Formation of hydroxyapatite in various aqueous solutions
Open Access
- Author:
- Sturgeon, Jacqueline Lee
- Graduate Program:
- Materials Science and Engineering
- Degree:
- Doctor of Philosophy
- Document Type:
- Dissertation
- Date of Defense:
- August 27, 2007
- Committee Members:
- Paul Wencil Brown, Committee Chair/Co-Chair
Della M Roy, Committee Member
Erwin A Vogler, Committee Member
Neil Sharkey, Committee Member - Keywords:
- hydroxyapatite
calcium phosphate cement
biomaterials
fluorapatite
carbonated apatite
phosphonate - Abstract:
- Hydroxyapatite (HAp), Ca10(PO4)6(OH)2, is important in the field of biomaterials as it is the mineral component of bones and teeth. Biological apatites do not maintain an exact composition and are usually calcium-deficient, represented as Ca(10-x)(HPO4)x(PO4)(6-x)(OH)(2-x), where x ranges from 0 to 1, with various ion substitutions. Formation of calcium-deficient hydroxyapatites (CDHAp) from solid calcium phosphate precursor materials was performed at physiologic temperature (37oC) in a variety of aqueous solutions. Two cement systems were utilized in these experiments: tetralcium phosphate (TetCP) with dicalcium phosphate anhydrous (DCPA) and b-tricalcium phosphate (b-TCP). The kinetics, solution chemistry, phase evolution, and microstructure of the developed apatites were analyzed as appropriate. Reaction of b-TCP in ammonium fluoride solutions formed HAp substituted with fluoride and calculated to be deficient in calcium. A new ratio of TetCP to DCPA was used with solutions of sodium bicarbonate to form a calcium-deficient carbonate hydroxyapatite. The capacity for sodium dihydrogen phosphate to buffer pH increases and enhance reaction kinetics in this system was also explored. Formation of a highly crystalline CDHAp was achieved by hydrolyzing b-TCP in water for extended time periods. Lattice parameters were among the features characterized for this apatite. The hydrolysis of b-TCP in phosphate buffered saline (PBS) and simulated body fluids (SBF) was also investigated; use of SBF was found to completely inhibit formation of HAp in this system while reaction in PBS was slow in comparison to water. The effects of filler materials on the mechanical properties of a calcium phosphate cement were examined using the TetCP/DCPA system. Dense aggregates were not found to decrease compressive strength in comparison to the cement alone. The use of aggregates was found to improve the compressive strength of cement formed using NaHCO3 solution as a setting liquid. The influence of phosphonates on formation of HAp from a TetCP/DCPA system was analyzed. Variations in concentration and phosphonate type were observed to influence the dissolution of precursors and HAp formation in this system. Bisphosphonates were more effective at inhibiting dissolution or growth of HAp in solutions with high liquid to solids ratios. Monophosphonate was found to slightly accelerate the formation of HAp at low concentration.