Preparation and Characterization of Bioceramic Nanocomposites Based on Hydroxyapatite (HA) and Carboxymethyl Cellulose (CMC)

Annamalai Pratheep Kumar; Kamal Khaja Mohaideen; Sameh A. S. Alariqi; Raj Pal Singh

Macromolecular Research, Vol.18, No.12, 1160-1167, December, 2010

DOI10.1007/s13233-010-1208-3 Export Citation

Preparation and Characterization of Bioceramic Nanocomposites Based on Hydroxyapatite (HA) and Carboxymethyl Cellulose (CMC)

Annamalai Pratheep Kumar^†, Kamal Khaja Mohaideen¹, Sameh A. S. Alariqi², and Raj Pal Singh^†

Division of Polymer Science and Engineering, National Chemical Laboratory, Dr. Homi Bhaba Road, Pune, 411 008, India
¹Physical and Materials Chemistry Division, National Chemical Laboratory, Dr. Homi Bhaba Road, Pune, 411 008, India
²Department of Chemistry, Faculty of Science, University of Taiz, Taiz, Taiz, Republic of Yemen

E-mail:,

We report the synthesis of biomimetic nanocomposites based on carboxymethyl cellulose (CMC) and hydroxyapatite (HA) nanoparticles via a co-precipitation method. Physico-chemical characterization was performed before and after calcination by Fourier transform infrared (FTIR) spectroscopy, solid state 31P nuclear magnetic resonance (NMR) spectroscopy, and thermogravimetric analysis (TGA). The formation of nanocomposites was observed by wide angle X-ray diffraction (WAXD), scanning electron microscopy (SEM) with energy dispersive Xray analysis (EDX), and transmission electron microscopy (TEM). The spectral and crystallographic data indicated the formation of hydroxyapatite in the presence of CMC. They were observed as aggregates of HA nanoparticles and CMC, whose sizes were approximately ~ 260 ± 40 nm. The crystallite size of the hydroxyapatite particles decreased (with 2 wt% 18 ± 3 nm) with increasing CMC content. The morphological aspects of the calcined samples revealed the sintering ability of HA nanoparticles. Nanocomposites of hydroxyapatite nanoparticles that mimic the process of nucleation and growth in nature can be prepared using biomacromolecules such as CMC.

Keywords:biopolymer;hydroxyapatite;cellulose;nanoparticles;X-ray diffraction;particle size.

[References]

Stupp SI, Braun PV, Science, 277(5330), 1242 (1997)
Kokubo T, Kim HM, Kawashita M, Biomaterials, 24, 2161 (2003)
Skrtic D, Antonucci JM, Eanes ED, J. Res. Natl. Inst. Stand. Technol., 108, 167 (2003)
Lowenstam HA, Weiner S, in On Biomineralization, Lowenstam HA, Weiner S, Eds., Oxford University Press, New York, 1989.
Mann S, Nature, 322, 119 (1988)
Berman A, Ahn DJ, Lio A, Salmeron M, Reichert A, Charych D, Science, 269(5223), 515 (1995)
Falini G, Albeck S, Weiner S, Addadi L, Science, 271(5245), 67 (1996)
Doi Y, Horiguchi T, Moriwaki Y, Kitago H, Kajimoto T, Iwayama Y, J. Biomed. Mater. Res., 31, 43 (1996)
Webster TJ, Ergun C, Doremus RH, Siegel RW, Bizios R, Biomaterials, 21, 1803 (2000)
Miyamoto Y, Ishikawa K, Takechi M, Toh T, Yuasa T, Nagayama M, Suzuki K, Biomaterials, 19, 707 (1998)
Lee I, Han SW, Choi HJ, Kim K, Adv. Mater., 13(21), 1617 (2001)
Murugan R, Rao KP, Macromol. Res., 11(1), 14 (2003)
Sheikh FA, Barakat NAM, Kanjwal MA, Park SJ, Park DK, Kim HY, Macromol. Res., 18(1), 59 (2010)
Dumitru S, Vidal PF, Chronet E, in Polysaccharides in medicinal applications, Dumitru S, Ed., Marcel Dekker, New York, 1996, pp. 87-106.
Won CY, Chu CC, in Biomaterials and bioengineering handbook, Wise DL, Ed., Marcel Dekker, New York, 2000, pp. 355-372.
Miyamoto T, Takahashi S, Ito H, Inagaki H, Noishiki Y, J. Biomed. Mater. Res., 23, 125 (1989)
Walton AG, Blackwell J, in Biopolymers, Walton AG, Blackwell J, Eds., Academic Press, New York, 1973, pp. 464-474.
Hutchens SA, Benson RS, Evans BR, O’Neill HM, Rawn CJ, Biomaterials, 27, 4661 (2006)
Heinze T, Koschella A, Macromol. Symp., 223, 13 (2005)
Guo JH, Skinner GW, Harcum WW, Barnum PE, Pharm. Sci. Technol. Today, 1, 254 (1998)
Ebadzadeh T, Sharifi L, J. Am. Ceram. Soc., 91, 3408 (2008)
Zakharov NA, Ezhova ZA, Koval EM, Kalinnikov VT, Chalykh AE, Inorg. Mater., 41, 509 (2005)
Jiang L, Li Y, Wang X, Zhang L, Wen J, Gong M, Carbohydr. Polym., 74, 680 (2008)
Jiang LY, Li YB, Zhang L, Liao JG, J. Mater. Sci. -Mater. Med., 19, 981 (2008)
Markovic M, Fowler BO, Tung MS, J. Res. Natl. Inst. Stand. Technol., 109, 553 (2004)
Holcomb DW, Young RA, Calcif. Tissue Int., 31, 489 (1980)
Botha J, Lee-Thorp J, Sponheimer M, Calcif. Tissue Int., 74, 162 (2004)
Jager C, Welzel T, Meyer-Zaika W, Epple M, Magn. Reson. Chem., 44, 573 (2006)
Murugan R, Ramakrishna S, Biomaterials, 25, 3829 (2004)
Wilson OC, Hull JR, Mater. Sci. Eng. C-Biomimetic Supramol. Syst., 28, 434 (2008)
Mortier A, Lemaitre J, Rouxhet PG, Thermochim. Acta, 143, 265 (1989)
Bohner M, Lemaitre J, Legrand AP, d’Espinose de la Caillerie JBD, Belgrand P, J. Mater. Sci. Mater. Med., 7, 457 (1996)
Klug HP, Alexander LE, X-ray Diffraction Procedures for Polycrystalline and Amorphous Materials, John Wiley & Sons, New York, 1974, p.618.
Bigi A, Incerti A, Roveri N, Foresti-Serantoni E, Mongiorgi R, di Sanseverino LR, Krajewski A, Ravaglioli A, Biomaterials, 1, 140 (1980)
Arita IH, Wilkinson DS, Mondragon MA, Castano VM, Biomaterials, 16, 403 (1995)
Juang HY, Hon MH, Biomaterials, 17, 2059 (1996)
Eshtiagh-Hosseini H, Housaindokht MR, Chahkandi M, Mater. Chem. Phys., 106(2-3), 310 (2007)
Peppas NA, Lustig SR, Ann. NY Acad. Sci., 446, 26 (1985)
Kim HS, Kim JT, Jung YJ, Ryu SC, Son HJ, Kim YG, Macromol. Res., 15(1), 65 (2007)
Depan D, Kumar AP, Singh RP, Acta Biomater., 5, 93 (2009)
Murray CB, Norris DJ, Bawendi MG, J. Am. Chem. Soc., 115, 8706 (1993)
Burda C, Chen XB, Narayanan R, El-Sayed MA, Chem. Rev., 105(4), 1025 (2005)
Otsuka M, Matsuda Y, Suwa Y, Fox JL, Higuchi WI, J. Biomed. Mater. Res., 29, 25 (1995)
Cai Y, Tang R, J. Mater. Chem., 18, 3775 (2008)
Zhang J, Wang Q, Wang A, Acta Biomater., 6, 445 (2010)
Vodouhe C, Guen EL, Garza JM, Francuis G, Dejugnat C, Ogier J, Schaaf P, Voegel JC, Lavelle P, Biomaterials, 27, 4149 (2006)

[Referenced By]

[1] Stupp SI, Braun PV, Science, 277(5330), 1242 (1997)

[2] Kokubo T, Kim HM, Kawashita M, Biomaterials, 24, 2161 (2003)

[3] Skrtic D, Antonucci JM, Eanes ED, J. Res. Natl. Inst. Stand. Technol., 108, 167 (2003)

[4] Lowenstam HA, Weiner S, in On Biomineralization, Lowenstam HA, Weiner S, Eds., Oxford University Press, New York, 1989.

[5] Mann S, Nature, 322, 119 (1988)

[6] Berman A, Ahn DJ, Lio A, Salmeron M, Reichert A, Charych D, Science, 269(5223), 515 (1995)

[7] Falini G, Albeck S, Weiner S, Addadi L, Science, 271(5245), 67 (1996)

[8] Doi Y, Horiguchi T, Moriwaki Y, Kitago H, Kajimoto T, Iwayama Y, J. Biomed. Mater. Res., 31, 43 (1996)

[9] Webster TJ, Ergun C, Doremus RH, Siegel RW, Bizios R, Biomaterials, 21, 1803 (2000)

[10] Miyamoto Y, Ishikawa K, Takechi M, Toh T, Yuasa T, Nagayama M, Suzuki K, Biomaterials, 19, 707 (1998)

[11] Lee I, Han SW, Choi HJ, Kim K, Adv. Mater., 13(21), 1617 (2001)

[12] Murugan R, Rao KP, Macromol. Res., 11(1), 14 (2003)

[13] Sheikh FA, Barakat NAM, Kanjwal MA, Park SJ, Park DK, Kim HY, Macromol. Res., 18(1), 59 (2010)

[14] Dumitru S, Vidal PF, Chronet E, in Polysaccharides in medicinal applications, Dumitru S, Ed., Marcel Dekker, New York, 1996, pp. 87-106.

[15] Won CY, Chu CC, in Biomaterials and bioengineering handbook, Wise DL, Ed., Marcel Dekker, New York, 2000, pp. 355-372.

[16] Miyamoto T, Takahashi S, Ito H, Inagaki H, Noishiki Y, J. Biomed. Mater. Res., 23, 125 (1989)

[17] Walton AG, Blackwell J, in Biopolymers, Walton AG, Blackwell J, Eds., Academic Press, New York, 1973, pp. 464-474.

[18] Hutchens SA, Benson RS, Evans BR, O’Neill HM, Rawn CJ, Biomaterials, 27, 4661 (2006)

[19] Heinze T, Koschella A, Macromol. Symp., 223, 13 (2005)

[20] Guo JH, Skinner GW, Harcum WW, Barnum PE, Pharm. Sci. Technol. Today, 1, 254 (1998)

[21] Ebadzadeh T, Sharifi L, J. Am. Ceram. Soc., 91, 3408 (2008)

[22] Zakharov NA, Ezhova ZA, Koval EM, Kalinnikov VT, Chalykh AE, Inorg. Mater., 41, 509 (2005)

[23] Jiang L, Li Y, Wang X, Zhang L, Wen J, Gong M, Carbohydr. Polym., 74, 680 (2008)

[24] Jiang LY, Li YB, Zhang L, Liao JG, J. Mater. Sci. -Mater. Med., 19, 981 (2008)

[25] Markovic M, Fowler BO, Tung MS, J. Res. Natl. Inst. Stand. Technol., 109, 553 (2004)

[26] Holcomb DW, Young RA, Calcif. Tissue Int., 31, 489 (1980)

[27] Botha J, Lee-Thorp J, Sponheimer M, Calcif. Tissue Int., 74, 162 (2004)

[28] Jager C, Welzel T, Meyer-Zaika W, Epple M, Magn. Reson. Chem., 44, 573 (2006)

[29] Murugan R, Ramakrishna S, Biomaterials, 25, 3829 (2004)

[30] Wilson OC, Hull JR, Mater. Sci. Eng. C-Biomimetic Supramol. Syst., 28, 434 (2008)

[31] Mortier A, Lemaitre J, Rouxhet PG, Thermochim. Acta, 143, 265 (1989)

[32] Bohner M, Lemaitre J, Legrand AP, d’Espinose de la Caillerie JBD, Belgrand P, J. Mater. Sci. Mater. Med., 7, 457 (1996)

[33] Klug HP, Alexander LE, X-ray Diffraction Procedures for Polycrystalline and Amorphous Materials, John Wiley & Sons, New York, 1974, p.618.

[34] Bigi A, Incerti A, Roveri N, Foresti-Serantoni E, Mongiorgi R, di Sanseverino LR, Krajewski A, Ravaglioli A, Biomaterials, 1, 140 (1980)

[35] Arita IH, Wilkinson DS, Mondragon MA, Castano VM, Biomaterials, 16, 403 (1995)

[36] Juang HY, Hon MH, Biomaterials, 17, 2059 (1996)

[37] Eshtiagh-Hosseini H, Housaindokht MR, Chahkandi M, Mater. Chem. Phys., 106(2-3), 310 (2007)

[38] Peppas NA, Lustig SR, Ann. NY Acad. Sci., 446, 26 (1985)

[39] Kim HS, Kim JT, Jung YJ, Ryu SC, Son HJ, Kim YG, Macromol. Res., 15(1), 65 (2007)

[40] Depan D, Kumar AP, Singh RP, Acta Biomater., 5, 93 (2009)

[41] Murray CB, Norris DJ, Bawendi MG, J. Am. Chem. Soc., 115, 8706 (1993)

[42] Burda C, Chen XB, Narayanan R, El-Sayed MA, Chem. Rev., 105(4), 1025 (2005)

[43] Otsuka M, Matsuda Y, Suwa Y, Fox JL, Higuchi WI, J. Biomed. Mater. Res., 29, 25 (1995)

[44] Cai Y, Tang R, J. Mater. Chem., 18, 3775 (2008)

[45] Zhang J, Wang Q, Wang A, Acta Biomater., 6, 445 (2010)

[46] Vodouhe C, Guen EL, Garza JM, Francuis G, Dejugnat C, Ogier J, Schaaf P, Voegel JC, Lavelle P, Biomaterials, 27, 4149 (2006)