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Title: Fate and transport of hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX) and its degradation products in sedimentary and volcanic rocks, Los Alamos, New Mexico

Abstract

High-explosive compounds including hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX) were used extensively in weapons research and testing at Los Alamos National Laboratory (LANL). Liquid effluents containing RDX were released to an outfall pond that flowed to Cañon de Valle at LANL's Technical Area 16 (TA-16), resulting in the contamination of the alluvial, intermediate and regional groundwater bodies. Monitoring of groundwater within Cañon de Valle has shown persistent RDX in the intermediate perched zone located between 225 and 311 m below ground surface. Monitoring data also show detectable levels of RDX putative anaerobic degradation products. Batch and column experiments were conducted to determine the extent of adsorption-desorption and transport of RDX and its degradation products (MNX, DNX, and TNX) in major rock types that are within the RDX plume. All experiments in this paper were performed in the dark using water obtained from a well located at the center of the plume, which is fairly oxic and has a neutral pH of 7.5. Retardation factors and partitioning coefficient (K d) values for RDX were calculated from batch experiments. Additionally, retardation factors and K d values for RDX and its degradation products were calibrated from column experiments using a one-dimensional transport model with equilibrium sorption (linearmore » isotherm). Results from the column and batch experiments showed little to no sorption of RDX to the aquifer materials tested, with retardation factors ranging from 1.0 to 1.8 and K d values varying from 0 to 0.70 L/kg. Finally, results also showed no measurable differences between the transport properties of RDX and its degradation products.« less

Authors:
 [1]; ORCiD logo [1];  [1];  [1];  [1];  [1];  [1];  [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Environmental Management (EM)
OSTI Identifier:
1357122
Alternate Identifier(s):
OSTI ID: 1396516
Report Number(s):
LA-UR-16-28243
Journal ID: ISSN 0045-6535
Grant/Contract Number:
AC52-06NA25396
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Chemosphere
Additional Journal Information:
Journal Volume: 182; Journal ID: ISSN 0045-6535
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; Earth Sciences; Environmental Protection; RDX, TNT, transport, adsorption, retardation

Citation Formats

Heerspink, Brent Porter, Pandey, Sachin, Boukhalfa, Hakim, Ware, Doug S., Marina, Oana, Perkins, George, Vesselinov, Velimir V., and WoldeGabriel, Giday. Fate and transport of hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX) and its degradation products in sedimentary and volcanic rocks, Los Alamos, New Mexico. United States: N. p., 2017. Web. doi:10.1016/j.chemosphere.2017.04.149.
Heerspink, Brent Porter, Pandey, Sachin, Boukhalfa, Hakim, Ware, Doug S., Marina, Oana, Perkins, George, Vesselinov, Velimir V., & WoldeGabriel, Giday. Fate and transport of hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX) and its degradation products in sedimentary and volcanic rocks, Los Alamos, New Mexico. United States. doi:10.1016/j.chemosphere.2017.04.149.
Heerspink, Brent Porter, Pandey, Sachin, Boukhalfa, Hakim, Ware, Doug S., Marina, Oana, Perkins, George, Vesselinov, Velimir V., and WoldeGabriel, Giday. Tue . "Fate and transport of hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX) and its degradation products in sedimentary and volcanic rocks, Los Alamos, New Mexico". United States. doi:10.1016/j.chemosphere.2017.04.149. https://www.osti.gov/servlets/purl/1357122.
@article{osti_1357122,
title = {Fate and transport of hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX) and its degradation products in sedimentary and volcanic rocks, Los Alamos, New Mexico},
author = {Heerspink, Brent Porter and Pandey, Sachin and Boukhalfa, Hakim and Ware, Doug S. and Marina, Oana and Perkins, George and Vesselinov, Velimir V. and WoldeGabriel, Giday},
abstractNote = {High-explosive compounds including hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX) were used extensively in weapons research and testing at Los Alamos National Laboratory (LANL). Liquid effluents containing RDX were released to an outfall pond that flowed to Cañon de Valle at LANL's Technical Area 16 (TA-16), resulting in the contamination of the alluvial, intermediate and regional groundwater bodies. Monitoring of groundwater within Cañon de Valle has shown persistent RDX in the intermediate perched zone located between 225 and 311 m below ground surface. Monitoring data also show detectable levels of RDX putative anaerobic degradation products. Batch and column experiments were conducted to determine the extent of adsorption-desorption and transport of RDX and its degradation products (MNX, DNX, and TNX) in major rock types that are within the RDX plume. All experiments in this paper were performed in the dark using water obtained from a well located at the center of the plume, which is fairly oxic and has a neutral pH of 7.5. Retardation factors and partitioning coefficient (Kd) values for RDX were calculated from batch experiments. Additionally, retardation factors and Kd values for RDX and its degradation products were calibrated from column experiments using a one-dimensional transport model with equilibrium sorption (linear isotherm). Results from the column and batch experiments showed little to no sorption of RDX to the aquifer materials tested, with retardation factors ranging from 1.0 to 1.8 and Kd values varying from 0 to 0.70 L/kg. Finally, results also showed no measurable differences between the transport properties of RDX and its degradation products.},
doi = {10.1016/j.chemosphere.2017.04.149},
journal = {Chemosphere},
number = ,
volume = 182,
place = {United States},
year = {Tue May 02 00:00:00 EDT 2017},
month = {Tue May 02 00:00:00 EDT 2017}
}

Journal Article:
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  • Hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX), a widely used munitions compound, and hexahydro-1-nitroso-3,5-dinitro-1,3,5-triazine (MNX), its N-nitroso product of anaerobic microbial nitroreduction, are contaminants of military sites. Previous studies have shown MNX to be the most acutely toxic among the nitroreduced degradation products of RDX and to cause mild anemia at high dose. The present study compares hematotoxicity with acute oral exposure to MNX with parent RDX. Both RDX and MNX caused a modest decrease in blood hemoglobin and ∼ 50% loss of granulocytes (NOAELs = 47 mg/kg) in female Sprague–Dawley rats observed 14 days post-exposure. We explored the possibility that blood cell loss observedmore » after 14 days was delayed in onset because of toxicity to bone marrow (BM) progenitors. RDX and MNX decreased granulocyte/macrophage-colony forming cells (GM-CFCs) at 14, but not 7, days (NOAELs = 24 mg/kg). The earliest observed time at which MNX decreased GM-CFCs was 10 days post-exposure. RDX and MNX likewise decreased BM burst-forming units-erythroid (BFU-Es) at 14, but not 7, days. Granulocyte–erythrocyte–monocyte–megakaryocyte (GEMM)-CFCs were unaffected by RDX and MNX at 7 days suggesting precursor depletion did not account for GM-CFC and BFU-E loss. MNX added to the culture media was without effect on GM-CFC formation indicating no direct inhibition. Flow cytometry showed no differential loss of BM multilineage progenitors (Thy1.1{sup +}) or erythroid (CD71{sup +}) precursors with MNX suggesting myeloid and erythroid lineages were comparably affected. Collectively, these data indicate that acute exposure to both RDX and MNX caused delayed suppression of myelo- and erythropoiesis with subsequent decrease of peripheral granulocytes and erythrocytes. Highlights: ► Acute oral exposure to munitions RDX causes myelosuppression. ► Environmental degradation product MNX is comparable in effect. ► RDX and MNX are cytotoxic to both myeloid and erythroid progenitor cells. ► Myelosuppression is delayed in onset by > 7 days after single exposure.« less
  • Soils amended with [[sup 14]C]hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX) were sampled over 60 d and subjected to exhaustive Soxhlet extraction followed by HPLC analysis. RDX was the only radiolabeled compound observed in soil extracts. Emission of volatile organics and [sup 14]CO[sub 2] from soil accounted for only 0.31 % of the amended radiolabel. Mass balance for RDX-amended soil was better than 84% throughout the two-month study. The analytical method developed for plants involved acid hydrolysis, solvent extraction, fractionation on Florisil adsorbent and separation by HPLC. The described methodology allowed for RDX recovery of 86 [+-] 3% from fortified bush bean leaf tissue. Furthermore » experiments were conducted with bush bean plants maintained on RDX-containing hydroponic solutions. Hydroponic plants did not emit detectable amounts of [sup 14]CO[sub 2] or radiolabeled volatile organics. Analysis of the plant tissue indicated bioaccumulation of RDX in the aerial tissues of hydroponic plants exposed for either 1 or 7 d. Metabolism of RDX to polar metabolites was observed in plants exposed for 7 d.« less
  • The biotransformation of hexahydro-1,3,5-trinitro-1,3,5 triazine (RDX) has been observed in liquid culture by a consortium of bacteria found in horse manure. Five types of bacteria were found to predominate in the consortium and were isolated. The most effective of these isolates at transforming RDX was Serratia marcescens. The biotransformation of RDX by all of these bacteria was found to occur only in the anoxic stationary phase. The process of bacterial growth and RDX biotransformation was quantified for the purpose of developing a predictive type model. Cell growth was assumed to follow Monod kinetics. All of the aerobic and anoxid growthmore » parameters were determined: {mu}{sub max}, K{sub s}, and Y{sub x/s}. RDX was found to competitively inhibit cell growth in both atmospheres. Degradation of RDX by Serratia marcescens was found to proceed through the stepwise reduction of the three nitro groups to nitroso groups. Each of these reductions was found to be first order in both component and cell concentrations. The degradation rate constant for the first step in this reduction process by the consortium was 0.022 L/g cells {center_dot} h compared to 0.033 L/g cells {center_dot} h for the most efficient isolate.« less
  • The U.S. Environmental Protection Agency (USEPA) has recently recommended a lifetime health advisory (HA) for hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX). The purpose of this brief article is to present the basis for the calculation of the HA so that the reader can compare it with a water quality criterion (WQC) that has been proposed. In the earlier article, a water quality criterion of 105 micrograms/liter for RDX in drinking water was proposed, and in the present article the methodology by which USEPA calculated a lifetime HA of 2 micrograms/liter is presented. The differences in the derivation of the WQC and the HA aremore » discussed. 7 references.« less