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.
abstract: 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 here 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. 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.
authors.affiliation: Texas A&M-Galveston, Galveston, TX, USA. Electronic address: santschi@tamug.edu.
authors.forename: P H
authors.initials: PH
authors.lastname: Santschi
authors.affiliation: Texas A&M-Galveston, Galveston, TX, USA.
authors.forename: C
authors.initials: C
authors.lastname: Xu
authors.affiliation: Texas A&M-Galveston, Galveston, TX, USA.
authors.forename: S
authors.initials: S
authors.lastname: Zhang
authors.affiliation: Texas A&M-Galveston, Galveston, TX, USA.
authors.forename: K A
authors.initials: KA
authors.lastname: Schwehr
authors.affiliation: Texas A&M-Galveston, Galveston, TX, USA.
authors.forename: P
authors.initials: P
authors.lastname: Lin
authors.affiliation: Los Alamos National Laboratory, Los Alamos, NM, USA.
authors.forename: C M
authors.initials: CM
authors.lastname: Yeager
authors.affiliation: Savannah River National Laboratory, Aiken, SC, USA.
authors.forename: D I
authors.initials: DI
authors.lastname: Kaplan
mesh_terms: D007457:Iodine Radioisotopes / Q000032:analysis*; D008956:Models, Chemical; D009930:Organic Chemicals / Q000737:chemistry; D011005:Plutonium / Q000032:analysis*; D011834:Radiation Monitoring / Q000379:methods*; D011848:Radioactive Pollutants / Q000032:analysis*; D012987:Soil / Q000737:chemistry
chemical_list: D007457:Iodine Radioisotopes; D009930:Organic Chemicals; D011848:Radioactive Pollutants; D012987:Soil; D011005:Plutonium
keywords: Aromatic acids; Hydroxamates; Iodine; Natural organic matter moieties; Plutonium; Speciation