UUnniivveerrssiittyy ooff CCeennttrraall FFlloorriiddaa SSTTAARRSS UCF Patents Technology Transfer 1-21-2014 SSiilliiccaa--bbaasseedd AAnnttiibbaacctteerriiaall aanndd AAnnttiiffuunnggaall NNaannooffoorrmmuullaattiioonn DDIIVV Swadeshmukul Santra University of Central Florida Find similar works at: https://stars.library.ucf.edu/patents University of Central Florida Libraries http://library.ucf.edu This Patent is brought to you for free and open access by the Technology Transfer at STARS. It has been accepted for inclusion in UCF Patents by an authorized administrator of STARS. For more information, please contact [email protected]. RReeccoommmmeennddeedd CCiittaattiioonn Santra, Swadeshmukul, "Silica-based Antibacterial and Antifungal Nanoformulation DIV" (2014). UCF Patents. 515. https://stars.library.ucf.edu/patents/515 I lllll llllllll Ill lllll lllll lllll lllll lllll 111111111111111111111111111111111 US008632811B 1 c12) United States Patent (10) Patent No.: US 8,632,811 Bl San tr a (45) Date of Patent: Jan.21,2014 (54) SILICA-BASED ANTIBACTERIAL AND Yeshchenko, Oleg, Influence of Annealing Conditions on Structure ANTIFUNGAL NANOFORMULATION and Optical Properties of Copper Nanoparticles Embedded in Silica Matrix, 2006, Physics Department, National Taras Shevchenko Kyiv University, Ukraine, pp. 1-25.* (75) Inventor: Swadeshmukul Santra, Orlando, FL H.W. Richardson, "Handbook of Copper Compounds and Applica (US) tions" Copper Fungicides/batericides H.W. Richardson Editor, 1997, Marcel Dekker, Inc.: New York, NY, pp. 93-122. (73) Assignee: University of Central Florida Research Torgeson, D.C., ed. "Fungicides-An Advanced Treatise" Agricul Foundation, Inc., Orlando, FL (US) tural and Industrial Applications and Enviromental Interaction, vol. 1, 1967, Academic Press: New York, NY, Ch. 6, p. 153-193 [chapter ( *) Notice: Subject to any disclaimer, the term ofthis Title: Formulation: Author: E. Somers. Navarro, E., et al., In "Environmental behavior and ecotoxicity of patent is extended or adjusted under 35 engineered nanoparticles to algae, plants, and fungi," Ecotoxicology, U.S.C. 154(b) by 32 days. 2008, 17(5): pp. 372-386. Oberdorster, G., et al., in Nanotoxicology: An Emerging Discipline (21) Appl. No.: 13/527,691 Evolving from Studies ofUltrafine Particles, Environmental Health Perspectives, 2005, 113(7): pp. 823-839. (22) Filed: Jun.20,2012 S. Santra, et al., In "Fluorescence Lifetime Measurements to Deter mine the Core-Shell Nanostructure of FITC-doped Silica Nanoparticles: An Optical Approach to Evaluate Nanoparticle Photo stability" Journal of Luminescence, 2006, 117(1) pp. 75-82. Related U.S. Application Data Maniprasad, et al.; Novel Copper (Cu) Loaded Core-Shell Silica Nanoparticles with Improved Cu Bioavailability: Synthesis, Charac (62) Division of application No. 12/332,021, filed on Dec. terization and Study of Antibacterial Properties; Journal of Biomedi 10, 2008, now Pat. No. 8,221,791. cal Nanotechnology; vol. 8, 1-9, 2012. Maniprasad, et al.; Antimicrobial Properties of Copper and Silver (51) Int. Cl. Loaded Silica Nanomaterials; Manuscript ID No. 1198620; to be A61K9/14 (2006.01) submitted to the 36th International Conference on Advanced Ceram AOJN59/20 (2006.01) ics and Composites (ICACC); Apr. 4, 2012. (52) U.S. Cl. * cited by examiner USPC ............ 424/484; 424/630; 514/499; 977/778 ( 58) Field of Classification Search Primary Examiner - Sue Liu USPC ................... 504/101; 424/484, 630; 514/499; Assistant Examiner - Andriae M Holt 977/778 (74) Attorney, Agent, or Firm - Thomas Horstemeyer, LLP See application file for complete search history. (57) ABSTRACT (56) References Cited A silica-based nanoformulation and method is used to treat U.S. PATENT DOCUMENTS citrus canker, inhibit the growth of mold and mildew, and add nutrients to soil used for agricultural purposes. The nanotech 3,983,214 A 9/1976 Misato et al. nology-enabled copper-loaded, silica nano formulation (CuS 3,992,146 A 1111976 Fazzalari 5,462,738 A 10/1995 LeFiles et al. iNP/NG) design is a "revolutionary re-invention" of Cu for 5,939,357 A 8/1999 Jones et al. safe application because it provides a formulation with maxi 6,471,976 Bl 10/2002 Taylor et al. mum abundance of ionic Cu, provides sustained and optimal 6,548,264 Bl 4/2003 Tan et al. Cu ion release for long-term disease protection, better adher 6,924,116 B2 8/2005 Tan et al. ence to plant surfaces and structural surfaces due to gel-based 7,163,709 B2 1/2007 Cook et al. 7,226,610 B2 6/2007 Winniczuk nano structure of CuSiNG, thus avoiding multiple spray appli 7,332,351 B2 2/2008 Tan et al. cations and reducing the amount of Cu used in comparison to 2001/0051174 Al 12/2001 Staats existing Cu compounds without compromising antibacterial 2007 /0098806 Al 5/2007 Ismail et al. activity. Thus, the silica-based nanoformulation releases cop OTHER PUBLICATIONS per in non-toxic quantities to the environment and the silica matrix provides an environmentally safe host material with a Kikteva, T.A., Probing the Sol-Gel Conversion m the flexible design that is optimized to provide specific antifungal Tetraethoxysilane/A lcohol/Water System with the Aid of Diffusion and antibacterial remediation using infrequent applications. Controlled Fluorescence Quenching, 1997, Journal of Colloid and Interface Science, vol. 193, pp. 163-166.* 6 Claims, 10 Drawing Sheets U.S. Patent Jan.21,2014 Sheet 1of10 US 8,632,811 Bl ....... c ~ oL--~~---~--==::::=::====::== c.. 10 100 1,000 Q,} ' Diameter (nm) Fig. la U.S. Patent Jan.21,2014 Sheet 2of10 US 8,632,811 Bl trf> -------- -----------------·-·-··- ---- -· ----- ~ • I)() ~ N s 5 .._ 10 ! ,;: 8 4 10 .!! :_; =' =~ u 103 ·u 8. a2 ....._ __ I _.,.----------t ti} ocoo 0 2000 4000 6000 8000 1 ParticJe size (nm) Fig. lb U.S. Patent Jan.21,2014 Sheet 3of10 US 8,632,811 Bl 'f O ~-• (c) Surface Cu oxide/hydroxide as !J\J::lf' nanoclusters/nanoparticles "·0 \A u " '(>) ~ Covalently~bound Cu t present in the hydrated 0 sutface and nanO{JOres ~ (a) Bectrostatically-bound Cu (counter ions not shown for simplicity) Fig. 2 U.S. Patent Jan.21,2014 Sheet 4of10 US 8,632,811 Bl Wonm HV= 100.0kV Direct Mau: lOSOOX Materials Ebaracteriz.ation Facility- UCF Fig. 3 U.S. Patent Jan.21,2014 Sheet 5of10 US 8,632,811 Bl ~Light Blue §Clear [Il] Deep Blue 2 ~\\'bite Fig. 4a Fig. 4b Fig. 4c Fig. 4d U.S. Patent Jan.21,2014 Sheet 6of10 US 8,632,811 Bl Cu loaded silica nanog.el - "' - :r:: -· 0 I'< -5 ::l .-!::' -ti ko-ci&! 0 -:::;; :-c I u 0 Q :-c" ' - - N0 u::J (::)J 0 0 -......-. -0 -::i () ..... M.... . 0 I..O.... 20 30 40 50 60 2e(I~gree) Fig. 5 U.S. Patent Jan.21,2014 Sheet 7of10 US 8,632,811 Bl Fig. 6a Fig. 6b Cu2p (b) (•) 930 940 950 960 970 9 932 934 936 938 Bimting &n-gy(e\I) Bmdm·~ eV) 01s (c) 5~ 103.1 (d} uo 95 100 105 115 120 125 Bmlq: ~(e\') Fig. 6c Fig. 6d U.S. Patent Jan.21,2014 Sheet 8of10 US 8,632,811 Bl Fig. 7a Fig. 7b 50 Filter Paper Disc Fig. 7c No E.coli Growth E.coli Colony
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