Preparation, Characterization and Drug-Release Behaviors of Crosslinked Chitosan/Attapulgite Hybrid Microspheres by a Facile Spray-Drying Technique
ABSTRACT
A series of chitosan/attapulgite (CTS/APT) hybrid microspheres were prepared by a facile spray-drying technique. The developed hybrid microspheres were characterized by Fourier transform infrared spectra (FTIR), X-ray powder diffraction (XRD), scanning electron microscopy (SEM) and the zeta potential. The encapsulation efficiency and in vitro controlled release properties of the microspheres for drug were evaluated using diclofenac sodium (DS) as a model drug. Results indicated that the introduction of APT into crosslinked CTS microspheres can achieve narrow size distribution and make them more uniform. The isoelectric point of the microspheres increased from 8.14 to 9.18 with increasing the content of APT to 10 wt.%. DS loaded in hybrid microspheres is hardly released in simulated gastric fluid, but quickly released in simulated intestinal fluid. The electrostatic interaction between hybrid microspheres and DS can improve the encapsulation efficiency and controlled release behavior of CTS/APT microspheres, and the release mechanism fits Fickian diffusion.
A series of chitosan/attapulgite (CTS/APT) hybrid microspheres were prepared by a facile spray-drying technique. The developed hybrid microspheres were characterized by Fourier transform infrared spectra (FTIR), X-ray powder diffraction (XRD), scanning electron microscopy (SEM) and the zeta potential. The encapsulation efficiency and in vitro controlled release properties of the microspheres for drug were evaluated using diclofenac sodium (DS) as a model drug. Results indicated that the introduction of APT into crosslinked CTS microspheres can achieve narrow size distribution and make them more uniform. The isoelectric point of the microspheres increased from 8.14 to 9.18 with increasing the content of APT to 10 wt.%. DS loaded in hybrid microspheres is hardly released in simulated gastric fluid, but quickly released in simulated intestinal fluid. The electrostatic interaction between hybrid microspheres and DS can improve the encapsulation efficiency and controlled release behavior of CTS/APT microspheres, and the release mechanism fits Fickian diffusion.
Cite this paper
nullQ. Wang, J. Wu, W. Wang and A. Wang, "Preparation, Characterization and Drug-Release Behaviors of Crosslinked Chitosan/Attapulgite Hybrid Microspheres by a Facile Spray-Drying Technique," Journal of Biomaterials and Nanobiotechnology, Vol. 2 No. 3, 2011, pp. 250-257. doi: 10.4236/jbnb.2011.23032.
nullQ. Wang, J. Wu, W. Wang and A. Wang, "Preparation, Characterization and Drug-Release Behaviors of Crosslinked Chitosan/Attapulgite Hybrid Microspheres by a Facile Spray-Drying Technique," Journal of Biomaterials and Nanobiotechnology, Vol. 2 No. 3, 2011, pp. 250-257. doi: 10.4236/jbnb.2011.23032.
References
[1] S. Freiberg and X. X. Zhu, “Polymer microspheres for controlled drug release”, International Journal of Pharmaceutics, Vol. 282, No. 1-2, 2004, pp.1-18. Udoi:10.1016/j.ijpharm.2004.04.013 [2] R.H. Qin, F.S. Li, M.Y. Chen and W. Jiang, “Preparation of chitosan–ethylene diaminetetraacetate-enwrapped magnetic CoFe2O4 nanoparticles via zero-length emulsion crosslinking method”. Applied Surface Science, Vol. 256, No.1, 2009, pp.27-32. [3] A. R. Dudhani and S.L.Kosaraju. “Bioadhesive chitosan nanoparticles: Preparation and characterization”, Carbohydrate Polymers, Vol. 81, No. 2, 2010, pp. 243-251. Udoi:10.1016/j.carbpol.2010.02.026 [4] S.A. Agnihotri and T.M. Aminabhavi, “Controlled release of clozapine through chitosan microparticles prepared by a novel method”, Journal of Controlled Release, Vol. 96, No. 2, 2004, pp. 245-259. Udoi:10.1016/j.jconrel.2004.01.025 [5] D. Chiou and T.A.G. Langrish, “Development and characterisation of novel nutraceuticals with spray drying technology”, Journal of Food Engineering, Vol. 82, No. 1, 2007, pp 84-91. Udoi:10.1016/j.jfoodeng.2007.01.021 [6] L. Ochiuz and J.E. Peris, “Preparation and Characterisation of Alendronate-Loaded Chitosan Microparticles Obtained Through the Spray Drying Technique”, Medicinal Chemistry, Vol. 5, No. 2, 2009, pp. 191-196(6). [7] P. Tewa-Tagne, S. Brian?on and H. Fessi, “Preparation of redispersible dry nanocapsules by means of spray-drying: Development and characterization”, European Journal of Pharmaceutical Sciences, Vol. 30, No. 2, 2007, pp. 124- 135. Udoi:10.1016/j.ejps.2006.10.006 [8] K. Vimala, M. M. Yallapu, K. Varaprasad, N. N. Reddy, S. Ravindra, N. S. Naidu, K. M. Raju, “Fabrication of Curcumin Encapsulated Chitosan-PVA Silver Nanocomposite Films for Improved Antimicrobial Activity”, Journal of Biomaterials and Nanobiotechnology, Vol.2, No.1, 2011, PP. 55-64. Udoi: 10.4236/jbnb.2011.21008 [9] H. Li, C.R. Zhou, J.H. Tian and J.H. Rong, “Preparation and Characterization of Homogeneous Hydroxyapatite/Chitosan Composite Scaffolds via In-Situ Hydration”, Journal of Biomaterials and Nanobiotechnology, Vol.1, No.1, 2010, pp.42-49. doi:10.4236/jbnb.2010.11006 [10] Y. Murata, D. Hirai, K. Kofuji, E. Miyamoto and S. Kawashima, “Properties of an Alginate Gel Bead Containing a Chitosan-Drug Salt”, Biological & Pharmaceutical Bulletin, Vol. 27, No. 3, 2004, pp. 440-442. Udoi:10.1248/bpb.27.440 [11] P. He, S.S. Davis and L. Illum,”Chitosan microspheres prepared by spray drying”, International Journal of Pharmaceutics, Vol. 187, No.1, 1999, pp. 53-65. Udoi:10.1016/S0378-5173(99)00125-8 [12] P. Giunchedi, C. Juliano, E. Gavini, M. Cossu and M. Sorrenti, “Formulation and in vivo evaluation of chlorhexidine buccal tablets prepared using drug-loaded chitosan microspheres”, European Journal of Pharmaceutics and Biopharmaceutics, Vol. 53, No. 2, 2002, pp.233-239. Udoi:10.1016/S0939-6411(01)00237-5 [13] D.O. Corrigan, A.M. Healy and O.I. Corrigan, “Preparation and release of salbutamol from chitosan and chitosan co-spray dried compacts and multiparticulates”, European Journal of Pharmaceutics and Biopharmaceutics, Vol. 62, No.3, 2006, pp. 295-305. Udoi:10.1016/j.ejpb.2005.09.008 [14] A. Alhalaweh, S. Andersson and S.P. Velaga, “Preparation of zolmitriptan–chitosan microparticles by spray drying for nasal delivery”, European Journal of Pharmaceutical Sciences, Vol. 38, No. 3, 2009, pp. 206-214. Udoi:10.1016/j.ejps.2009.07.003 [15] J.P.Zhang, Q. Wang and A.Q. Wang, “In situ generation of sodium alginate/ hydroxyapatite nanocomposite beads as drug-controlled release matrices”, Acta Biomaterialia, Vol.6, No.2, 2010, pp. 445-454. Udoi:10.1016/j.actbio.2009.07.001 [16] M. D. Arco, E. Cebadera, S. Gutiérrez, C. Martín, M.J. Montero, V. Rives, J. Rocha and M.A. Sevilla, “Mg, Al layered double hydroxides with intercalated indomethacin: Synthesis, characterization, and pharmacological study”, Journal of Pharmaceutical Science, Vol. 93, No.6, 2004, pp. 1649-1658. Udoi: 10.1002/jps.20054 [17] Q. Wang, X.L. Xie, X.W. Zhang, J.P. Zhang and A.Q. Wang, “Preparation and swelling properties of pH sensitive composite hydrogel beads based on chitosan-g-poly (acrylic acid)/vermiculite and sodium alginate for diclofenac controlled release”, International Journal of Biological Macromolecules, Vol.46, No.3, 2010, pp. 356- 362. Udoi:10.1016/j.ijbiomac.2010.01.009 [18] M.P.S. Krekeler and S. Guggenheim, “Defects in microstructure in palygorskite–sepiolite minerals: A transmission electron microscopy (TEM) study”, Applied Clay Science, Vol. 39, No. 1-2, 2008, pp. 98-105. Udoi:10.1016/j.clay.2007.05.001 [19] M.J. Fernández-Hervás, M.A. Holgado, A. Fini and J.T. Fell, “In vitro evaluation of alginate beads of diclofenac salts”, International Journal of Pharmaceutics, Vol.163, No. 1-2, 1998, pp. 23-34. Udoi:10.1016/S0378-5173(97)00333-5 [20] A. Lamprecht, N. Ubrich, H. Yamamoto, U. Sch?fer, H. Takeuchi, P. Maincent, Y. Kawashima andC.M. Lehr, “Biodegradable nanoparticles for targeted drug delivery in treatment of inflammatory bowel disease”, The Journal of Pharmacology and Experimental Therapeutics, Vol. 299, No. 2, pp.775-781. [21] A. Lamprecht, U. Schafer and C.M. Lehr, “Size-dependent bioadhesion of micro- and nanoparticulate carriers to the inflamed colonic mucosa”, Pharmaceutical Research, Vol.18, No. 6, pp.788-793. UDOI:10.1023/A:1011032328064 [22] R.R. Dubey and R.H. Parikh, “Studies of PLGA microspheres”, Pharmaceutical Technology Europe, Vol. 16, 2004, pp. 23-34. [23] N. Gottlieb and C. Schwartzbach, “Development of an internal mixing two-fluid nozzle by systematic variation of internal parts”, ILASS conference, Nottingham, UK. 2004. UHttp://www.niro.com/niro/cmsresources.nsf/filenames/TFN_Niro_Ilass_2004_Final.pdf/$file/TFN_Niro_Ilass_2004_Final.pdf [24] V.H. Kulkarni, P.V. Kulkarni and J. Keshavayya, “Glutaraldehyde- crosslinked chitosan beads for controlled release of diclofenac sodium”, Journal of Applied Polymer Science, Vol.103, No. 1, 2007, pp. 211-217. Udoi:10.1002/app.25161 [25] T. Iliescu, M. Baia and W. Kiefer, “FT-Raman, surface-enhanced Raman spectroscopy and theoretical investigations of diclofenac sodium”. Chemical Physics, Vol. 298, No. 1-3, 2004, pp.167-174. Udoi:10.1016/j.chemphys.2003.11.018 [26] F.L. Mi, C.Y. Kuan, S.S. Shyu, S.T. Lee and S.F. Chang, “The study of gelation kinetics and chain-relaxation properties of glutaraldehyde-cross-linked chitosan gel and their effects on microspheres preparation and drug release”, Carbohydrate Polymers, Vol.41, No.4, 2000, pp. 389-396. [27] M. Gibaldi and S. Feldman, “Establishment of sink conditions in dissolution rate determinations-theoretical considerations and application to nondisintegrating dosage forms”, Journal of Pharmaceutical Sciences, Vol. 56, No.10, 1967, pp. 1238-1242. Udoi: 10.1002/jps.2600561005 [28] J.G. Wagner, “Interpretation of percent dissolved-time plots derived from in vitro testing of conventional tablets and capsules”, Journal of Pharmaceutical Sciences, Vol.58, No. 10, 1969, pp. 1253-1257. Udoi: 10.1002/jps.2600581021 [29] T. Higuchi, “Mechanism of sustained‐action medication. Theoretical analysis of rate of release of solid drugs dispersed in solid matrices”. Journal of Pharmaceutical Sciences, Vol. 52, No.12, 1963, pp.1145-1149. Udoi: 10.1002/jps.2600521210 [30] P.L. Ritger and N.A. Peppas, “A simple equation for description of solute release. I. Fickian and non-Fickian release from non-swellable devices in the form of slabs, spheres, cylinders or discs”. Journal of Controlled Release, Vol. 5, No 1, 1987, pp. 23-36. [31] J. Siepmann and N.A. Peppas, “Modeling of drug release from delivery systems based on hydroxypropyl methylcellulose (HPMC)”, Advanced Drug Delivery Reviews, Vol.48, No.2-3, 2001, pp.139-157.
[1] S. Freiberg and X. X. Zhu, “Polymer microspheres for controlled drug release”, International Journal of Pharmaceutics, Vol. 282, No. 1-2, 2004, pp.1-18. Udoi:10.1016/j.ijpharm.2004.04.013 [2] R.H. Qin, F.S. Li, M.Y. Chen and W. Jiang, “Preparation of chitosan–ethylene diaminetetraacetate-enwrapped magnetic CoFe2O4 nanoparticles via zero-length emulsion crosslinking method”. Applied Surface Science, Vol. 256, No.1, 2009, pp.27-32. [3] A. R. Dudhani and S.L.Kosaraju. “Bioadhesive chitosan nanoparticles: Preparation and characterization”, Carbohydrate Polymers, Vol. 81, No. 2, 2010, pp. 243-251. Udoi:10.1016/j.carbpol.2010.02.026 [4] S.A. Agnihotri and T.M. Aminabhavi, “Controlled release of clozapine through chitosan microparticles prepared by a novel method”, Journal of Controlled Release, Vol. 96, No. 2, 2004, pp. 245-259. Udoi:10.1016/j.jconrel.2004.01.025 [5] D. Chiou and T.A.G. Langrish, “Development and characterisation of novel nutraceuticals with spray drying technology”, Journal of Food Engineering, Vol. 82, No. 1, 2007, pp 84-91. Udoi:10.1016/j.jfoodeng.2007.01.021 [6] L. Ochiuz and J.E. Peris, “Preparation and Characterisation of Alendronate-Loaded Chitosan Microparticles Obtained Through the Spray Drying Technique”, Medicinal Chemistry, Vol. 5, No. 2, 2009, pp. 191-196(6). [7] P. Tewa-Tagne, S. Brian?on and H. Fessi, “Preparation of redispersible dry nanocapsules by means of spray-drying: Development and characterization”, European Journal of Pharmaceutical Sciences, Vol. 30, No. 2, 2007, pp. 124- 135. Udoi:10.1016/j.ejps.2006.10.006 [8] K. Vimala, M. M. Yallapu, K. Varaprasad, N. N. Reddy, S. Ravindra, N. S. Naidu, K. M. Raju, “Fabrication of Curcumin Encapsulated Chitosan-PVA Silver Nanocomposite Films for Improved Antimicrobial Activity”, Journal of Biomaterials and Nanobiotechnology, Vol.2, No.1, 2011, PP. 55-64. Udoi: 10.4236/jbnb.2011.21008 [9] H. Li, C.R. Zhou, J.H. Tian and J.H. Rong, “Preparation and Characterization of Homogeneous Hydroxyapatite/Chitosan Composite Scaffolds via In-Situ Hydration”, Journal of Biomaterials and Nanobiotechnology, Vol.1, No.1, 2010, pp.42-49. doi:10.4236/jbnb.2010.11006 [10] Y. Murata, D. Hirai, K. Kofuji, E. Miyamoto and S. Kawashima, “Properties of an Alginate Gel Bead Containing a Chitosan-Drug Salt”, Biological & Pharmaceutical Bulletin, Vol. 27, No. 3, 2004, pp. 440-442. Udoi:10.1248/bpb.27.440 [11] P. He, S.S. Davis and L. Illum,”Chitosan microspheres prepared by spray drying”, International Journal of Pharmaceutics, Vol. 187, No.1, 1999, pp. 53-65. Udoi:10.1016/S0378-5173(99)00125-8 [12] P. Giunchedi, C. Juliano, E. Gavini, M. Cossu and M. Sorrenti, “Formulation and in vivo evaluation of chlorhexidine buccal tablets prepared using drug-loaded chitosan microspheres”, European Journal of Pharmaceutics and Biopharmaceutics, Vol. 53, No. 2, 2002, pp.233-239. Udoi:10.1016/S0939-6411(01)00237-5 [13] D.O. Corrigan, A.M. Healy and O.I. Corrigan, “Preparation and release of salbutamol from chitosan and chitosan co-spray dried compacts and multiparticulates”, European Journal of Pharmaceutics and Biopharmaceutics, Vol. 62, No.3, 2006, pp. 295-305. Udoi:10.1016/j.ejpb.2005.09.008 [14] A. Alhalaweh, S. Andersson and S.P. Velaga, “Preparation of zolmitriptan–chitosan microparticles by spray drying for nasal delivery”, European Journal of Pharmaceutical Sciences, Vol. 38, No. 3, 2009, pp. 206-214. Udoi:10.1016/j.ejps.2009.07.003 [15] J.P.Zhang, Q. Wang and A.Q. Wang, “In situ generation of sodium alginate/ hydroxyapatite nanocomposite beads as drug-controlled release matrices”, Acta Biomaterialia, Vol.6, No.2, 2010, pp. 445-454. Udoi:10.1016/j.actbio.2009.07.001 [16] M. D. Arco, E. Cebadera, S. Gutiérrez, C. Martín, M.J. Montero, V. Rives, J. Rocha and M.A. Sevilla, “Mg, Al layered double hydroxides with intercalated indomethacin: Synthesis, characterization, and pharmacological study”, Journal of Pharmaceutical Science, Vol. 93, No.6, 2004, pp. 1649-1658. Udoi: 10.1002/jps.20054 [17] Q. Wang, X.L. Xie, X.W. Zhang, J.P. Zhang and A.Q. Wang, “Preparation and swelling properties of pH sensitive composite hydrogel beads based on chitosan-g-poly (acrylic acid)/vermiculite and sodium alginate for diclofenac controlled release”, International Journal of Biological Macromolecules, Vol.46, No.3, 2010, pp. 356- 362. Udoi:10.1016/j.ijbiomac.2010.01.009 [18] M.P.S. Krekeler and S. Guggenheim, “Defects in microstructure in palygorskite–sepiolite minerals: A transmission electron microscopy (TEM) study”, Applied Clay Science, Vol. 39, No. 1-2, 2008, pp. 98-105. Udoi:10.1016/j.clay.2007.05.001 [19] M.J. Fernández-Hervás, M.A. Holgado, A. Fini and J.T. Fell, “In vitro evaluation of alginate beads of diclofenac salts”, International Journal of Pharmaceutics, Vol.163, No. 1-2, 1998, pp. 23-34. Udoi:10.1016/S0378-5173(97)00333-5 [20] A. Lamprecht, N. Ubrich, H. Yamamoto, U. Sch?fer, H. Takeuchi, P. Maincent, Y. Kawashima andC.M. Lehr, “Biodegradable nanoparticles for targeted drug delivery in treatment of inflammatory bowel disease”, The Journal of Pharmacology and Experimental Therapeutics, Vol. 299, No. 2, pp.775-781. [21] A. Lamprecht, U. Schafer and C.M. Lehr, “Size-dependent bioadhesion of micro- and nanoparticulate carriers to the inflamed colonic mucosa”, Pharmaceutical Research, Vol.18, No. 6, pp.788-793. UDOI:10.1023/A:1011032328064 [22] R.R. Dubey and R.H. Parikh, “Studies of PLGA microspheres”, Pharmaceutical Technology Europe, Vol. 16, 2004, pp. 23-34. [23] N. Gottlieb and C. Schwartzbach, “Development of an internal mixing two-fluid nozzle by systematic variation of internal parts”, ILASS conference, Nottingham, UK. 2004. UHttp://www.niro.com/niro/cmsresources.nsf/filenames/TFN_Niro_Ilass_2004_Final.pdf/$file/TFN_Niro_Ilass_2004_Final.pdf [24] V.H. Kulkarni, P.V. Kulkarni and J. Keshavayya, “Glutaraldehyde- crosslinked chitosan beads for controlled release of diclofenac sodium”, Journal of Applied Polymer Science, Vol.103, No. 1, 2007, pp. 211-217. Udoi:10.1002/app.25161 [25] T. Iliescu, M. Baia and W. Kiefer, “FT-Raman, surface-enhanced Raman spectroscopy and theoretical investigations of diclofenac sodium”. Chemical Physics, Vol. 298, No. 1-3, 2004, pp.167-174. Udoi:10.1016/j.chemphys.2003.11.018 [26] F.L. Mi, C.Y. Kuan, S.S. Shyu, S.T. Lee and S.F. Chang, “The study of gelation kinetics and chain-relaxation properties of glutaraldehyde-cross-linked chitosan gel and their effects on microspheres preparation and drug release”, Carbohydrate Polymers, Vol.41, No.4, 2000, pp. 389-396. [27] M. Gibaldi and S. Feldman, “Establishment of sink conditions in dissolution rate determinations-theoretical considerations and application to nondisintegrating dosage forms”, Journal of Pharmaceutical Sciences, Vol. 56, No.10, 1967, pp. 1238-1242. Udoi: 10.1002/jps.2600561005 [28] J.G. Wagner, “Interpretation of percent dissolved-time plots derived from in vitro testing of conventional tablets and capsules”, Journal of Pharmaceutical Sciences, Vol.58, No. 10, 1969, pp. 1253-1257. Udoi: 10.1002/jps.2600581021 [29] T. Higuchi, “Mechanism of sustained‐action medication. Theoretical analysis of rate of release of solid drugs dispersed in solid matrices”. Journal of Pharmaceutical Sciences, Vol. 52, No.12, 1963, pp.1145-1149. Udoi: 10.1002/jps.2600521210 [30] P.L. Ritger and N.A. Peppas, “A simple equation for description of solute release. I. Fickian and non-Fickian release from non-swellable devices in the form of slabs, spheres, cylinders or discs”. Journal of Controlled Release, Vol. 5, No 1, 1987, pp. 23-36. [31] J. Siepmann and N.A. Peppas, “Modeling of drug release from delivery systems based on hydroxypropyl methylcellulose (HPMC)”, Advanced Drug Delivery Reviews, Vol.48, No.2-3, 2001, pp.139-157.