A Green Approach to Synthesize Silver Nanoparticles in Starch-co-Poly(acrylamide) Hydrogels by Tridax procumbens Leaf Extract and Their Antibacterial Activity
A series of starch-co-poly(acrylamide) (starch-co-PAAm) hydrogels were synthesized by employing free radical redox polymerization. A novel green approach, Tridax procumbens (TD) leaf extract, was used for reduction of silver ions (Ag+) into silver nanoparticles in the starch-co-PAAm hydrogel network. The formation of silver nanoparticles was confirmed by UV-visible spectroscopy (UV-Vis), thermogravimetric analysis (TGA), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and X-ray diffraction (X-RD) studies. 22% of weight loss difference between hydrogel and silver nanocomposite hydrogel (SNCH) clearly indicates the formation of silver nanoparticles by TGA. TEM images indicate the successful incorporation of silver nanoparticles ranging from 5 to 10？nm in size and spherical in shape with a narrow size distribution. These developed SNCHs were used to study the antibacterial activity by inhibition zone method against gram-positive and gram-negative bacteria such as Bacillus and Escherichia coli. The results indicated that these SNCHs can be used potentially for biomedical applications. 1. Introduction Hydrogels have three-dimensional polymeric networks that are fabricated from polymers stabilized through physical or chemical crosslinking. They absorb large quantities of water without losing their structural integrity [1]. Since they mimic body tissues and respond to external stimuli, they are made important and promising forms of biomaterials for various applications including tissue engineering, controlled drug release devices, biosensors, and mechanical actuators [2–4]. Due to the presence of water solubilizing groups, such as –OH, –COOH, –CONH2, –CONH–, and –SO3H, these hydrogels show higher hydrophilicity. The three-dimensional network of hydrogel provides relative stability to its structure. Their swollen state results from a balance between the dispersing forces acting on hydrated chains and cohesive forces that do not prevent the penetration of water through the network [5]. Based on these properties the hydrogels have been used recently as templates for production of metallic nanoparticles. Hence the design and development of metal nanoparticles dispersed in polymer matrix have attracted potential applications in various fields like electrical, optical, or mechanical properties [6, 7] making them valuable for applications in areas like optics [8], photo imaging and patterning [9], electronic devices [10], sensors and biosensors [11–13], catalysis [14, 15], and antibacterial and antimicrobial coatings [16]. Silver
References
[1]
K. Y. Lee and D. J. Mooney, “Hydrogels for tissue engineering,” Chemical Reviews, vol. 101, no. 7, pp. 1869–1879, 2001.
[2]
N. A. Peppas, P. Bures, W. Leobandung, and H. Ichikawa, “Hydrogels in pharmaceutical formulations,” European Journal of Pharmaceutics and Biopharmaceutics, vol. 50, no. 1, pp. 27–46, 2000.
[3]
J. Kim, I. S. Kim, T. H. Cho et al., “Bone regeneration using hyaluronic acid-based hydrogel with bone morphogenic protein-2 and human mesenchymal stem cells,” Biomaterials, vol. 28, no. 10, pp. 1830–1837, 2007.
[4]
N. A. Peppas, J. Z. Hilt, A. Khademhosseini, and R. Langer, “Hydrogels in biology and medicine: from molecular principles to bionanotechnology,” Advanced Materials, vol. 18, no. 11, pp. 1345–1360, 2006.
[5]
H. F. Mark, N. M. Bikals, C. G. Overberger, and J. I. Kroschwitz, Encyclopedia of Polymer Science and Engineering, Wiley-Interscience, New York, NY, USA, 1986.
[6]
Y. Xia, P. Yang, Y. Sun et al., “One-dimensional nanostructures: synthesis, characterization, and applications,” Advanced Materials, vol. 15, no. 5, pp. 353–389, 2003.
[7]
W. Caseri, “Nanocomposites of polymers and metals or semiconductors: historical background and optical properties,” Macromolecular Rapid Communications, vol. 21, no. 11, pp. 705–722, 2000.
[8]
M. José-Yacamán, R. Pérez, P. Santiago, M. Benaissa, K. Gonsalves, and G. Carlson, “Microscopic structure of gold particles in a metal polymer composite film,” Applied Physics Letters, vol. 69, no. 7, pp. 913–915, 1996.
[9]
F. Stellacci, C. A. Bauer, T. M. Friedrichsen et al., “Laser and electron-beam induced growth of nanoparticles for 2D and 3D metal patterning,” Advanced Materials, vol. 14, no. 3, pp. 194–198, 2002.
[10]
S. Pothukuchi, Y. Li, and C. P. Wong, “Development of a novel polymer-metal nanocomposite obtained through the route of in situ reduction for integral capacitor application,” Journal of Applied Polymer Science, vol. 93, no. 4, pp. 1531–1538, 2004.
[11]
D. N. Muraviev, J. Macanás, M. J. Esplandiu, M. Farre, M. Mu？oz, and S. Alegret, “Simple route for intermatrix synthesis of polymer stabilized core-shell metal nanoparticles for sensor applications,” Physica Status Solidi (A), vol. 204, no. 6, pp. 1686–1692, 2007.
[12]
J. Macanás, M. Farre, M. Mu？oz, S. Alegret, and D. N. Muraviev, “Preparation and characterization of polymer-stabilized metal nanoparticles for sensor applications,” Physica Status Solidi (A), vol. 203, no. 6, pp. 1194–1200, 2006.
[13]
F. P. Zamborini, M. C. Leopold, J. F. Hicks, P. J. Kulesza, M. A. Malik, and R. W. Murray, “Electron hopping conductivity and vapor sensing properties of flexible network polymer films of metal nanoparticles,” Journal of the American Chemical Society, vol. 124, no. 30, pp. 8958–8964, 2002.
[14]
D. N. Muraviev, J. Macanás, P. Ruiz, and M. Munoz, “Synthesis, stability and electrocatalytic activity of polymer-stabilized monometallic Pt and bimetallic Pt/Cu core-shell nanoparticles,” Physica Status Solidi (A), vol. 205, no. 6, pp. 1460–1464, 2008.
[15]
T. Yao, C. Wang, J. Wu et al., “Preparation of raspberry-like polypyrrole composites with applications in catalysis,” Journal of Colloid and Interface Science, vol. 338, no. 2, pp. 573–577, 2009.
[16]
K. Varaprasad, Y. Murali Mohan, S. Ravindra et al., “Hydrogel–silver nanoparticle composites: a new generation of antimicrobials,” Journal of Applied Polymer Science, vol. 115, no. 2, pp. 1199–1207, 2010.
[17]
Y. Mo, I. M？rke, and P. Wachter, “Surface enhanced Raman scattering of pyridine on silver surfaces of different roughness,” Surface Science, vol. 133, no. 1, pp. L452–L458, 1983.
[18]
Y.-C. Chung, I.-H. Chen, and C.-J. Chen, “The surface modification of silver nanoparticles by phosphoryl disulfides for improved biocompatibility and intracellular uptake,” Biomaterials, vol. 29, no. 12, pp. 1807–1816, 2008.
[19]
G. Cao, Nanostructures and Nanomaterials: Synthesis, Properties and Applications, Imperial College Press, London, UK, 2004.
[20]
N. Grier, Disinfection, Sterilization and Preservation, S. S. Block, Ed., Lea & Febiger, Philadelphia, Pa, USA, 3rd edition, 1983.
[21]
J. Kusnetsov, E. Iivanainen, N. Elomaa, O. Zacheus, and P. J. Martikainen, “Copper and silver ions more effective against Legionellae than against mycobacteria in a hospital warm water system,” Water Research, vol. 35, no. 17, pp. 4217–4225, 2001.
[22]
J. Keleher, J. Bashant, N. Heldt, L. Johnson, and Y. Li, “Photo-catalytic preparation of silver-coated TiO2 particles for antibacterial applications,” World Journal of Microbiology and Biotechnology, vol. 18, no. 2, pp. 133–139, 2002.
[23]
J.-Y. Li and A.-I. Yeh, “Relationships between thermal, rheological characteristics and swelling power for various starches,” Journal of Food Engineering, vol. 50, no. 3, pp. 141–148, 2001.
[24]
H. Mark and O. Kirk, Encyclopedia of Chemical Technology, John Willy & Sons, New York, NY, USA, 3rd edition, 1986.
[25]
S. C. Pang, S. F. Chin, S. H. Tay, and F. M. Tchong, “Starch–maleate–polyvinyl alcohol hydrogels with controllable swelling behaviors,” Carbohydrate Polymers, vol. 84, no. 1, pp. 424–429, 2011.
[26]
A. Biswas, R. L. Shogren, G. Selling, J. Salch, J. L. Willett, and C. M. Buchanan, “Rapid and environmentally friendly preparation of starch esters,” Carbohydrate Polymers, vol. 74, no. 1, pp. 137–141, 2008.
[27]
S. F. Chin, S. C. Pang, and L. S. Lim, “Synthesis and characterization of novel water soluble starch tartarate nanoparticles,” ISRN Materials Science, vol. 2012, Article ID 723686, 5 pages, 2012.
[28]
B. Singh, N. Chauhan, S. Kumar, and R. Bala, “Psyllium and copolymers of 2-hydroxylethylmethacrylate and acrylamide-based novel devices for the use in colon specific antibiotic drug delivery,” International Journal of Pharmaceutics, vol. 352, no. 1-2, pp. 74–80, 2008.
[29]
B. Singh and R. Bala, “Design of dietary polysaccharide and binary monomer mixture of acrylamide and 2-acrylamido-2-methylpropane sulphonic acid based antiviral drug delivery devices,” Chemical Engineering Research and Design, vol. 90, no. 3, pp. 346–358, 2012.
[30]
J. Rosiak, K. Burozak, and W. P？kala, “Polyacrylamide hydrogels as sustained release drug delivery dressing materials,” Radiation Physics and Chemistry, vol. 22, no. 3–5, pp. 907–915, 1983.
[31]
A. C. Babu, M. N. Prabhakar, A. S. Babu, B. Mallikarjuna, M. C. S. Subha, and K. C. Rao, “Development and characterization of semi-IPN silver nanocomposite hydrogels for antibacterial applications,” International Journal of Carbohydrate Chemistry, vol. 2013, Article ID 243695, 8 pages, 2013.
[32]
P. S. K. Murthy, Y. M. Mohan, K. Varaprasad, B. Sreedhar, and K. M. Raju, “First successful design of semi-IPN hydrogel–silver nanocomposites: a facile approach for antibacterial application,” Journal of Colloid and Interface Science, vol. 318, no. 2, pp. 217–224, 2008.
[33]
V. R. Babu, C. Kim, S. Kim, C. Ahn, and Y.-I. Lee, “Development of semi-interpenetrating carbohydrate polymeric hydrogels embedded silver nanoparticles and its facile studies on E. coli,” Carbohydrate Polymers, vol. 81, no. 2, pp. 196–202, 2010.
[34]
S. Ravindra, Y. M. Mohan, N. N. Reddy, and K. M. Raju, “Fabrication of antibacterial cotton fibres loaded with silver nanoparticles via ‘Green Approach’,” Colloids and Surfaces A, vol. 367, no. 1–3, pp. 31–40, 2010.
[35]
S. Barua, R. Konwarh, S. S. Bhattacharya et al., “Non-hazardous anticancerous and antibacterial colloidal “green”silver nanoparticles,” Colloids and Surfaces B, vol. 105, pp. 37–42, 2013.
[36]
C. Dipankar and S. Murugan, “The green synthesis, characterization and evaluation of the biological activities of silver nanoparticles synthesized from Iresine herbstii leaf aqueous extracts,” Colloids and Surfaces B, vol. 98, pp. 112–119, 2012.
[37]
V. S. Kotakadi, Y. S. Rao, S. A. Gaddam, T. N. V. K. Prasad, A. V. Reddy, and D. V. R. S. Gopai, “Simple and rapid biosynthesis of stable silver nanoparticles using dried leaves of Catharanthus roseus. Linn. G. Donn and its antimicrobial activity,” Colloids and Surfaces B, vol. 105, pp. 194–198, 2013.
[38]
L. Suseela, A. Sarsvathy, and P. Brindha, “Pharmacognostic studies on Tridax procumbens L. (Asteraceae),” Journal of Phytological Research, vol. 15, no. 2, pp. 141–147, 2002.
[39]
M. H. Prasad, C. Rameshz, N. Jayakumar, V. Ragunathan, and D. Kalpana, “Biosynthesis of bimetallic Ag/Cu2O nanocomposites using Tridax procumbens leaf extract,” Advanced Science, Engineering and Medicine, vol. 4, no. 1, pp. 85–88, 2012.
[40]
H. Acharya, J. Sung, H.-I. Shin, S.-Y. Park, B. G. Min, and C. Park, “Deposition of silver nanoparticles on single wall carbon nanotubes via a self assembled block copolymer micelles,” Reactive and Functional Polymers, vol. 69, no. 7, pp. 552–557, 2009.
[41]
K. B. Holt and A. J. Bard, “Interaction of silver(I) ions with the respiratory chain of Escherichia coli: an electrochemical and scanning electrochemical microscopy study of the antimicrobial mechanism of micromolar Ag+,” Biochemistry, vol. 44, no. 39, pp. 13214–13223, 2005.
[42]
C.-N. Lok, C.-M. Ho, R. Chen et al., “Proteomic analysis of the mode of antibacterial action of silver nanoparticles,” Journal of Proteome Research, vol. 5, no. 4, pp. 916–924, 2006.
