Temperature-sensitive hydrogels with SiO2-Au nanoshells for controlled drug delivery.

Silica-gold (SiO(2)-Au) nanoshells are a new class of nanoparticles that consist of a silica dielectric core that is surrounded by a gold shell. These nanoshells are unique because their peak extinctions are very easily tunable over a wide range of wavelengths particularly in the near infrared (IR) region of the spectrum. Light in this region is transmitted through tissue with relatively little attenuation due to absorption. In addition, irradiation of SiO(2)-Au nanoshells at their peak extinction coefficient results in the conversion of light to heat energy that produces a local rise in temperature. Thus, to develop a photothermal modulated drug delivery system, we have fabricated nanoshell-composite hydrogels in which SiO(2)-Au nanoshells of varying concentrations have been embedded within temperature-sensitive hydrogels, for the purpose of initiating a temperature change with light. N-isopropylacrylamide-co-acrylamide (NIPAAm-co-AAm) hydrogels are temperature-sensitive hydrogels that were fabricated to exhibit a lower critical solution temperature (LCST) slightly above body temperature. The resulting composite hydrogels had the extinction spectrum of the SiO(2)-Au nanoshells in which the hydrogels collapsed reversibly in response to temperature (50 degrees C) and laser irradiation. The degree of collapse of the hydrogels was controlled by the laser fluence as well as the concentration of SiO(2)-Au nanoshells. Modulated drug delivery profiles for methylene blue, insulin, and lysozyme were achieved by irradiation of the drug-loaded nanoshell-composite hydrogels, which showed that drug release was dependent upon the molecular weight of the therapeutic molecule.

[1]  H. Smulyan Nitrates, arterial function, wave reflections and coronary heart disease. , 2007, Advances in cardiology.

[2]  T Terahara,et al.  Dependence of low-frequency sonophoresis on ultrasound parameters; distance of the horn and intensity. , 2002, International journal of pharmaceutics.

[3]  R. Langer,et al.  Enzymatically controlled drug delivery. , 1988, Proceedings of the National Academy of Sciences of the United States of America.

[4]  Sven Frokjaer,et al.  Loading into and electro-stimulated release of peptides and proteins from chondroitin 4-sulphate hydrogels. , 2002, European journal of pharmaceutical sciences : official journal of the European Federation for Pharmaceutical Sciences.

[5]  Wim E Hennink,et al.  Recombinant gelatin hydrogels for the sustained release of proteins. , 2007, Journal of controlled release : official journal of the Controlled Release Society.

[6]  Leon Hirsch,et al.  Gold nanoshell bioconjugates for molecular imaging in living cells. , 2005, Optics letters.

[7]  David J. Mooney,et al.  Controlled growth factor release from synthetic extracellular matrices , 2000, Nature.

[8]  H. Fain,et al.  Ultrasound-enhanced tumor targeting of polymeric micellar drug carriers. , 2004, Molecular pharmaceutics.

[9]  C. Gomer,et al.  Clinical and preclinical photodynamic therapy , 1995, Lasers in surgery and medicine.

[10]  G. Grover,et al.  Recent Advances in the Development of Agonists Selective for β1-Type Thyroid Hormone Receptor , 2007 .

[11]  Hyun Chul Lee,et al.  Remission in models of type 1 diabetes by gene therapy using a single-chain insulin analogue , 2000, Nature.

[12]  Yan Jiang,et al.  Effects of surface coating on the controlled release of vitamin B1 from mesoporous silica tablets. , 2007, Journal of controlled release : official journal of the Controlled Release Society.

[13]  Peter P. Edwards,et al.  A new hydrosol of gold clusters. 1. Formation and particle size variation , 1993 .

[14]  San-Yuan Chen,et al.  Nano-ferrosponges for controlled drug release. , 2007, Journal of controlled release : official journal of the Controlled Release Society.

[15]  T. Okano,et al.  Modulating the phase transition temperature and thermosensitivity in N-isopropylacrylamide copolymer gels. , 1994, Journal of biomaterials science. Polymer edition.

[16]  Akira Matsumoto,et al.  Glucose-responsive polymer gel bearing phenylborate derivative as a glucose-sensing moiety operating at the physiological pH. , 2004, Biomacromolecules.

[17]  Y. Bae,et al.  Electrically credible polymer gel for controlled release of drugs , 1991, Nature.

[18]  Andrzej Nowicki,et al.  In vitro ultrasound-mediated leakage from phospholipid vesicles. , 2006, Ultrasonics.

[19]  Y. Tabata,et al.  Controlled-release of epidermal growth factor from cationized gelatin hydrogel enhances corneal epithelial wound healing. , 2006, Journal of controlled release : official journal of the Controlled Release Society.

[20]  J L West,et al.  A whole blood immunoassay using gold nanoshells. , 2003, Analytical chemistry.

[21]  Z. Gucev,et al.  Insulin detemir compared with NPH insulin in children and adolescents with Type 1 diabetes , 2007, Diabetic medicine : a journal of the British Diabetic Association.

[22]  R. Barr,et al.  Electric Fields in Tumors Exposed to External Voltage Sources: Implication for Electric Field-Mediated Drug and Gene Delivery , 2006, Annals of Biomedical Engineering.

[23]  R. Eisenthal,et al.  A reversible hydrogel membrane for controlling the delivery of macromolecules. , 2003, Biotechnology and bioengineering.

[24]  Yi-Yan Yang,et al.  Evaluating proteins release from, and their interactions with, thermosensitive poly (N-isopropylacrylamide) hydrogels. , 2005, Journal of controlled release : official journal of the Controlled Release Society.

[25]  K. Kataoka,et al.  Temperature-related change in the properties relevant to drug delivery of poly(ethylene glycol)-poly(D,L-lactide) block copolymer micelles in aqueous milieu. , 2002, Journal of controlled release : official journal of the Controlled Release Society.

[26]  Masahiro Irie,et al.  Photoinduced phase transition of gels , 1990 .

[27]  R. Reis,et al.  Synthesis and Characterization of pH-Sensitive Thiol-Containing Chitosan Beads for Controlled Drug Delivery Applications , 2007, Drug delivery.

[28]  W. Stöber,et al.  Controlled growth of monodisperse silica spheres in the micron size range , 1968 .

[29]  Toyoichi Tanaka,et al.  Phase transition in polymer gels induced by visible light , 1990, Nature.

[30]  S. L. Westcott,et al.  Infrared extinction properties of gold nanoshells , 1999 .

[31]  External control of drug release: controlled release of insulin from a hydrophilic polymer implant by ultrasound irradiation in diabetic rats , 1988, The Journal of pharmacy and pharmacology.

[32]  Jung-Hwan Park,et al.  Biodegradable polymer microneedles: fabrication, mechanics and transdermal drug delivery. , 2005, Journal of controlled release : official journal of the Controlled Release Society.

[33]  J. West,et al.  Immunotargeted nanoshells for integrated cancer imaging and therapy. , 2005, Nano letters.

[34]  Naomi J. Halas,et al.  Linear optical properties of gold nanoshells , 1999 .

[35]  Mark G. Allen,et al.  Polymer Microneedles for Controlled-Release Drug Delivery , 2006, Pharmaceutical Research.

[36]  Qiang Zhang,et al.  Controlled delivery of recombinant hirudin based on thermo-sensitive Pluronic F127 hydrogel for subcutaneous administration: In vitro and in vivo characterization. , 2007, Journal of controlled release : official journal of the Controlled Release Society.

[37]  Sung Wan Kim,et al.  Reverse thermal gelation of aliphatically modified biodegradable triblock copolymers. , 2006, Macromolecular bioscience.

[38]  J. Fujimoto,et al.  Optical Coherence Tomography , 1991 .

[39]  Paul A Dayton,et al.  Ultrasound radiation force enables targeted deposition of model drug carriers loaded on microbubbles. , 2006, Journal of controlled release : official journal of the Controlled Release Society.

[40]  J. Boatright,et al.  Delivery of several forms of DNA, DNA-RNA hybrids, and dyes across human sclera by electrical fields. , 2003, Molecular vision.

[41]  Darrell M. Wilson,et al.  Duration of Nocturnal Hypoglycemia Before Seizures , 2008, Diabetes Care.

[42]  D. Huhn,et al.  Preclinical experiences with magnetic drug targeting: tolerance and efficacy. , 1996, Cancer research.

[43]  Naomi J. Halas,et al.  Nanoengineering of optical resonances , 1998 .

[44]  L. D. Taylor,et al.  Preparation of films exhibiting a balanced temperature dependence to permeation by aqueous solutions—a study of lower consolute behavior , 1975 .

[45]  Cory Berkland,et al.  NanoCipro encapsulation in monodisperse large porous PLGA microparticles. , 2007, Journal of controlled release : official journal of the Controlled Release Society.

[46]  A. Hoffman,et al.  Lower critical solution temperatures of aqueous copolymers of N-isopropylacrylamide and other N-substituted acrylamides , 1987 .

[47]  You Han Bae,et al.  TAT peptide-based micelle system for potential active targeting of anti-cancer agents to acidic solid tumors. , 2007, Journal of controlled release : official journal of the Controlled Release Society.

[48]  Yan Jin,et al.  Novel glycidyl methacrylated dextran (Dex-GMA)/gelatin hydrogel scaffolds containing microspheres loaded with bone morphogenetic proteins: formulation and characteristics. , 2007, Journal of controlled release : official journal of the Controlled Release Society.

[49]  Rebekah A Drezek,et al.  Near infrared laser‐tissue welding using nanoshells as an exogenous absorber , 2005, Lasers in surgery and medicine.