Simultaneous sub-picogram speciation of methylmercury and ethylmercury in caustic nuclear tank waste using direct aqueous propylation
Abstract
Organomercury species are present at regulatory levels in the tanks at the Savannah River Site. Calibration of methylmercury and ethylmercury ranged three orders of magnitude, generating detection limits of 0.033 pg and 7.50 pg, respectively. Calibration verifications maintained 101 and 103% accuracy, respectively, with mean recovery from waste samples of 104%. Here, dilution volume was optimized to eliminate sample distillation, decreasing method runtime by 337% and reducing total instrumentation footprint by 60.4% compared with current standard methods. Finally, compared with standard methods, this work represents a significant improvement in safety, efficiency, and reproducibility of organomercury speciation, particularly for industrial and nuclear analysis.
- Authors:
-
[1];
- Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL). Analytical Development, Science and Technology
- Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL). Wasteform Processing Technology. Environmental Stewardship
- Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL). Chemical Processing Technologies. Environmental Stewardship
- Publication Date:
- Research Org.:
- Savannah River National Laboratory (SRNL), Aiken, SC (United States)
- Sponsoring Org.:
- USDOE Office of Environmental Management (EM)
- OSTI Identifier:
- 1476268
- Alternate Identifier(s):
- OSTI ID: 1501350
- Report Number(s):
- SRNL-L4130-2017-00007
Journal ID: ISSN 0236-5731; PII: 6085
- Grant/Contract Number:
- AC09-08SR22470; DE-AC09-08SR22470
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Radioanalytical and Nuclear Chemistry
- Additional Journal Information:
- Journal Volume: 318; Journal Issue: 1; Journal ID: ISSN 0236-5731
- Publisher:
- Springer
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; atomic fluorescence; propylation; organomercury; purge and trap; nuclear waste
Citation Formats
Boggess, Andrew J., White, Thomas L., Jones, Mark A., Bannochie, Christopher J., Ekechukwu, Amy A., and Wilmarth, William R. Simultaneous sub-picogram speciation of methylmercury and ethylmercury in caustic nuclear tank waste using direct aqueous propylation. United States: N. p., 2018.
Web. doi:10.1007/s10967-018-6085-9.
Boggess, Andrew J., White, Thomas L., Jones, Mark A., Bannochie, Christopher J., Ekechukwu, Amy A., & Wilmarth, William R. Simultaneous sub-picogram speciation of methylmercury and ethylmercury in caustic nuclear tank waste using direct aqueous propylation. United States. https://doi.org/10.1007/s10967-018-6085-9
Boggess, Andrew J., White, Thomas L., Jones, Mark A., Bannochie, Christopher J., Ekechukwu, Amy A., and Wilmarth, William R. Tue .
"Simultaneous sub-picogram speciation of methylmercury and ethylmercury in caustic nuclear tank waste using direct aqueous propylation". United States. https://doi.org/10.1007/s10967-018-6085-9. https://www.osti.gov/servlets/purl/1476268.
@article{osti_1476268,
title = {Simultaneous sub-picogram speciation of methylmercury and ethylmercury in caustic nuclear tank waste using direct aqueous propylation},
author = {Boggess, Andrew J. and White, Thomas L. and Jones, Mark A. and Bannochie, Christopher J. and Ekechukwu, Amy A. and Wilmarth, William R.},
abstractNote = {Organomercury species are present at regulatory levels in the tanks at the Savannah River Site. Calibration of methylmercury and ethylmercury ranged three orders of magnitude, generating detection limits of 0.033 pg and 7.50 pg, respectively. Calibration verifications maintained 101 and 103% accuracy, respectively, with mean recovery from waste samples of 104%. Here, dilution volume was optimized to eliminate sample distillation, decreasing method runtime by 337% and reducing total instrumentation footprint by 60.4% compared with current standard methods. Finally, compared with standard methods, this work represents a significant improvement in safety, efficiency, and reproducibility of organomercury speciation, particularly for industrial and nuclear analysis.},
doi = {10.1007/s10967-018-6085-9},
journal = {Journal of Radioanalytical and Nuclear Chemistry},
number = 1,
volume = 318,
place = {United States},
year = {Tue Aug 14 00:00:00 EDT 2018},
month = {Tue Aug 14 00:00:00 EDT 2018}
}
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Works referenced in this record:
Simultaneous Speciation of Monomethylmercury and Monoethylmercury by Aqueous Phenylation and Purge-and-Trap Preconcentration Followed by Atomic Spectrometry Detection
journal, September 2008
- Mao, Yuxiang; Liu, Guangliang; Meichel, George
- Analytical Chemistry, Vol. 80, Issue 18
Long-Term Stability of Inorganic, Methyl and Ethyl Mercury in Whole Blood: Effects of Storage Temperature and Time
journal, February 2016
- Sommer, Yuliya L.; Ward, Cynthia D.; Pan, Yi
- Journal of Analytical Toxicology, Vol. 40, Issue 3
Mercury in aqueous tank waste at the Savannah River Site: Facts, forms, and impacts
journal, March 2017
- Bannochie, C. J.; Fellinger, T. L.; Garcia-Strickland, P.
- Separation Science and Technology, Vol. 53, Issue 12
Determination of artifactual formation of monomethylmercury (CH 3 Hg + ) in environmental samples using stable Hg 2+ isotopes with ICP-MS detection: Calculation of contents applying species specific isotope addition
journal, June 1997
- Hintelmann, H.; Falter, R.; Ilgen, G.
- Fresenius' Journal of Analytical Chemistry, Vol. 358, Issue 3
Bonding of methyl mercury to reduced sulfur groups in soil and stream organic matter as determined by x-ray absorption spectroscopy and binding affinity studies
journal, November 2002
- Qian, Jin; Skyllberg, Ulf; Frech, Wolfgang
- Geochimica et Cosmochimica Acta, Vol. 66, Issue 22
Mercury speciation in seafood samples by LC–ICP-MS with a rapid ultrasound-assisted extraction procedure: Application to the determination of mercury in Brazilian seafood samples
journal, June 2011
- Batista, Bruno Lemos; Rodrigues, Jairo L.; de Souza, Samuel S.
- Food Chemistry, Vol. 126, Issue 4
Inorganic and methylmercury speciation in environmental samples
journal, November 1998
- Sánchez Uría, J.
- Talanta, Vol. 47, Issue 3
Comparison of different derivatization approaches for mercury speciation in biological tissues by gas chromatography/inductively coupled plasma mass spectrometry
journal, May 2000
- Garc�a Fern�ndez, Rub�n; Montes Bay�n, Mar�a; Garc�a Alonso, J. Ignacio
- Journal of Mass Spectrometry, Vol. 35, Issue 5
Comparison of Modifiers for Mercury Speciation in Water by Solid Phase Extraction and High Performance Liquid Chromatography–Atomic Fluorescence Spectrometry
journal, August 2014
- Xiong, Xiong; Qi, Xiaoting; Liu, Jiantong
- Analytical Letters, Vol. 47, Issue 14
Global mercury emissions to the atmosphere from anthropogenic and natural sources
journal, January 2010
- Pirrone, N.; Cinnirella, S.; Feng, X.
- Atmospheric Chemistry and Physics, Vol. 10, Issue 13
Preservation and storage techniques for low-level aqueous mercury speciation
journal, January 2005
- Parker, Jennifer L.; Bloom, Nicolas S.
- Science of The Total Environment, Vol. 337, Issue 1-3
Comparison of distillation with other current isolation methods for the determination of methyl mercury compounds in low level environmental samples
journal, September 1993
- Horvat, Milena; Bloom, Nicolas S.; Liang, Lian
- Analytica Chimica Acta, Vol. 281, Issue 1
Development of a new HPLC method for the determination of inorganic and methylmercury in biological samples with ICP-MS detection
journal, January 2007
- Vallant, Birgit; Kadnar, Rainer; Goessler, Walter
- Journal of Analytical Atomic Spectrometry, Vol. 22, Issue 3
A simple method for methylmercury, inorganic mercury and ethylmercury determination in plasma samples by high performance liquid chromatography–cold-vapor-inductively coupled plasma mass spectrometry
journal, January 2013
- de Souza, Samuel S.; Campiglia, Andres Dobal; Barbosa, Fernando
- Analytica Chimica Acta, Vol. 761
Trace-level automated mercury speciation analysis
journal, January 2011
- Taylor, Vivien F.; Carter, Annie; Davies, Colin
- Analytical Methods, Vol. 3, Issue 5
An inter-laboratory comparison of different analytical methods for the determination of monomethylmercury in various soil and sediment samples: A platform for method improvement
journal, February 2017
- Kodamatani, Hitoshi; Balogh, Steven J.; Nollet, Yabing H.
- Chemosphere, Vol. 169
Derivatization by ethylation with sodium tetraethylborate for the speciation of metals and organometallics in environmental samples. A review
journal, January 1994
- Rapsomanikis, Spyridon
- The Analyst, Vol. 119, Issue 7
Online anion exchange column preconcentration and high performance liquid chromatographic separation with inductively coupled plasma mass spectrometry detection for mercury speciation analysis
journal, May 2014
- Cheng, Heyong; Wu, Chunling; Shen, Lihuan
- Analytica Chimica Acta, Vol. 828
Demonstration Of The Caustic-side Solvent Extraction Process For The Removal Of 137 Cs From Savannah River Site High Level Waste
journal, January 2003
- Norato, M. A.; Beasley, M. H.; Campbell, S. G.
- Separation Science and Technology, Vol. 38, Issue 12-13
Changes in methylmercury concentration during storage: effect of temperature
journal, May 2001
- Devai, Istvan; Delaune, Ronald D.; Patrick Jr, William H.
- Organic Geochemistry, Vol. 32, Issue 5
The Minamata Convention on Mercury: Attempting to address the global controversy of dental amalgam use and mercury waste disposal
journal, February 2014
- Mackey, Tim K.; Contreras, John T.; Liang, Bryan A.
- Science of The Total Environment, Vol. 472
Determination of Picogram Levels of Methylmercury by Aqueous Phase Ethylation, Followed by Cryogenic Gas Chromatography with Cold Vapour Atomic Fluorescence Detection
journal, July 1989
- Bloom, Nicolas
- Canadian Journal of Fisheries and Aquatic Sciences, Vol. 46, Issue 7
Minamata Disease: Methylmercury Poisoning in Japan Caused by Environmental Pollution
journal, January 1995
- Harada, Masazumi
- Critical Reviews in Toxicology, Vol. 25, Issue 1
Assessing bias in total mercury results after removing a subsample from the bottle
journal, August 2016
- Creswell, Joel E.; Carter, Annie; Chen, Bin
- International Journal of Environmental Analytical Chemistry, Vol. 96, Issue 11
Validation of Methylmercury Determinations in Aquatic Systems by Alkyl Derivatization Methods for GC Analysis Using ICP-IDMS
journal, July 2001
- Demuth, Natascha; Heumann, Klaus G.
- Analytical Chemistry, Vol. 73, Issue 16
Methylmercury in water samples at the pg/L level by online preconcentration liquid chromatography cold vapor-atomic fluorescence spectrometry
journal, March 2015
- Brombach, Christoph-Cornelius; Chen, Bin; Corns, Warren T.
- Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 105
Tc-99 and Cs-137 Volatility from the DWPF Production Melter During Vitrification of the First Macrobatch of HLW Sludge at the Savannah River Site
journal, January 1999
- Bibler, N. E.; Fellinger, T. L.; Marra, S. L.
- MRS Proceedings, Vol. 608
Global mercury emissions to the atmosphere from anthropogenic and natural sources
journal, January 2010
- Pirrone, N.; Cinnirella, S.; Feng, X.
- Atmospheric Chemistry and Physics Discussions, Vol. 10, Issue 2