skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: 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:
ORCiD logo [1];  [1];  [1];  [2];  [1];  [3]
  1. Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL). Analytical Development, Science and Technology
  2. Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL). Wasteform Processing Technology. Environmental Stewardship
  3. Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL). Chemical Processing Technologies. Environmental Stewardship
Publication Date:
Research Org.:
Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
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:
Journal Article: 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. doi: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. doi: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},
issn = {0236-5731},
number = 1,
volume = 318,
place = {United States},
year = {2018},
month = {8}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Save / Share:

Works referenced in this record:

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
  • DOI: 10.1093/jat/bkw007

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
  • DOI: 10.1080/01496395.2017.1310239

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


Inorganic and methylmercury speciation in environmental samples
journal, November 1998


Comparison of different derivatization approaches for mercury speciation in biological tissues by gas chromatography/inductively coupled plasma mass spectrometry
journal, May 2000


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
  • DOI: 10.5194/acp-10-5951-2010

Preservation and storage techniques for low-level aqueous mercury speciation
journal, January 2005


Comparison of distillation with other current isolation methods for the determination of methyl mercury compounds in low level environmental samples
journal, September 1993


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
  • DOI: 10.1039/b615463h

Trace-level automated mercury speciation analysis
journal, January 2011

  • Taylor, Vivien F.; Carter, Annie; Davies, Colin
  • Analytical Methods, Vol. 3, Issue 5
  • DOI: 10.1039/c0ay00528b

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
  • DOI: 10.1081/SS-120022565

Changes in methylmercury concentration during storage: effect of temperature
journal, May 2001


The Minamata Convention on Mercury: Attempting to address the global controversy of dental amalgam use and mercury waste disposal
journal, February 2014


Minamata Disease: Methylmercury Poisoning in Japan Caused by Environmental Pollution
journal, January 1995


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
  • DOI: 10.1080/03067319.2016.1221405

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
  • DOI: 10.1016/j.sab.2014.09.014