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Development of methodology to generate, measure, and characterize the chemical composition of oxidized mercury nanoparticles

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Abstract

The phase of oxidized mercury is critical in the fate, transformation, and bioavailability of mercury species in Earth’s ecosystem. There is now evidence that what is measured as gaseous oxidized mercury (GOM) is not only gaseous but also consists of airborne nanoparticles with distinct physicochemical properties. Herein, we present the development of the first method for the consistent and reproducible generation of oxidized mercury nano- and sub-micron particles (~ 5 to 400 nm). Oxidized mercury nanoparticles are generated using two methods, vapor-phase condensation and aqueous nebulization, for three proxies: mercury(II) bromide (HgBr2), mercury(II) chloride (HgCl2), and mercury(II) oxide (HgO). These aerosols are characterized using scanning mobility and optical sizing, high-resolution scanning transmission electron microscopy (STEM), and nano/microparticle interface coupled to soft ionization mercury mass spectrometric techniques. Synthetic nanoparticle stability was studied in aqueous media, and using a microcosm at ambient tropospheric conditions of ~ 740 Torr pressure, room temperature, and at relative humidity of approximately 20%. Analysis of microcosm airborne nanoparticles confirmed that generated synthetic mercury nanoparticles retain their physical properties once in air. KCl-coated denuders, which are currently used globally to measure gaseous mercury compounds, were exposed to generated oxidized mercury nanoparticles. The degree of synthetic mercury nanoparticle capture by KCl-coated denuders and particulate filters was assessed. A significant portion of nanoparticulate and sub-micron particulate mercury was trapped on the KCl-coated denuder and measured as GOM. Finally, we demonstrate the applicability of soft ionization mercury mass spectrometry to the measurement of mercury species present in the gaseous and solid phase. We recommend coupling of this technique with existing methodology for a more accurate representation of mercury biogeochemistry cycling.

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  • 16 January 2020

    The authors would like to call the reader’s attention to the fact that, unfortunately, there was an unintentional oversight regarding the funding information in this manuscript; please find the correct information below.

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Acknowledgments

The authors thank Dr. Hojatollah Vali and David Liu of the Facility for Electron Microscopy Research and also acknowledge Dr. Janusz Rak and Laura Montermini at the Montreal Children’s Hospital for the use of the Nanosight NS500.

Funding information

This study received financial support from the Natural Sciences and Engineering Research Council of Canada (NSERC), the Canadian Foundation for Innovation (CFI), Le Fonds de recherche du Québec – Nature et technologies (FRQNT), Environment and Climate Change Canada, McGill University, and the Walter C. Sumner Foundation.

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Correspondence to Parisa A. Ariya.

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Ghoshdastidar, A.J., Ramamurthy, J., Morissette, M. et al. Development of methodology to generate, measure, and characterize the chemical composition of oxidized mercury nanoparticles. Anal Bioanal Chem (2019) doi:10.1007/s00216-019-02279-y

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Keywords

  • Gaseous oxidized mercury (GOM)
  • KCl-coated denuders
  • Particulate-bound mercury (PBM)
  • Mercury mass spectrometry