Abstract
A simple, universal method to quantify soil methylmercury (MeHg) is not available. Here, we developed a solid-phase extraction-based method using gas chromatography mass spectrometry. MeHg was purified from the soil matrix using an optimized solid-phase extraction method, which reduced the use of organic solvents and eliminated the requirement for harmful reagents. The sample limit of quantification was 7.5 ng/g. MeHg recovery in the reference samples was 96.2%–102.6%; the intra- and inter-assay coefficients of variation were 3.4%–7.1% and 4.3%–7.1%, respectively, indicating high validation performance. This analysis method is simple as it can be performed using general-purpose reagents and instruments; has a high degree of trueness and accuracy; could be useful for soil MeHg quantification with improved sensitivity; and can provide reliable data to prevent MeHg contamination and improve food safety.
Similar content being viewed by others
Data Availability
Not applicable.
Code Availability
Not applicable.
References
Amendola G, Pelosi P, Dommarco R (2010) Solid-phase extraction for multi-residue analysis of pesticides in honey. J Environ Sci Health B 46:24–34. https://doi.org/10.1080/03601234.2010.515170
Du H, Guo P, Wang T, Ma M, Wang D (2021) Significant bioaccumulation and biotransformation of methyl mercury by organisms in rice paddy ecosystems: a potential health risk to humans. Environ Pollut 273:116431. https://doi.org/10.1016/j.envpol.2021.116431
Kodamatani H, Maeda C, Balogh SJ, Nollet YH, Kanzaki R, Tomiyasu T (2017) The influence of sample drying and storage conditions on methylmercury determination in soils and sediments. Chemosphere 173:380–386. https://doi.org/10.1016/j.chemosphere.2017.01.053
Kodamatani H, Daiba Y, Morisaki S, Ichitani K, Kanzaki R, Tomiyasu T (2020) Detailed investigation of methylmercury accumulation in rice grain from Hg2+-spiked non-contaminated paddy field soils. Chemosphere 247:125827. https://doi.org/10.1016/j.chemosphere.2020.125827
Liem-Nguyen V, Nguyen-Ngoc H-T, Adediran GA, Björn E (2020) Determination of picomolar levels of methylmercury complexes with low molecular mass thiols by liquid chromatography tandem mass spectrometry and online preconcentration. Anal Bioanal Chem 412:1619–1628. https://doi.org/10.1007/s00216-020-02389-y
Lin J, Sun D, Zhang Z, Duan Z, Dong J (2021) Heavy metals and health risk of rice sampled in Yangtze River Delta, China. Food Addit Contam B 14:133–140. https://doi.org/10.1080/19393210.2021.1903568
Łozowicka B, Rutkowska E, Jankowska M (2017) Influence of QuEChERS modifications on recovery and matrix effect during the multi-residue pesticide analysis in soil by GC/MS/MS and GC/ECD/NPD. Environ Sci Pollut Int 24:7124–7138. https://doi.org/10.1007/s11356-016-8334-1
Mishra S, Tripathi RM, Bhalke S, Shukla VK, Puranik VD (2005) Determination of methylmercury and mercury(II) in a marine ecosystem using solid-phase microextraction gas chromatography-mass spectrometry. Anal Chim Acta 551:192–198. https://doi.org/10.1016/j.aca.2005.07.026
Morita H, Sakurai H, Shimomura S (1982) Combined use of potassium iodide and L-ascorbic acid in solvent extraction and determination of methylmercuric compounds (in Japanese). Bunseki Kagaku 31:314–317
Rothenberg SE, Windham-Myers L, Creswell JE (2014) Rice methylmercury exposure and mitigation: a comprehensive review. Environ Res 133:407–423. https://doi.org/10.1016/j.envres.2014.03.001
Schenck FJ, Brown AN, Podhorniak LV, Parker A, Reliford M, Wong JW (2008) A rapid multiresidue method for determination of pesticides in fruits and vegetables by using acetonitrile extraction/partitioning and solid-phase extraction column cleanup. J AOAC Int 91:422–438. https://doi.org/10.1093/jaoac/91.2.422
Sunderland EM, Krabbenhoft DP, Moreau JW, Strode SA, Landing WM (2009) Mercury sources, distribution, and bioavailability in the North Pacific Ocean: insights from data and models. Glob Biogeochem Cycles. https://doi.org/10.1029/2008GB003425
The Ministry of Health, Labour and Welfare of Japan (2012) Guidelines for the validation of analytical methods for testing metals in food. Notification No. 0926001 (in Japanese). http://www.nihs.go.jp/food/_src/1634/metal_qagl.pdf?v=1599555029849. Accessed 10 June 2021
The Ministry of the Environment, Japan (2004) Mercury analysis manual 2004. http://nimd.env.go.jp/kenkyu/docs/march_mercury_analysis_manual(e).pdf. Accessed 8 June 2021
The Ministry of the Environment, Japan (2014) Development of simple, rapid, and sensitive determination method for measurement of methylmercury in mercury contaminated soil/sediment. https://www.env.go.jp/policy/kenkyu/suishin/kadai/syuryo_report/h26/pdf/5RF-1303.pdf. Accessed 10 June 2021
United Nations Environment Programme, UNEP (2013) Global mercury assessment 2013 sources, emissions, releases and environmental transport. https://wedocs.unep.org/handle/20.500.11822/7984. Accessed 10 June 2021
US Environmental Protection Agency, USEPA (2014) Method 3200. Mercury species fractionation and quantification by microwave assisted extraction, selective solvent extraction and/or solid phase extraction. https://www.epa.gov/sites/production/files/2015-12/documents/3200.pdf. Accessed 13 Sep 2021
Acknowledgements
The authors would like to thank Dr. Toshiaki Yoshida (Osaka Institute of Public Health), Dr. Tetsuo Yamano (Osaka Institute of Public Health), and Dr. Shuntaro Yamazaki (Waters Corporation) for providing valuable advice and technical support.
Funding
This work was supported by the Japan Society for the Promotion of Science KAKENHI (Grant No. 19K10592).
Author information
Authors and Affiliations
Contributions
Conceptualization: SK, MY; Resources: SK; Methodology: SK, MY; Formal analysis: SK; Validation: SK, MY, KK; Investigation: SK; Writing–original draft: SK; Writing–review and editing: MY, KK; Funding acquisition: SK.
Corresponding author
Ethics declarations
Conflict of interest
The authors have no relevant financial or non-financial interests to disclose.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
About this article
Cite this article
Kakimoto, S., Yoshimitsu, M. & Kiyota, K. Development of a Solid Phase Extraction-Based Method for the Quantitative Analysis of Methylmercury in Soil and Sediment. Bull Environ Contam Toxicol 109, 332–337 (2022). https://doi.org/10.1007/s00128-022-03547-x
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s00128-022-03547-x