental solution after experiments (Mean ± SD, n = 10)

SD, standard deviation; NM, not measurable, no fluoride was added to the experimental solutions.

Different letters denote statistically different (p < 0.05).

Table 3

Weight increments of the HA seed after crystal growth (Mean ± SD, n = 10)

SD, standard deviation.

Different letters denote statistically different (p < 0.05).

Table 4

Molecular ratio in crystallized samples (Mean ± SD, n = 10)

SD, standard deviation.

^*1 sample is missed in two groups (groups 6 and 8, n = 9).

Different letters denote statistically different (p < 0.05).

REFERENCES

1. Margolis HC, Moreno EC. Kinetic and thermodynamic aspects of enamel demineralization. Caries Res. 1985;19: 22-35.Article PubMed
2. Aoba T. Solubility properties of human tooth mineral and pathogenesis of dental caries. Oral Dis. 2004;10: 249-257.Article PubMed
3. Robinson C, Brookes SJ, Bonass WA, Shore RC, Kirkham J. Enamel maturation. Ciba Found Symp. 1997;205: 156-170.Article PubMed
4. Nancollas GH, Mohan MS. The growth of hydroxyapatite crystals. Arch Oral Biol. 1970;15: 731-745.Article PubMed
5. Aoba T, Moreno EC. Preparation of hydroxyapatite crystals and their behavior as seeds for crystal growth. J Dent Res. 1984;63: 874-880.Article PubMed PDF
6. Barone JP, Nancollas GH, Tomson M. The seeded growth of calcium phosphates. The kinetics of growth of dicalcium phosphate dihydrate on hydroxyapatite. Calcif Tissue Res. 1976;21: 171-182.Article PubMed PDF
7. Eanes ED. The influence of fluoride on the seeded growth of apatite from stable supersaturated solutions at pH 7.4. J Dent Res. 1980;59: 144-150.Article PubMed PDF
8. Mura-Galelli MJ, Narusawa H, Shimada T, Iijima M, Aoba T. Effects of fluoride on precipitation and hydrolysis of octacalcium phosphate in an experimental model simulating enamel mineralization during amelogenesis. Cells Mater. 1992;2: 221-230.
9. Kwun JW, Kim KY, Lee SJ, Jung IY, Lee CY. The effect of the supersaturated solutions containing high concentrations of fluoride on seeded crystal growth. J Korean Acad Conserv Dent. 1999;24: 330-336.
10. Lee CY, Aoba T. Seeded crystal growth onto enamal mineral and synthetic hydroxyapatite in dilute supersaturated solutions containing low concentration of fluoride. J Korean Acad Conserv Dent. 1995;20: 818-826.
11. Oh SY, Jung IY, Kum KY, Lee CY. Effects of fluoride concentration and seed material on seeded crystal growth. J Korean Acad Conserv Dent. 1997;22: 560-574.
12. Iijima M, Moradian-Oldak J. Control of apatite crystal growth in a fluoride containing amelogenin-rich matrix. Biomaterials. 2005;26: 1595-1603.Article PubMed
13. Fan Y, Nelson JR, Alvarez JR, Hagan J, Berrier A, Xu X. Amelogenin-assisted ex vivo remineralization of human enamel: effects of supersaturation degree and fluoride concentration. Acta Biomater. 2011;7: 2293-2302.PubMed PMC
14. Matsumoto T, Okazaki M, Inoue M, Sasaki J, Hamada Y, Takahashi J. Role of acidic amino acid for regulating hydroxyapatite crystal growth. Dent Mater J. 2006;25: 360-364.Article PubMed
15. Iijima M, Tohda H, Suzuki H, Yanagisawa T, Moriwaki Y. Effects of F- on apatite-octacalcium phosphate intergrowth and crystal morphology in a model system of tooth enamel formation. Calcif Tissue Int. 1992;50: 357-361.Article PubMed PDF
16. Aoba T. The effect of fluoride on apatite structure and growth. Crit Rev Oral Biol Med. 1997;8: 136-153.Article PubMed PDF
17. Elliot JC. Studies in inorganic chemistry: structure and chemistry of the apatites and other calcium orthophosphates. 1994;Amsterdam: Elsevier; 111.
18. Robinson C, Connell S, Kirkham J, Brookes SJ, Shore RC, Smith AM. The effect of fluoride on the developing tooth. Caries Res. 2004;38: 268-276.PubMed
19. Yanagisawa T, Takuma S, Tohda H, Fejerskov O, Fearnhead RW. High resolution electron microscopy of enamel crystals in cases of human dental fluorosis. J Electron Microsc (Tokyo). 1989;38: 441-448.PubMed
20. Amjad Z, Nancollas GH. Effect of fluoride on the growth of hydroxyapatite and human dental enamel. Caries Res. 1979;13: 250-258.Article PubMed
21. Cate JM, Arends J. Remineralization of artificial enamel lesions in vitro. Caries Res. 1977;11: 277-286.Article PubMed
22. Han WS, Kum KY, Lee CY. The influence of fluoride on remineralization of artificial dental caries. J Korean Acad Conserv Dent. 1996;21: 161-173.
23. Lammers PC, Borggreven JM, Driessens FC. Influence of fluoride on in vitro remineralization of artificial subsurface lesions determined with a sandwich technique. Caries Res. 1990;24: 81-85.Article PubMed
24. Feagin F, Patel PR, Koulourides T, Pigman W. Study of the effect of calcium, phosphate, fluoride and hydrogen ion concentrations on the remineralization of partially demineralized human and bovine enamel surfaces. Arch Oral Biol. 1971;16: 535-548.Article PubMed
25. Featherstone JD, Rodgers BE, Smith MW. Physicochemical requirements for rapid remineralization of early carious lesions. Caries Res. 1981;15: 221-235.Article PubMed
26. Kim MK, Kum KY, Lee CY. The influence of pH on remineralization of artificial dental caries. J Korean Acad Conserv Dent. 1997;22: 193-208.
27. Kwon JW, Suh DG, Song YJ, Lee Y, Lee CY. The effect of lactic acid concentration and pH of lactic acid buffer solutions on enamel remineralization. J Korean Acad Conserv Dent. 2008;33: 507-517.Article
28. Yamazaki H, Margolis HC. Enhanced enamel remineralization under acidic conditions in vitro. J Dent Res. 2008;87: 569-574.Article PubMed PDF
29. Song YJ. Development of diffusion pathway in the initial enamel caries lesion. 2009;Graduate School of Yonsei University; Doctoral Dissertation.
30. Song SC. Effect of fluoride on remineralization of artificial enamel caries in pH 4.3 and pH 7.0 remineralized solution. 2011;Graduate School of Yonsei University; Doctoral Dissertation.
31. Kwak YJ, Kim ES, Park SH, Gong HK, Lee Y, Lee CY. The remineralizing features of pH 5.5 solutions of different degree of saturations on artifically demineralized enamel. J Korean Acad Conserv Dent. 2008;33: 481-492.Article
32. Yi JS, Roh BD, Shin SJ, Lee Y, Kong HK, Lee CY. The dynamic change of artificially demineralized enamel by degree of saturation of remineralization soultion at pH 4.3. J Korean Acad Conserv Dent. 2009;34: 20-29.
33. Park JS, Park SH, Park JW, Lee CY. The remineralization aspect of enamel according to change of the degree of saturation of the organic acid buffering solution in pH 5.5. J Korean Acad Conserv Dent. 2010;35: 96-105.Article
34. Eanes ED, Meyer JL. The influence of fluoride on apatite formation from unstable supersaturated solutions at pH 7.4. J Dent Res. 1978;57: 617-624.Article PubMed PDF
35. LeGeros RZ. Calcium phosphates in oral biology and medicine. Monogr Oral Sci. 1991;15: 1-201.PubMed
36. Nelson DG, Featherstone JD, Duncan JF, Cutress TW. Effect of carbonate and fluoride on the dissolution behaviour of synthetic apatites. Caries Res. 1983;17: 200-211.PubMed
37. Wu W, Nancollas GH. Determination of interfacial tension from crystallization and dissolution data: a comparison with other methods. Adv Colloid Interface Sci. 1999;79: 229-279.Article PubMed
38. Barone JP, Nancollas GH. The growth of calcium phosphates on hydroxyapatite crystals. The effect of fluoride and phosphonate. J Dent Res. 1978;57: 735-742.Article PubMed PDF

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Qualitative analysis on crystal growth of synthetic hydroxyapatite influenced by fluoride concentration
Sumi Kang, Jeong Taeg Seo, Sung-Ho Park, Il Young Jung, Chan Young Lee, Jeong-Won Park
Archives of Oral Biology.2019; 104: 52. CrossRef

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Effect of fluoride concentration in pH 4.3 and pH 7.0 supersaturated solutions on the crystal growth of hydroxyapatite

Restor Dent Endod. 2012;37(1):16-23. Published online March 2, 2012

DOI: https://doi.org/10.5395/rde.2012.37.1.16

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Figure

Effect of fluoride concentration in pH 4.3 and pH 7.0 supersaturated solutions on the crystal growth of hydroxyapatite

Figure 1 Schematic illustration of experimental set-up.

Figure 2 Schematic illustrations of calculating the amounts of crystal growth. (a) Amounts of seed crystals oriinally placed in the reaction column; (b) Weighed amounts of solid sampe recovered at the end of experiment; (b)-(a) Difference between (b) and (a), amounts of crystal growth.

Figure 1

Figure 2

Effect of fluoride concentration in pH 4.3 and pH 7.0 supersaturated solutions on the crystal growth of hydroxyapatite

Table 1

Initial composition of experimental solutions

Table 2

Changes in compositions of the experimental solution after experiments (Mean ± SD, n = 10)

SD, standard deviation; NM, not measurable, no fluoride was added to the experimental solutions.

Different letters denote statistically different (p < 0.05).

Table 3

Weight increments of the HA seed after crystal growth (Mean ± SD, n = 10)

SD, standard deviation.

Different letters denote statistically different (p < 0.05).

Table 4

Molecular ratio in crystallized samples (Mean ± SD, n = 10)

SD, standard deviation.

^*1 sample is missed in two groups (groups 6 and 8, n = 9).

Different letters denote statistically different (p < 0.05).

Table 1 Initial composition of experimental solutions

Table 2 Changes in compositions of the experimental solution after experiments (Mean ± SD, n = 10)

SD, standard deviation; NM, not measurable, no fluoride was added to the experimental solutions.

Different letters denote statistically different (p < 0.05).

Table 3 Weight increments of the HA seed after crystal growth (Mean ± SD, n = 10)

SD, standard deviation.

Different letters denote statistically different (p < 0.05).

Table 4 Molecular ratio in crystallized samples (Mean ± SD, n = 10)

SD, standard deviation.

^*1 sample is missed in two groups (groups 6 and 8, n = 9).

Different letters denote statistically different (p < 0.05).