Skip to main content
SpringerLink
Log in

Agglomeration, isolation and dissolution of commercially manufactured silver nanoparticles in aqueous environments

  • Research Paper
  • Published:
Journal of Nanoparticle Research Aims and scope Submit manuscript

Abstract

The increasing use of manufactured nanoparticles ensures these materials will make their way into the environment. Silver nanoparticles in particular, due to use in a wide range of applications, have the potential to get into water systems, e.g., drinking water systems, ground water systems, estuaries, and/or lakes. One important question is what is the chemical and physical state of these nanoparticles in water? Are they present as isolated particles, agglomerates or dissolved ions, as this will dictate their fate and transport. Furthermore, does the chemical and physical state of the nanoparticles change as a function of size or differ from micron-sized particles of similar composition? In this study, an electrospray atomizer coupled to a scanning mobility particle sizer (ES-SMPS) is used to investigate the state of silver nanoparticles in water and aqueous nitric acid environments. Over the range of pH values investigated, 0.5–6.5, silver nanoparticles with a bimodal primary particle size distribution with the most intense peak at 5.0 ± 7.4 nm, as determined from transmission electron microscopy (TEM), show distinct size distributions indicating agglomeration between pH 6.5 and 3 and isolated nanoparticles at pH values from 2.5 to 1. At the lowest pH investigated, pH 0.5, there are no peaks detected by the SMPS, indicating complete nanoparticle dissolution. Further analysis of the solution shows dissolved Ag ions at a pH of 0.5. Interestingly, silver nanoparticle dissolution shows size dependent behavior as larger, micron-sized silver particles show no dissolution at this pH. Environmental implications of these results are discussed.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8
Fig. 9

Similar content being viewed by others

References

  • Agency for Toxic Substances and Disease Registry (ATSDR) (1990) Toxicological profile for silver. In: US Department of Health and Human Services, Public Health Service and Agency for Toxic Substances and Disease Registry (Eds). Atlanta, GA

  • Alvarez PJ (2006) Nanotechnology in the environment—the good, the bad, and the ugly. J Environ Eng Asce 132(10):1233

    Article  CAS  Google Scholar 

  • Anselmann R (2001) Nanoparticles and nanolayers in commercial applications. J Nanopart Res 3(4):329–336

    Article  CAS  Google Scholar 

  • Asharani PVN, Gong ZY, Hande MP, Valiyaveettil S (2007) Potential health impacts of silver nanoparticles. Chem Res Toxicol 20(12):99

    Google Scholar 

  • Asharani PV, Wu YL, Gong ZY, Valiyaveettil S (2008) Toxicity of silver nanoparticles in zebrafish models. Nanotechnology 19(25):5102–5109

    Article  Google Scholar 

  • Becher P, Schuster D (1983) Encyclopedia of emulsion technology: basic theory, measurement, applications, vol 1. M. Dekker, New York

  • Benn TM, Westerhoff P (2008) Nanoparticle silver released into water from commercially available sock fabrics. Environ Sci Technol 42(11):4133–4139

    Article  CAS  PubMed  Google Scholar 

  • Borm P, Klaessig FC, Landry TD, Moudgil B, Pauluhn J, Thomas K, Trottier R, Wood S (2006) Research strategies for safety evaluation of nanomaterials. Part V. Role of dissolution in biological fate and effects of nanoscale particles. Toxicol Sci 90(1):23–32

    Article  CAS  PubMed  Google Scholar 

  • Bottger PHM, Bi Z, Adolph D, Dick KA, Karlsson LS, Karlsson MNA, Wacaser BA, Deppert K (2007) Electrospraying of colloidal nanoparticles for seeding of nanostructure growth. Nanotechnology 18(10):5304–5309

    Article  Google Scholar 

  • Chen KL, Elimelech M (2006) Aggregation and deposition kinetics of fullerene (C-60) nanoparticles. Langmuir 22(26):10994–11001

    Article  CAS  PubMed  Google Scholar 

  • Chen KL, Elimelech M (2007) Influence of humic acid on the aggregation kinetics of fullerene (C-60) nanoparticles in monovalent and divalent electrolyte solutions. J Colloid Interf Sci 309(1):126–134

    Article  CAS  Google Scholar 

  • Chen X, Schluesener HJ (2008) Nanosilver: a nanoproduct in medical application. Toxicol Lett 176(1):1–12

    Article  CAS  PubMed  Google Scholar 

  • Chen Y, Wang CG, Ma ZF, Su ZM (2007) Controllable colours and shapes of silver nanostructures based on pH: application to surface-enhanced Raman scattering. Nanotechnology 18(32):5602–5606

    Google Scholar 

  • Cwiertny DM, Baltrusaitis J, Hunter GJ, Laskin A, Scherer MM, Grassian VH (2008). Characterization and acid-mobilization study of iron-containing mineral dust source materials. J Geophys Res 113(D05202). doi:10.1029/2007JD009332

  • Doumanidis H (2002) The Nanomanufacturing programme at the National Science Foundation. Nanotechnology 13(3):248–252

    Article  ADS  Google Scholar 

  • Eckelman MJ, Graedel TE (2007) Silver emissions and their environmental impacts: a multilevel assessment. Environ Sci Technol 41(17):6283–6289

    Article  CAS  PubMed  Google Scholar 

  • Emerich DF, Thanos CG (2003) Nanotechnology and medicine. Expert Opin Biol Therapy 3(4):655–663

    Article  CAS  Google Scholar 

  • Falkenhagen D (1995) Small particles in medicine. Artif Organs 19(8):792–794

    Article  CAS  PubMed  Google Scholar 

  • Fornes JA (1985) Secondary minimum analysis in the DLVO-theory. Colloid Polym Sci 263(12):1004–1007

    Article  CAS  Google Scholar 

  • Frank BP, Saltiel S, Hogrefe O, Grygas J, Lala GG (2008) Determination of mean particle size using the electrical aerosol detector and the condensation particle counter: comparison with the scanning mobility particle sizer. J Aerosol Sci 39(1):19–29

    Article  CAS  Google Scholar 

  • Gao XY, Wang SY, Li J, Zheng YX, Zhang RJ, Zhou P, Yang YM, Chen LY (2004) Study of structure and optical properties of silver oxide films by ellipsometry, XRD and XPS methods. Thin Solid Films 455:438–442

    Article  ADS  Google Scholar 

  • Grassian VH (2008) When size really matters: size-dependent properties and surface chemistry of metal and metal oxide nanoparticles in gas and liquid phase environments. J Phys Chem C 112(47):18303–18313

    CAS  Google Scholar 

  • Grassian VH (2009) New directions: nanodust—a source of metals in the atmospheric environment? Atmos Environ 43(30):4666–4667

    Article  CAS  Google Scholar 

  • Griffitt RJ, Luo J, Gao J, Bonzongo JC, Barber DS (2008) Effects of particle composition and species on toxicity of metallic nanomaterials in aquatic organisms. Environ Toxicol Chem 27(9):1972–1978

    Article  CAS  PubMed  Google Scholar 

  • Gupta RB, Kompella UB (2006) Physical characterization of nanoparticles. In: Gupta RB, Kompella UB (eds) Nanoparticle technology for drug delivery. Taylor & Francis Group, New York, p 109

    Google Scholar 

  • Guzman KAD, Taylor MR, Banfield JF (2006) Environmental risks of nanotechnology: national nanotechnology initiative funding, 2000–2004. Environ Sci Technol 40(5):1401–1407

    Article  PubMed  Google Scholar 

  • Howe PD, Dobson S (2002) Silver and silver compounds: environmental aspects. In: United Nations Environment Programme, International Labour Organization, World Health Organization and Inter-Organization Programme for the Sound Management of Chemicals (Eds), Geneva

  • Huang F, Gilbert B, Zhang HH, Banfield JF (2004) Reversible, surface-controlled structure transformation in nanoparticles induced by an aggregation state. Phys Rev Lett 92(15):5501.1–5501.4

    Google Scholar 

  • Kuchibhatla SV, Karakoti AS, Seal S (2008) Colloidal stability by surface modification. J Miner Met Mater Soc 57(12):52–56

    Google Scholar 

  • Lecoanet HF, Bottero JY, Wiesner MR (2004) Laboratory assessment of the mobility of nanomaterials in porous media. Environ Sci Technol 38(19):5164–5169

    Article  CAS  PubMed  Google Scholar 

  • Lowe T (2002) The revolution in nanometals. Adv Mater Process 160(1):63–65

    CAS  Google Scholar 

  • Lubick N (2008) Nanosilver toxicity: ions, nanoparticies-or both? Environ Sci Technol 42(23):8617

    Article  CAS  PubMed  Google Scholar 

  • Luoma SN (2008) Silver nanotechnologies and the environment: old problems or new challenges? Woodrow Wilson International Center for Scholars, Washington

  • Maynard AD (2006) Nanotechnology: a research strategy for addressing risk. Woodrow Wilson International Center for Scholars, Washington

  • McAllister K, Sazani P, Adam M, Cho MJ, Rubinstein M, Samulski RJ, DeSimone JM (2002) Polymeric nanogels produced via inverse microemulsion polymerization as potential gene and antisense delivery agents. J Am Chem Soc 124(51):15198–15207

    Article  CAS  PubMed  Google Scholar 

  • Meskhidze N, Chameides WL, Nenes A, Chen G (2003) Iron mobilization in mineral dust: Can anthropogenic SO2 emissions affect ocean productivity? Geophys Res Lett 30(21):2085

    Article  ADS  Google Scholar 

  • Meskhidze N, Chameides WL, Nenes A (2005) Dust and pollution: a recipe for enhanced ocean fertilization? J Geophys Res 110:D03301

    Article  Google Scholar 

  • Moskovits M, Vlckova B (2005) Adsorbate-induced silver nanoparticle aggregation kinetics. J Phys Chem B 109(31):14755–14758

    Article  CAS  PubMed  Google Scholar 

  • Mueller NC, Nowack B (2008) Exposure modeling of engineered nanoparticles in the environment. Environ Sci Technol 42(12):4447–4453

    Article  CAS  PubMed  Google Scholar 

  • Navarro E, Piccapietra F, Wagner B, Marconi F, Kaegi R, Odzak N, Sigg L, Behra R (2008) Toxicity of silver nanoparticles to Chlamydomonas reinhardtii. Environ Sci Technol 42(23):8959–8964

    Article  CAS  PubMed  Google Scholar 

  • Oberdorster G, Maynard A, Donaldson K, Castranova V, Fitzpatrick J, Ausman K, Carter J, Karn B, Kreyling W, Lai D, Olin S, Monteiro-Riviere N, Warheit D, Yang H (2005) Principles for characterizing the potential human health effects from exposure to nanomaterials: elements of a screening strategy. Part Fibre Toxicol 2:8

    Article  PubMed  Google Scholar 

  • Ozmetin C, Copur M, Yartasi A, Kocakerim MM (2000) Kinetic investigation of reaction between metallic silver and nitric acid solutions. Chem Eng Technol 23(8):707–711

    Article  CAS  Google Scholar 

  • Panyala NR, Pena-Mendez EM, Havel J (2008) Silver or silver nanoparticles: a hazardous threat to the environment and human health? J Appl Biomed 6(3):117–129

    CAS  Google Scholar 

  • Pease LF, Tsai DH, Zangmeister RA, Zachariah MR, Tarlov MJ (2007) Quantifying the surface coverage of conjugate molecules on functionalized nanoparticles. J Phys Chem C 111:17155–17157

    Article  CAS  Google Scholar 

  • Pettibone JB, Elzey S, Grassian VH (2008) An integrated approach toward understanding the environmental fate, transport, toxicity and health hazards of nanomaterials. In: Grassian VH (ed) Nanoscience and nanotechnology: environmental and health impacts. Wiley, Hoboken, p 47

    Google Scholar 

  • Powers KW, Brown SC, Krishna VB, Wasdo SC, Moudgil BM, Roberts SM (2006) Research strategies for safety evaluation of nanomaterials. Part VI. Characterization of nanoscale particles for toxicological evaluation. Toxicol Sci 90(2):296–303

    Article  CAS  PubMed  Google Scholar 

  • Richardson SD (2007) Water analysis: emerging contaminants and current issues. Anal Chem 79(12):4295–4323

    Article  CAS  PubMed  Google Scholar 

  • Sadrnezhaad SK, Ahmadi E, Mozammel M (2006) Kinetics of silver dissolution in nitric acid from Ag-AU(0.04)-CU0.10 and Ag–Cu-0.23 scraps. J Mater Sci Technol 22(5):696–700

    CAS  Google Scholar 

  • Schneider T, Jensen KA (2008) Combined single-drop and rotating drum dustiness test of fine to nanosize powders using a small drum. Ann Occup Hyg 52(1):23–34

    Article  CAS  PubMed  Google Scholar 

  • Shin W, Wang J, Mertler M, Sachweh B, Fissan H, Pui D (2009) Structural properties of silver nanoparticle agglomerates based on transmission electron microscopy: relationship to particle mobility analysis. J Nanopart Res 11(1):163–173

    Article  CAS  Google Scholar 

  • Skebo JE, Grabinski CM, Schrand AM, Schlager JJ, Hussain SM (2007) Assessment of metal nanoparticle agglomeration, uptake, and interaction using high-illuminating system. Int J Toxicol 26(2):135–141

    Article  CAS  PubMed  Google Scholar 

  • Suh J, Han B, Okuyama K, Choi M (2005) Highly charging of nanoparticles through electrospray of nanoparticle suspension. J Colloid Interf Sci 287(1):135–140

    Article  CAS  Google Scholar 

  • Tinke AP, Govoreanu R, Vanhoutte K (2006) Particle size and shape characterization of nano and submicron liquid dispersions. Am Pharm Rev 9(6):1–5

    Google Scholar 

  • Tsai CJ, Wu CH, Leu ML, Chen SC, Huang CY, Tsai PJ, Ko FH (2009) Dustiness test of nanopowders using a standard rotating drum with a modified sampling train. J Nanopart Res 11(1):121–131

    Article  CAS  Google Scholar 

  • TSI I. (2008) Real-time measurement of nanoparticle size distributions using electrical mobility technique. Vol. Application Note SMPS-004

  • U. S. Environmental Protection Agency (2006) High production volume information system (HPVIS). In: U.S.E.P. Agency (Ed)

  • Wada Y, Totoki S, Watanabe M, Moriya N, Tsunazawa Y, Shimaoka H (2006) Nanoparticle size analysis with relaxation of induced grating by dielectrophoresis. Optics Express 14(12):5755–5764

    Article  PubMed  ADS  Google Scholar 

  • Wiesner MR, Lowry GV, Alvarez P, Dionysiou D, Biswas P (2006) Assessing the risks of manufactured nanomaterials. Environ Sci Technol 40(14):4336–4345

    Article  CAS  PubMed  Google Scholar 

  • Wijnhoven SWP, Peijnenburg WJGM, Herberts CA, Hagens WI, Oomen AG, Heugens EHW, Roszek B, Bisschops J, Gosens I, Van De Meent D, Dekkers S, De Jong WH, van Zijverden M, Sips AJAM, Geertsma RE (2009) Nano-silver—a review of available data and knowledge gaps in human and environmental risk assessment. Nanotoxicology 3(2):109–138

    Article  Google Scholar 

  • Xu RL (2008) Progress in nanoparticles characterization: Sizing and zeta potential measurement. Particuology 6(2):112–115

    Article  CAS  Google Scholar 

  • Zelenyuk A, Cai Y, Imre D (2006) From agglomerates of spheres to irregularly shaped particles: determination of dynamic shape factors from measurements of mobility and vacuum aerodynamic diameters. Aerosol Sci Technol 40(3):197–217

    Article  CAS  Google Scholar 

Download references

Acknowledgments

The authors would like to thank Dr. Jonas Baltrusaitis for the XPS analysis. Although the research described in this article has been funded wholly or in part by the Environmental Protection Agency through grant number EPA R83389101-0 to VHG, it has not been subjected to the Agency’s required peer and policy review and therefore does not necessarily reflect the views of the Agency and no official endorsement should be inferred. This research was also supported in part by the Department of Defense (DoD) through the National Defense Science & Engineering Graduate Fellowship (NDSEG) Program and by the Center for Health Effects of Environmental Contamination. CRIF equipment grant 0639096 from the National Science Foundation is also gratefully acknowledged.

Author information

Authors and Affiliations

  1. Department of Chemical and Biochemical Engineering, University of Iowa, Iowa City, IA, 52242, USA

    Sherrie Elzey & Vicki H. Grassian

  2. Department of Chemistry, University of Iowa, Iowa City, IA, 52242, USA

    Vicki H. Grassian

  3. Nanoscience and Nanotechnology Institute, University of Iowa, Iowa City, IA, 52242, USA

    Vicki H. Grassian

Authors
  1. Sherrie Elzey
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Vicki H. Grassian
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Vicki H. Grassian.

Rights and permissions

Reprints and permissions

About this article

Cite this article

Elzey, S., Grassian, V.H. Agglomeration, isolation and dissolution of commercially manufactured silver nanoparticles in aqueous environments. J Nanopart Res 12, 1945–1958 (2010). https://doi.org/10.1007/s11051-009-9783-y

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11051-009-9783-y

Keywords

Search

Navigation