Bioprocess and Biosystems Engineering

, Volume 39, Issue 5, pp 759–772 | Cite as

Plant extract-mediated biogenic synthesis of silver, manganese dioxide, silver-doped manganese dioxide nanoparticles and their antibacterial activity against food- and water-borne pathogens

  • Chandran Krishnaraj
  • Byoung-Jun Ji
  • Stacey L. Harper
  • Soon-Il Yun
Original Paper


Silver nanoparticles (AgNPs), manganese dioxide nanoparticles (MnO2NPs) and silver-doped manganese dioxide nanoparticles (Ag-doped MnO2NPs) were synthesized by simultaneous green chemistry reduction approach. Aqueous extract from the leaves of medicinally important plant Cucurbita pepo was used as reducing and capping agents. Various characterization techniques were carried out to affirm the formation of nanoparticles. HR-TEM analysis confirmed the size of nanoparticles in the range of 15–70 nm and also metal doping was confirmed through XRD and EDS analyses. FT-IR analysis confirmed that the presence of biomolecules in the aqueous leaves extract was responsible for nanoparticles synthesis. Further, the concentration of metals and their doping in the reaction mixture was achieved by ICP–MS. The growth curve and well diffusion study of synthesized nanoparticles were performed against food- and water-borne Gram-positive and Gram-negative bacterial pathogens. The mode of interaction of nanoparticles on bacterial cells was demonstrated through Bio-TEM analysis. Interestingly, AgNPs and Ag-doped MnO2 NPs showed better antibacterial activity against all the tested bacterial pathogens; however, MnO2NPs alone did not show any antibacterial properties. Hence, AgNPs and Ag-doped MnO2 NPs synthesized from aqueous plant leaves extract may have important role in controlling various food spoilage caused by bacteria.


Cucurbita pepo leaves extract AgNPs MnO2NPs Ag-doped MnO2NPs Antibacterial activity 



This research was supported by Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Education (2013R1A1A2007953) and also funds from Chonbuk National University, Republic of Korea.


  1. 1.
    Jaganyi D, Altaf M, Wekesa I (2013) Synthesis and characterization of whisker-shaped MnO2 nanostructure at room temperature. Appl Nanosci 3:329–333CrossRefGoogle Scholar
  2. 2.
    Xu R, Wang D, Zhang J, Li Y (2006) Shape-dependent catalytic activity of silver nanoparticles for the oxidation of styrene. Chem Asian J 1:888–893CrossRefGoogle Scholar
  3. 3.
    Ren X, Meng X, Chen D, Tang F, Jiao J (2005) Using silver nanoparticle to enhance current response of biosensor. Biosens Bioelectron 21:433–437CrossRefGoogle Scholar
  4. 4.
    Wei H, Li J, Wang YL, Wang EL (2007) Silver nanoparticles coated with adenine: preparation, self-assembly and application in surface-enhanced Raman scattering. Nanotechnology 18:175610CrossRefGoogle Scholar
  5. 5.
    Krishnaraj C, Muthukumaran P, Ramachandran R, Balakumaran MD, Kalaichelvan PT (2014) Acalypha indica Linn: biogenic synthesis of silver and gold nanoparticles and their cytotoxic effects against MDA-MB-231, human breast cancer cells. Biotechnol Rep 4:42–49CrossRefGoogle Scholar
  6. 6.
    Reddy AS, Chen CY, Chen CC, Jean JS, Chen HR, Tseng MJ, Fan CW, Wang JC (2010) Biological synthesis of gold and silver nanoparticles mediated by the bacteria Bacillus subtilis. J Nanosci Nanotechnol 10:6567–6574CrossRefGoogle Scholar
  7. 7.
    Li G, He D, Qian Y, Guan B, Gao S, Cui Y, Yokoyama K, Wang L (2012) Fungus-mediated green synthesis of silver nanoparticles using Aspergillus terreus. Int J Mol Sci 13:466–476CrossRefGoogle Scholar
  8. 8.
    Binupriya A, Sathishkumar M, Yun S (2010) Biocrystallization of silver and gold ions by inactive cell filtrate of Rhizopus stolonifer. Colloid Surf B 79:531–534CrossRefGoogle Scholar
  9. 9.
    Binupriya A, Sathishkumar M, Yun S (2010) Myco-crystallization of silver ions to nanosized particles by live and dead cell filtrates of Aspergillus oryzae var. viridis and its bactericidal activity toward Staphylococcus aureus KCCM 12256. Ind Eng Chem Res 49:852–858CrossRefGoogle Scholar
  10. 10.
    Saravanan M, Amelash T, Negash L, Gebreyesus A, Selvaraj A, Rayar V, Deekonda K (2013) Extracellular biosynthesis and biomedical application of silver nanoparticles synthesized from Baker’s Yeast. Int J Res Pharm Biomed Sci 4:822–828Google Scholar
  11. 11.
    Rajeshkumar S, Malarkodi C, Paulkumar K, Vanaja M, Gnanajobitha G, Annadurai G (2014) Algae mediated green fabrication of silver nanoparticles and examination of its antifungal activity against clinical pathogens. Int J Metal. doi: 10.1155/2014/692643 Google Scholar
  12. 12.
    Sathishkumar M, Mahadevan A, Pavagadhi S, Kaushik R, Sharma VK, Balasubramanian R (2013) Biological synthesis of silver nanoparticles and assessment of their bactericidal activity. Sustainable nanotechnology and the environment: advances and achievements. ACS 7:107–120Google Scholar
  13. 13.
    Krishnaraj C, Jagan EG, Rajasekar S, Selvakumar P, Kalaichelvan PT, Mohan N (2010) Synthesis of silver nanoparticles using Acalypha indica leaf extracts and its antibacterial activity against water borne pathogens. Colloids Surf B Biointerfaces 76:50–56CrossRefGoogle Scholar
  14. 14.
    Kunkalekar RK, Naik MM, Dubey SK, Salker AV (2013) Antibacterial activity of silver-doped manganese dioxide nanoparticles on multidrug-resistant bacteria. J Chem Technol Biotechnol 88:873–877CrossRefGoogle Scholar
  15. 15.
    Jana S, Basu S, Pande S, Ghosh SK, Pal T (2007) Shape-selective synthesis, magnetic properties, and catalytic activity of single crystalline B-MnO2 nanoparticles. J Phys Chem C 111:16272–16277CrossRefGoogle Scholar
  16. 16.
    Khan Z, Thabaiti SA, Obaid AY, Khan ZA (2010) MnO2 nanostructures of different morphologies from amino acids- MnO4 reactions in aqueous solutions. Colloids Surf B Biointerface 81:381–384CrossRefGoogle Scholar
  17. 17.
    Troy MB, Westerhoff P (2008) Nanoparticle silver released into water from commercially available sock fabrics. Environ Sci Technol 42:4133–4139CrossRefGoogle Scholar
  18. 18.
    Kessler R (2011) Engineered nanoparticles in consumer products: understanding a new ingredient. Environ Health Perspect 119:A120–A125CrossRefGoogle Scholar
  19. 19.
    Sathishkumar M, Sneha K, Yun YS (2010) Immobilization of silver nanoparticles synthesized using Curcuma longa tuber powder and extract on cotton cloth for bactericidal activity. Bioresour Technol 101:7958–7965CrossRefGoogle Scholar
  20. 20.
    Sathishkumar M, Sneha K, Won SW, Cho CW, Kim S, Yun YS (2009) Cinnamon zeylanicum bark extract and powder mediated green synthesis of nano-crystalline silver particles and its bactericidal activity. Colloids Surf B 73:332–338CrossRefGoogle Scholar
  21. 21.
    Krishnaraj C, Ramachandran R, Mohan K, Kalaichelvan PT (2012) Optimization for rapid synthesis of silver nanoparticles and its effect on phytopathogenic fungi. Spectrochim Acta A Mol Biomol Spectorsc 93:95–99CrossRefGoogle Scholar
  22. 22.
    Sneha K, Sathishkumar M, Mao J, Kwak IS, Yun YS (2010) Corynebacterium glutamicum-mediated crystallization of silver ions through sorption and reduction processes. Chem Eng J 162:989–996CrossRefGoogle Scholar
  23. 23.
    Kunkalekar RK, Salker AV (2010) Low temperature carbon monoxide oxidation over nanosized silver doped manganese dioxide catalysts. Catal Commun 12:193–196CrossRefGoogle Scholar
  24. 24.
    Martınez-Castanon GA, Nino-Martınez N, Martınez-Gutierrez F, Martınez-Mendoza JR, Ruiz FJ (2008) Synthesis and antibacterial activity of silver nanoparticles with different sizes. Nanoparticle Res 10:1343–1348CrossRefGoogle Scholar
  25. 25.
    Naik B, Desai V, Kowshik M, Prasad VS, Fernando GF, Ghosh NN (2011) Synthesis of Ag/AgCl–mesoporous silica nanocomposites using a simple aqueous solution-based chemical method and a study of their antibacterial activity on E. coli. Particuology 9:243–247CrossRefGoogle Scholar
  26. 26.
    Pal S, Tak YK, Song JM (2007) Does the antibacterial activity of silver nanoparticles depend on the shape of the nanoparticle? A Study of the gram-negative bacterium Escherichia coli. Appl Environ Microbiol 73:1712–1720CrossRefGoogle Scholar
  27. 27.
    Krishnaraj C HS, Choe HS, Kim KP, Yun SI (2015) Mechanistic aspects of biologically synthesized silver nanoparticles against food- and water-borne microbes. Bioprocess Biosyst Eng 38:1943–1958CrossRefGoogle Scholar
  28. 28.
    Klaine SJ, Alvarez PJJ, Batley GE, Fernandes TF, Handy RD, Lyon DY, Mahendra S, McLaughlin MJ, Lead JR (2008) Nanomaterials in the environment: behavior, fate, bioavailability, and effects. Environ Toxicol Chem 27:1825–1851CrossRefGoogle Scholar
  29. 29.
    Salker AV, Kunkalekar RK (2009) Palladium doped manganese dioxide catalysts for low temperature carbon monoxide oxidation. Catal Commun 10:1776–1780CrossRefGoogle Scholar
  30. 30.
    Iwu MW (1983) Traditional Igbo medicine. Institute of African Studies University of Nigeria, NsukkaGoogle Scholar
  31. 31.
    Oyewole OA, Abalaka ME (2012) Antimicrobial activities of Telfairia occidentalis (fluted pumpkins) leaf extract against selected intestinal pathogens. J Health Sci 2:1–4Google Scholar
  32. 32.
    Gbile ZO (1986) (ed) Ethnobotany, taxonomy and conservation of Medicinal plants in A. Sofowora “The state of Medicinal plant Research”. University of Ibadan press, Ibadan, Nigeria, pp 13–29Google Scholar
  33. 33.
    Mulvaney P (1996) Surface plasmon spectroscopy of nanosized metal particles. Langmuir 12:788–800CrossRefGoogle Scholar
  34. 34.
    Chacon-Patino ML, Blanco-Tirado C, Hinestroza JP, Combariza MY (2013) Biocomposite of nanostructured MnO2 and fique fibers for efficient dye degradation. Green Chem 15:2920CrossRefGoogle Scholar
  35. 35.
    Moon SA, Salunke BK, Alkotaini B, Sathiyamoorthi E, Kim BS (2015) Biological synthesis of manganese dioxide nanoparticles by Kalopanax pictus plant extract. IET Nanobiotechnol 9:220–225CrossRefGoogle Scholar
  36. 36.
    Jana S, Pande S, Sinha AK, Sarkar S, Pradhan M, Basu M, Saha S, Pal T (2009) A green chemistry approach for the synthesis of flower-like Ag-doped MnO2 nanostructures probed by surface-enhanced Raman spectroscopy. J Phys Chem C 113:1386–1392CrossRefGoogle Scholar
  37. 37.
    Shankar SS, Rai A, Ahmad A, Sastry M (2004) Rapid synthesis of Au, Ag and bimetallic Au core Ag shell nanoparticles using Neem (Azadirachta indica) leaf broth. J Colloid Interface Sci 275:496–502CrossRefGoogle Scholar
  38. 38.
    Song JY, Kim BS (2009) Rapid biological synthesis of silver nanoparticles using plant leaf extract. Bioprocess Biosyst Eng 32:79–84CrossRefGoogle Scholar
  39. 39.
    Banerjee P, Satapathy M, Mukhopahayay A, Das P (2014) Leaf extract mediated green synthesis of silver nanoparticles from widely available Indian plants: synthesis, characterization, antimicrobial property and toxicity analysis. Bioresour Bioprocess 1:3CrossRefGoogle Scholar
  40. 40.
    Jose D, Jagirdar BR (2011) Ag@Pd core-shell nanoparticles. Indian J Chem 50:1308–1317Google Scholar
  41. 41.
    Chen W, Rakhi RB, Hu L, Xie X, Cui Y, Alshareef HN (2011) High-performance nanostructured supercapacitors on a sponge. Nano Lett 11:5165–5172CrossRefGoogle Scholar
  42. 42.
    Elavazhagan T, Arunachalam KD (2011) Memecylon edule leaf extract mediated green synthesis of silver and gold nanoparticles. Int J Nanomed 6:1265–1278CrossRefGoogle Scholar
  43. 43.
    Sondi I, Salopek-Sondi B (2004) Silver nanoparticles as antimicrobial agent: a case study on E. coli as a model for Gram-negative bacteria. J Colloid Interface Sci 275:177–182CrossRefGoogle Scholar
  44. 44.
    Kunkalekar RK, Prabhu MS, Naik MM, Salkera AV (2014) Silver-doped manganese dioxide and trioxide nanoparticles inhibit both gram positive and gram negative pathogenic bacteria. Colloid Surf B Biointerface 113:429–434CrossRefGoogle Scholar
  45. 45.
    Prabhu S, Poulose EK (2012) Silver nanoparticles: mechanism of antimicrobial action, synthesis, medical applications, and toxicity effects. Int Nano Lett 2:32CrossRefGoogle Scholar
  46. 46.
    Ganeshprabu P, Selvi S, Mathivanan V (2013) Antibacterial activity of silver nanoparticles against bacterial pathogens from gut of silkworm, Bombyx mori (L.) (Lepidoptera: Bombycidae). Int J Res Pure Appl Microbiol 3:89–93Google Scholar
  47. 47.
    Kora AJ, Sashidhar RB, Arunachalam J (2010) Gum kondagogu (Cochlospermum gossypium): a template for the green synthesis and stabilization of silver nanoparticles with antibacterial application. Carbohydr Polym 82:670–679CrossRefGoogle Scholar
  48. 48.
    Yamanaka M, Hara K, Kudo J (2005) Bactericidal actions of a silver ion solution on Escherichia coli, studied by energy-filtering transmission electron microscopy and proteomic analysis. Appl Environ Microbiol 71:7589–7593CrossRefGoogle Scholar
  49. 49.
    Shahverdi AR, Fakhimi A, Shahverdi HR, Minaian S (2007) Synthesis and effect of silver nanoparticles on the antibacterial activity of different antibiotics against Staphylococcus aureus and Escherichia coli. Nanomed Nanotechnol Biol Med 3:168–171CrossRefGoogle Scholar

Copyright information

© Springer-Verlag Berlin Heidelberg 2016

Authors and Affiliations

  • Chandran Krishnaraj
    • 1
  • Byoung-Jun Ji
    • 1
  • Stacey L. Harper
    • 2
  • Soon-Il Yun
    • 1
  1. 1.Department of Food Science and Technology, College of Agriculture and Life SciencesChonbuk National UniversityJeonjuRepublic of Korea
  2. 2.Department of Environmental and Molecular ToxicologyOregon State UniversityCorvallisUSA

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