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Title: Recent advances in the detection of specific natural organic compounds as carriers for radionuclides in soil and water environments, with examples of radioiodine and plutonium

Among the key environmental factors influencing the fate and transport of radionuclides in the environment is natural organic matter (NOM). While this has been known for decades, there still remains great uncertainty in predicting NOM-radionuclide interactions because of lack of understanding of radionuclide interactions with the specific organic moieties within NOM. Furthermore, radionuclide-NOM studies conducted using modelled organic compounds or elevated radionuclide concentrations provide compromised information related to true environmental conditions. Thus, sensitive techniques are required not only for the detection of radionuclides, and their different species, at ambient and/or far-field concentrations, but also for potential trace organic compounds that are chemically binding these radionuclides. GC-MS and AMS techniques developed in our lab are reviewed in this paper that aim to assess how two radionuclides, iodine and plutonium, form strong bonds with NOM by entirely different mechanisms; iodine tends to bind to aromatic functionalities, whereas plutonium binds to N-containing hydroxamate siderophores at ambient concentrations. While low-level measurements are a prerequisite for assessing iodine and plutonium migration at nuclear waste sites and as environmental tracers, it is necessary to determine their in-situ speciation, which ultimately controls their mobility and transport in natural environments. Finally and more importantly, advanced molecular-level instrumentation (e.g.,more » nuclear magnetic resonance (NMR) and Fourier-transform ion cyclotron resonance coupled with electrospray ionization (ESI-FTICRMS) were applied to resolve either directly or indirectly the molecular environments in which the radionuclides are associated with the NOM.« less
Authors:
ORCiD logo [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [2] ;  [3]
  1. Texas A & M Univ., Galveston, TX (United States)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  3. Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
Publication Date:
Report Number(s):
LA-UR-17-21389
Journal ID: ISSN 0265-931X
Grant/Contract Number:
AC52-06NA25396; AC09-08SR22470; SC0014152; ER64567- 1031562-0014364
Type:
Accepted Manuscript
Journal Name:
Journal of Environmental Radioactivity
Additional Journal Information:
Journal Volume: 171; Journal ID: ISSN 0265-931X
Publisher:
Elsevier
Research Org:
Texas A & M Univ., Galveston, TX (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Savannah River Site (SRS), Aiken, SC (United States)
Sponsoring Org:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Iodine; Plutonium; Speciation; Natural organic matter moieties; Aromatic acids; Hydroxamates
OSTI Identifier:
1369198
Alternate Identifier(s):
OSTI ID: 1414317

Santschi, P. H., Xu, C., Zhang, S., Schwehr, K. A., Lin, P., Yeager, C. M., and Kaplan, D. I.. Recent advances in the detection of specific natural organic compounds as carriers for radionuclides in soil and water environments, with examples of radioiodine and plutonium. United States: N. p., Web. doi:10.1016/j.jenvrad.2017.02.023.
Santschi, P. H., Xu, C., Zhang, S., Schwehr, K. A., Lin, P., Yeager, C. M., & Kaplan, D. I.. Recent advances in the detection of specific natural organic compounds as carriers for radionuclides in soil and water environments, with examples of radioiodine and plutonium. United States. doi:10.1016/j.jenvrad.2017.02.023.
Santschi, P. H., Xu, C., Zhang, S., Schwehr, K. A., Lin, P., Yeager, C. M., and Kaplan, D. I.. 2017. "Recent advances in the detection of specific natural organic compounds as carriers for radionuclides in soil and water environments, with examples of radioiodine and plutonium". United States. doi:10.1016/j.jenvrad.2017.02.023. https://www.osti.gov/servlets/purl/1369198.
@article{osti_1369198,
title = {Recent advances in the detection of specific natural organic compounds as carriers for radionuclides in soil and water environments, with examples of radioiodine and plutonium},
author = {Santschi, P. H. and Xu, C. and Zhang, S. and Schwehr, K. A. and Lin, P. and Yeager, C. M. and Kaplan, D. I.},
abstractNote = {Among the key environmental factors influencing the fate and transport of radionuclides in the environment is natural organic matter (NOM). While this has been known for decades, there still remains great uncertainty in predicting NOM-radionuclide interactions because of lack of understanding of radionuclide interactions with the specific organic moieties within NOM. Furthermore, radionuclide-NOM studies conducted using modelled organic compounds or elevated radionuclide concentrations provide compromised information related to true environmental conditions. Thus, sensitive techniques are required not only for the detection of radionuclides, and their different species, at ambient and/or far-field concentrations, but also for potential trace organic compounds that are chemically binding these radionuclides. GC-MS and AMS techniques developed in our lab are reviewed in this paper that aim to assess how two radionuclides, iodine and plutonium, form strong bonds with NOM by entirely different mechanisms; iodine tends to bind to aromatic functionalities, whereas plutonium binds to N-containing hydroxamate siderophores at ambient concentrations. While low-level measurements are a prerequisite for assessing iodine and plutonium migration at nuclear waste sites and as environmental tracers, it is necessary to determine their in-situ speciation, which ultimately controls their mobility and transport in natural environments. Finally and more importantly, advanced molecular-level instrumentation (e.g., nuclear magnetic resonance (NMR) and Fourier-transform ion cyclotron resonance coupled with electrospray ionization (ESI-FTICRMS) were applied to resolve either directly or indirectly the molecular environments in which the radionuclides are associated with the NOM.},
doi = {10.1016/j.jenvrad.2017.02.023},
journal = {Journal of Environmental Radioactivity},
number = ,
volume = 171,
place = {United States},
year = {2017},
month = {3}
}