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WIREs Nanomed Nanobiotechnol
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Recent progress on fabrication and drug delivery applications of nanostructured hydroxyapatite

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Through this brief review, we provide a comprehensive historical background of the development of nanostructured hydroxyapatite (nHAp), and its application potentials for controlled drug delivery, drug conjugation, and other biomedical treatments. Aspects associated with efficient utilization of hydroxyapatite (HAp) nanostructures such as their synthesis, interaction with drug molecules, and other concerns, which need to be resolved before they could be used as a potential drug carrier in body system, are discussed. This review focuses on the evolution of perceptions, practices, and accomplishments in providing improved delivery systems for drugs until date. The pioneering developments that have presaged today's fascinating state of the art drug delivery systems based on HAp and HAp‐based composite nanostructures are also discussed. Special emphasis has been given to describe the application and effectiveness of modified HAp as drug carrier agent for different diseases such as bone‐related disorders, carriers for antibiotics, anti‐inflammatory, carcinogenic drugs, medical imaging, and protein delivery agents. As only a very few published works made comprehensive evaluation of HAp nanostructures for drug delivery applications, we try to cover the three major areas: concepts, practices and achievements, and applications, which have been consolidated and patented for their practical usage. The review covers a broad spectrum of nHAp and HAp modified inorganic drug carriers, emphasizing some of their specific aspects those needed to be considered for future drug delivery applications.

Schematic representation of pH‐responsive drug carrier, based on the interaction between negatively charged carboxyl groups of citrate upon hollow hydroxyapatite (HAp) nanorods surfaces and positively charged poly dimethyldiallyl ammonium (PDDA) molecules. The interaction formed the gates to open or close to store or release vancomycin from the hollow nanorods, as controlled by environment pH. (Reprinted with permission from Ref . Copyright 2010 Elsevier)
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Schematic representation of hollow hydroxyapatite (HAp) nanoparticles fabrication from P123 and Tween‐60 core–shell structured micelles templates. (Recreated with permission from Ref . Copyright 2010 Elsevier)
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SEM images of DEX‐loaded PLGA microspheres immobilized onto hydroxyapatite (HAp) scaffold. (a, a1, a2) HAp scaffold after shaking for 4 h with water‐dispersed control PLGA microspheres; (b, b1, b2) HAp scaffold after shaking for 4 h with water‐dispersed PEI coated PLGA microspheres. (Reprinted with permission from Ref . Copyright 2011 Elsevier)
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Schematic diagram of the porous hydroxyapatite (HAp) scaffold containing Dex‐loaded PLGA microspheres. PLGA microspheres were pre‐coated with PEI molecules. The counter charge of the microsphere and HAp surfaces permitted fabrication of the system via electrostatic interactions. (Reprinted with permission from Ref . Copyright 2011 Elsevier)
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Schematic presentation of drug conjugation processes over hydroxyapatite (HAp) nanoparticles.
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Molecular structure of hydroxyapatite (HAp): (a) computational modeled hexagonal crystal structure with P63 symmetry. Calcium ions are at the vertices of the triangles around each hydroxyl group (red). (Reprinted with permission from Ref . Copyright 2010 Royal Society of Chemistry. (b) Unit cell perspective. (Reprinted with permission from Ref . Copyright 2007 Elsevier)
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Bio‐sources for hydroxyapatite (HAp) synthesis: Animal (top left), plant (top right) and aquatic (bottom).
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In vivo PL imaging of the mice after subcutaneous injection without (a) and with (b) Eu3+/Gd3+‐HAp (Eu3+: Gd3+ = 1:2) nanorods. (c) PL emission images of Eu3+/Gd3+‐HAp nanorods at different concentrations. The excitation wavelength was 430 nm. (Reprinted with permission from Ref . Copyright 2011 Elsevier)
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Top: Schematic representation of different pore structures. Bottom: Mesoporous hydroxyapatite (HAp) scaffold: (a) stereoscopic and (b) SEM image. (Reprinted with permission from Ref . Copyright 2011 Elsevier)
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Three generations of nanoparticles engineered for biomedical applications.
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(i). Magnetic hydroxyapatite (mHAp) nanoparticles based on different dopants. (ii) The clinical photographs of the tumor (mHAp with magnetic field). The tumor in day 1 (A), day 5 (B), and day 14 (C). (iii) The clinical photographs of the tumor (mHAp without magnetic field). The tumor in day 1 (a), day 5 (b), and day 14 (c). (Reprinted with permission from Ref . Copyright 2009 Elsevier)
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(a) Schematic illustration of the preparation of DOX@PAA–MHAPNs and the intracellular pH‐responsive drug delivery system (b) Cumulative release profiles of DOX from (i) DOX@PAA–MHAPNs and (ii) DOX@MHAPNs at different pH values. (Reprinted with permission from Ref . Copyright 2016 Royal Society of Chemistry)
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(a) Schematic illustration of redox‐responsive system based on collagen capped MHAp (mesoporous hydroxyapatite) for cell‐targeted drug delivery (b) Cumulative release profiles of FITC from LA‐Col‐S‐S‐MHAp with/without DTT solution: (i) controlled release of FITC from LA‐Col‐S‐SMHAp (a and b without DTT, c with DTT) and the Col/MHAp system (b); (ii) delayed release of FITC from LA‐Col‐S‐S‐MHAp by addition of DTT solution after incubation for 5 h. (Reprinted with permission from Ref . Copyright 2014 Royal Society of Chemistry)
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TEM micrographs of (a)–(c) CaCO3 cores with different sizes (d)–(i) HAp hollow ellipsoidal capsules nanostructures with different shell thicknesses prepared by using the CaCO3 cores. (Reprinted with permission from Ref . Copyright 2008 Royal Society of Chemistry)
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Mauro Ferrari

Mauro Ferrari

started out in mechanical engineering and became interested in nanotechnology with his studies on nanomechanics and nanofluidics. His research work and involvement with setting up some of the premier nano centers and alliances in the world, bringing together universities, hospitals, and federal agencies, showcases interdisciplinarity at work.

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