UUnniivveerrssiittyy ooff CCeennttrraall FFlloorriiddaa SSTTAARRSS UCF Patents Technology Transfer 7-17-2012 SSiilliiccaa--bbaasseedd AAnnttiibbaacctteerriiaall aanndd AAnnttiiffuunnggaall NNaannooffoorrmmuullaattiioonn 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" (2012). UCF Patents. 516. https://stars.library.ucf.edu/patents/516 I lllll llllllll Ill lllll lllll lllll lllll lllll 111111111111111111111111111111111 US008221791Bl c12) United States Patent (10) Patent No.: US 8,221,791 Bl San tr a (45) Date of Patent: Jul. 17, 2012 (54) SILICA-BASED ANTIBACTERIAL AND Zhang, K., Synthesis and Characterization of Silica-Copper Oxide ANTIFUNGAL NANOFORMULATION Composite Derived from Microemulsion Processing, 1999, Langmuir, vol. 15, pp. 3056-3061.* (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 Title: Formulation: Author: E. Somers. ( *) Notice: Subject to any disclaimer, the term ofthis 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 691 days. 2008, 17(5): pp. 372-386. Oberdorster, G., et al, in Nanotoxicology: An Emerging Discipline (21) Appl. No.: 12/332,021 Evolving from Studies ofUltrafine Particles, Environmental Health Perspectives, 2005, 113(7): pp. 823-839. (22) Filed: Dec.10,2008 S. Santra, et al., in "Fluorescence Lifetime Measurements to Deter mine the Core-Shell Nanostructure of FITC-doped Silica (51) Int. Cl. Nanoparticles: An Optical Approach to Evaluate Nanoparticle A61K 9114 (2006.01) Photo stability" Journal of Luminescence, 2006, 117(1) pp. 75-82. A61K 33134 (2006.01) * cited by examiner AOJN 59120 (2006.01) (52) U.S. Cl. ......... 424/484; 424/630; 514/499; 977/778 Primary Examiner - Johann Richter (58) Field of Classification Search .................. 504/101; Assistant Examiner - Andriae M Holt 424/630, 484; 514/499; 516/80; 977/778 (74) Attorney, Agent, or Firm - Thomas, Kayden, See application file for complete search history. Horstemeyer & Risley, LLP (56) References Cited (57) ABSTRACT U.S. PATENT DOCUMENTS A silica-based nanoformulation and method is used to treat citrus canker, inhibit the growth of mold and mildew, and add 3,983,214 A 9/1976 Misato et al. 3,992,146 A 1111976 Fazzalari nutrients to soil used for agricultural purposes. The nanotech 5,462,738 A 10/1995 LeFiles et al. nology-enabled copper-loaded, silica nano formulation (CuS 5,939,357 A 8/1999 Jones et al. iNP/NG) design is a "revolutionary re-invention" of Cu for 6,471,976 Bl 10/2002 Taylor et al. safe application because it provides a formulation with maxi 6,548,264 Bl 4/2003 Tan et al. mum abundance of ionic Cu, provides sustained and optimal 6,924,116 B2 8/2005 Tan et al. 7,147,921 B2 * 12/2006 Camp et al. ................... 428/418 Cu ion release for long-term disease protection, better adher 7,163,709 B2 1/2007 Cook et al. ence to plant surfaces and structural surfaces due to gel-based 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 2004/0091417 Al* 512004 Yadav ........................ 423/592.1 2005/0084438 Al* 412005 Do et al. .................. 423/244.02 activity. Thus, the silica-based nanoformulation releases cop 2007 /0098806 Al 5/2007 Ismail et al. per in non-toxic quantities to the environment and the silica matrix provides an environmentally safe host material with a OTHER PUBLICATIONS flexible design that is optimized to provide specific antifungal Zhang, X. A New Solution Route to Hydrogen-terminated Silicon and antibacterial remediation using infrequent applications. Nanoparticles: Synthesis, Functionalization and Water Stability, Jan. 2007, Nanotechnology, vol. 18, pp. 1-6.* 3 Claims, 10 Drawing Sheets U.S. Patent Jul. 17, 2012 Sheet 1of10 US 8,221,791 Bl ....... c:: ~ oL-----=::;::==~~ aQ..J 1 10 100 1,000 Diameter (nm) Fig. la U.S. Patent Jul. 17, 2012 Sheet 2of10 US 8,221,791 Bl 106 --=----"""'·--· ~---~-=--=---=----~~--'""""'-----~----=----=--~---~----··=--~----............,......._,,. I 8 104 .!! ~ :i QI) ·u- 103 -= 0 8. _,__-------....--1"'----:1 a2 UJ I 0 2000 4000 6000 8000 10000 Particle sjze (nm) Fig. lb U.S. Patent Jul. 17, 2012 Sheet 3of10 US 8,221,791 Bl l.f O .-:--r (c) Su/face cu oxide/hydroxide as nanoctusterslnanopamcles ~ Covalentty~bound Cu present in the hydrated sutface and nanopores -i--1 I I -t1-o-s1-o-s1-o-a1-o-11- I I I ·I I "0 0 0 0 Q C! ·::--H '\'H \"H \'H \-H ~ K, • . •· 11. 'eu" H,Gbu" H'.P'col' H: o c.,>• H, C; l,ir MH.0:. M H" I• I("H '.:' M' :H6 · • H 'O' '-o·: 'o}. . ·c,/'·'"\,. 6• "c,/'·· I -~i-0-Ji-O-~i-O~i--O-ti I (a) Bectrostatically-bound Cu (counter ions not shown for simpJ;city) F'ig. 2 U.S. Patent Jul. 17, 2012 Sheet 4of10 US 8,221,791 Bl ( ~ ~;·, ~t f:u-Silicate.tif lOOnm Print Mag: 7 - 600m (iiJ7.6 lm HV= 100.0kV J 5: 12 08/06/008 Dfrect Mxa: 10500X Ma teria Is Eharacteriza lion Facility- tr Cf Fig. 3 U.S. Patent Jul. 17, 2012 Sheet 5of10 US 8,221,791 Bl - - ~Light Blue §Clear -3 [IlJ Deep Blue 2 ~White Fig. 4a Fig. 4b Fig. 4c Fig. 4d U.S. Patent Jul. 17, 2012 Sheet 6of10 US 8,221,791 Bl Cu loaded silica nru.l02Cl .... - N -:c a,,....."._" 0 - - :a - kocidc l"I N 0.... ..... -;:; -:t: :-:c: - ,.- u 0 0 I"'< :-c N- - 0 N :J -:J 0 0- .(,...). {.) Q 0 u-::J - - T- ("') """" """" 0 "° .,,..... 20 30 40 50 60 26(I~gree) Fig. 5 U.S. Patent Jul. 17, 2012 Sheet 7of10 US 8,221,791 Bl Fig. 6a Fig. 6b (•) Cu~ (b) - _. I '- -f' I .I 970 9 931 934 936 938 Bm.tiD. eV ) 132.1 015 (c) 5:tp3 103.1 (d} f It i Ii f 95 100 105 110 115 120 125 Fig. 6c Fig. 6d U.S. Patent Jul. 17, 2012 Sheet 8of10 US 8,221,791 Bl Fig. 7a Fig. 7b 50 Filter Paper Disc Fig. 7c No E.coli Growth ------... .:~".;:_-re. f; ... ~~ E.coli Colony '~
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