Skip to main content
SpringerLink
Log in

An effective approach for size characterization and mass quantification of silica nanoparticles in coffee creamer by AF4-ICP-MS

  • Research Paper
  • Published:
Analytical and Bioanalytical Chemistry Aims and scope Submit manuscript

Abstract

Silicon dioxide (SiO2) has been used as a food additive (E551) for decades. However, some safety concerns have been raised recently due to the detection of silica nanoparticles (SiO2 NPs) in a variety of foodstuffs and their unknown long-term health risk to humans. In order for risk assessment to be conducted, it is essential to establish a reliable, valid, and pragmatic method for analysis of SiO2 NPs in foods for estimation of exposure. This paper presents an effective approach for both size characterization and mass quantification of SiO2 NPs in commercial high-fat coffee creamer using asymmetric flow field-flow fractionation (AF4) coupled to inductively coupled plasma mass spectrometry (ICP-MS). SiO2 NPs from coffee creamer were well extracted after cleanup with hexane in a two-phase (hexane vs. water) aqueous environment. Size determination of SiO2 NPs was performed by on-line AF4-ICP-MS based on calibration with monodispersed standards. The dominant primary size of SiO2 NPs in the studied sample was 36.5 nm. The mass percentages of SiO2 NPs (vs. total SiO2) were 18.6% for the dominant primary nano-silica particles by prechannel calibration and 35.7% for total SiO2 NPs (≤ 100 nm) by postchannel calibration, with recoveries of 89–96% for the former and 75% for the latter. The established approach was demonstrated to be efficient and practical for routine analysis of polydispersed SiO2 NPs with wide nano-size distribution in coffee creamer. This method may be extended to monitor the presence of SiO2 NPs in other similar complex food matrices.

Graphical abstract

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

Similar content being viewed by others

References

  1. Mattarozzi M, Suman M, Cascio C, Calestani D, Weigel S, Undas A, et al. Analytical approaches for the characterization and quantification of nanoparticles in food and beverages. Anal Bioanal Chem. 2017;409(1):63–80.

    Article  CAS  PubMed  Google Scholar 

  2. Calzolai L, Gilliland D, Rossi F. Measuring nanoparticles size distribution in food and consumer products: a review. Food Addit Contam Part A Chem Anal Control Expo Risk Assess. 2012;29(8):1183–93.

    Article  CAS  PubMed  Google Scholar 

  3. Peters R, Kramer E, Oomen AG, Herrera Rivera ZE, Oegema G, Tromp PC, et al. Presence of nano-sized silica during in vitro digestion of foods containing silica as a food additive. ACS Nano. 2012;6(3):2441–51.

    Article  CAS  PubMed  Google Scholar 

  4. EC recommendation on the definition of NM (2011/696/EU), Off J Eur Union, L275/38.

  5. Peters R, Brandhoff P, Weigel S, Marvin H, Bouwmeester H, Aschberger K, et al. Inventory of nanotechnology applications in the agricultural, feed and food sector. EFSA supporting publication. 2014:EN-621, 125 pp.

  6. Barahona F, Ojea-Jimenez I, Geiss O, Gilliland D, Barrero-Moreno J. Multimethod approach for the detection and characterisation of food-grade synthetic amorphous silica nanoparticles. J Chromatogr A. 2016;1432:92–100.

    Article  CAS  PubMed  Google Scholar 

  7. Regulation (EC) No 1333/2008 of the European Parliament and of the Council on Food Additives. Off J Eur Union. 2008;L 354/16.

  8. Regulation (EU) No 1169/2011 of the European Parliament and of the Council on the Provision of Food Information to Consumers. Off J Eur Union. 2011;L 304/18.

  9. EFSA ANS Panel (EFSA Panel on Food Additives and Nutrient Sources added to Food). Scientific opinion on the re-evaluation of silicon dioxide (E 551) as a food additive. EFSA J. 2018;16(1):5088.

    Google Scholar 

  10. Contado C, Ravani L, Passarella M. Size characterization by sedimentation field flow fractionation of silica particles used as food additives. Anal Chim Acta. 2013;788:183–92.

    Article  CAS  PubMed  Google Scholar 

  11. Grombe R, Charoud-Got J, Emteborg H, Linsinger TP, Seghers J, Wagner S, et al. Production of reference materials for the detection and size determination of silica nanoparticles in tomato soup. Anal Bioanal Chem. 2014;406(16):3895–907.

    CAS  PubMed  Google Scholar 

  12. Lim JH, Sisco P, Mudalige TK, Sánchez-Pomales G, Howard PC, Linder SW. Detection and characterization of SiO2 and TiO2 nanostructures in dietary supplements. J Agric Food Chem. 2015;63(12):3144–52.

    Article  CAS  PubMed  Google Scholar 

  13. Wagner S, Legros S, Loeschner K, Liu J, Navratilova J, Grombe R, et al. First steps towards a generic sample preparation scheme for inorganic engineered nanoparticles in a complex matrix for detection, characterization, and quantification by asymmetric flow-field flow fractionation coupled to multi-angle light scattering and ICP-MS. J Anal At Spectrom. 2015;30:1286–96.

    Article  CAS  Google Scholar 

  14. Contado C, Mejia J, Lozano García O, Piret JP, Dumortier E, Toussaint O, et al. Physicochemical and toxicological evaluation of silica nanoparticles suitable for food and consumer products collected by following the EC recommendation. Anal Bioanal Chem. 2016;408(1):271–86.

    Article  CAS  PubMed  Google Scholar 

  15. de la Calle I, Menta M, Klein M, Séby F. Study of the presence of micro- and nanoparticles in drinks and foods by multiple analytical techniques. Food Chem. 2018;266:133–45.

    Article  PubMed  Google Scholar 

  16. Geiss O, Bianchi I, Senaldi C, Barrero J. Challenges in isolating silica particles from organic food matrices with microwave-assisted acidic digestion. Anal Bioanal Chem. 2019;411(22):5817–31.

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  17. Dekkers S, Krystek P, Peters RJB, Lankveld DPK, Bokkers BGH, van Hoeven-Arentzen PH, et al. Presence and risks of nanosilica in food products. Nanotoxicology. 2011;5(3):393–405.

    Article  CAS  PubMed  Google Scholar 

  18. Heroult J, Nischwitz V, Bartczak D, Goenaga-Infante H. The potential of asymmetric flow field-flow fractionation hyphenated to multiple detectors for the quantification and size estimation of silica nanoparticles in a food matrix. Anal Bioanal Chem. 2014;406(16):3919–27.

    Article  CAS  PubMed  Google Scholar 

  19. von der Kammer F, Legros S, Larsen EH, Loeschner K, Hofmann T. Separation and characterization of nanoparticles in complex food and environmental samples by field-flow fractionation. TrAC Trends Anal Chem. 2011;30(3):425–36.

    Article  Google Scholar 

  20. Montaño MD, Majestic BJ, Jämting ÅK, Westerhoff P, Ranville JF. Methods for the detection and characterization of silica colloids by microsecond spICP-MS. Anal Chem. 2016;88(9):4733–41.

    Article  PubMed  Google Scholar 

  21. Li T, Senesi AJ, Lee B. Small angle X-ray scattering for nanoparticle research. Chem Rev. 2016;116(18):11128–80.

    Article  CAS  PubMed  Google Scholar 

  22. Pabisch S, Feichtenschlager B, Kickelbick G, Peterlik H. Effect of interparticle interactions on size determination of zirconia and silica based systems – a comparison of SAXS, DLS, BET, XRD and TEM. Chem Phys Lett. 2012;521:91–7.

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  23. Aureli F, D’Amato M, Raggi A, Cubadd F. Quantitative characterization of silica nanoparticles by asymmetric flow field flow fractionation coupled with online multiangle light scattering and ICP-MS/MS detection. J Anal At Spectrom. 2015;30:1266–73.

    Article  CAS  Google Scholar 

  24. Barahona F, Geiss O, Urbán P, Ojea-Jimenez I, Gilliland D, Barrero-Moreno J. Simultaneous determination of size and quantification of silica nanoparticles by asymmetric flow field-flow fractionation coupled to ICPMS using silica nanoparticles standards. Anal Chem. 2015;87(5):3039–47.

    Article  CAS  PubMed  Google Scholar 

  25. Raghavan SR, Walls HJ, Khan SA. Rheology of silica dispersions in organic liquids: new evidence for solvation forces dictated by hydrogen bonding. Langmuir. 2000;16(21):7920–30.

    Article  CAS  Google Scholar 

  26. Geiss O, Cascio C, Gilliland D, Franchini F, Barrero-Moreno J. Size and mass determination of silver nanoparticles in an aqueous matrix using asymmetric flow field flow fractionation coupled to inductively coupled plasma mass spectrometer and ultraviolet–visible detectors. J Chromatogr A. 2013;1321:100–8.

    Article  CAS  PubMed  Google Scholar 

  27. Makan AC, Spallek MJ, du Toit M, Klein T, Pasch H. Advanced analysis of polymer emulsions: particle size and particle size distribution by field-flow fractionation and dynamic light scattering. J Chromatogr A. 2016;1442:94–106.

    Article  CAS  PubMed  Google Scholar 

  28. Sánchez-García L, Bolea E, Laborda F, Cubel C, Ferrer P, Gianolio D, et al. Size determination and quantification of engineered cerium oxide nanoparticles by flow field-flow fractionation coupled to inductively coupled plasma mass spectrometry. J Chromatogr A. 2016;1438:205–15.

    Article  PubMed  Google Scholar 

  29. Prestel H, Schott L, Niessner R, Panne U. Characterization of sewage plant hydrocolloids using asymmetrical flow field-flow fractionation and ICP-mass spectrometry. Water Res. 2005;39(15):3541–52.

    Article  CAS  PubMed  Google Scholar 

  30. Petersen E, Montoro Bustos A, Toman B, Johnson M, Ellefson M, Caceres G, et al. Determining what really counts: modelling and measuring nanoparticle number concentrations. Environ Sci Nano. 2019;6:2876–96.

  31. Athinarayanan J, Periasamy VS, Alsaif MA, Al-Warthan AA, Alshatwi AA. Presence of nanosilica (E551) in commercial food products: TNF-mediated oxidative stress and altered cell cycle progression in human lung fibroblast cells. Cell Biol Toxicol. 2014;30(2):89–100.

    Article  CAS  PubMed  Google Scholar 

  32. Athinarayanan J, Alshatwi AA, Periasamy VS, Al-Warthan AA. Identification of nanoscale ingredients in commercial food products and their induction of mitochondrially mediated cytotoxic effects on human mesenchymal stem cells. J Food Sci. 2015;80(2):N459–64.

    Article  CAS  PubMed  Google Scholar 

  33. Yang Y, Faust JJ, Schoepf J, Hristovski K, Capco DG, Herckes P, et al. Survey of food-grade silica dioxide nanomaterial occurrence, characterization, human gut impacts and fate across its lifecycle. Sci Total Environ. 2016;565:902–12.

    Article  CAS  PubMed  Google Scholar 

Download references

Acknowledgments

The authors are very grateful to Dr. Xu Li and Dr. Suxi Wang from the Institute of Materials Research and Engineering (IMRE) in Singapore for their technical assistance with TEM data acquisition.

Funding

This research was supported by the Reinvestment Fund (RF), Ministry of Finance (MOF), Singapore.

Author information

Authors and Affiliations

  1. National Centre for Food Science, Singapore Food Agency, 10 Perahu Road, Singapore, 718837, Singapore

    Bin Li, Sew Lay Chua, Dingyi Yu, Shoo Peng Koh, Helen Phang & Paul K. T. Chiew

  2. Veterinary Public Health Laboratory, Agri-Food and Veterinary Authority of Singapor, 10 Perahu Road, Singapore, 718837, Singapore

    Ai Lee Ch’ng

Authors
  1. Bin Li
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Sew Lay Chua
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Ai Lee Ch’ng
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Dingyi Yu
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Shoo Peng Koh
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Helen Phang
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Paul K. T. Chiew
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Shoo Peng Koh.

Ethics declarations

Conflict of interest

The authors declare that they have no conflict of interest.

Additional information

Publisher’s note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

The study was conducted under the Management of the Veterinary Public Health Laboratory, Agri-Food and Veterinary Authority of Singapore before it was subsumed under the National Centre for Food Science, Singapore Food Agency with effectivity from 1 April 2019.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Li, B., Chua, S.L., Ch’ng, A.L. et al. An effective approach for size characterization and mass quantification of silica nanoparticles in coffee creamer by AF4-ICP-MS. Anal Bioanal Chem 412, 5499–5512 (2020). https://doi.org/10.1007/s00216-020-02770-x

Download citation

  • Received:

  • Revised:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s00216-020-02770-x

Keywords

Search

Navigation