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Title: Dissolved Organic Carbon 14C in Southern Nevada Groundwater and Implications for Groundwater Travel Times

Abstract

Dissolved inorganic carbon (DIC) carbon-14 ( 14C) ages must be corrected for complex chemical and physical reactions and processes that change the amount of 14C in groundwater as it flows from recharge to downgradient areas. Because of these reactions, DIC 14C can produce unrealistically old ages and long groundwater travel times that may, or may not, agree with travel times estimated by other methods. Dissolved organic carbon (DOC) 14C ages are often younger than DIC 14C ages because there are few chemical reactions or physical processes that change the amount of DOC 14C in groundwater. However, there are several issues that create uncertainty in DOC 14C groundwater ages including limited knowledge of the initial (A 0) DOC 14C in groundwater recharge and potential changes in DOC composition as water moves through an aquifer. This study examines these issues by quantifying A 0 DOC 14C in recharge areas of southern Nevada groundwater flow systems and by evaluating changes in DOC composition as water flows from recharge areas to downgradient areas. The effect of these processes on DOC 14C groundwater ages is evaluated and DOC and DIC 14C ages are then compared along several southern Nevada groundwater flow paths. Twenty-seven groundwater samplesmore » were collected from springs and wells in southern Nevada in upgradient, midgradient, and downgradient locations. DOC 14C for upgradient samples ranged from 96 to 120 percent modern carbon (pmc) with an average of 106 pmc, verifying modern DOC 14C ages in recharge areas, which decreases uncertainty in DOC 14C A 0 values, groundwater ages, and travel times. The HPLC spectra of groundwater along a flow path in the Spring Mountains show the same general pattern indicating that the DOC compound composition does not change along this flow path. Although DOC concentration decreases from recharge-area to downgradient groundwater, the organic compounds are similar, indicating that DOC 14C is unaffected by other processes such as microbial degradation. A small amount of organic carbon was leached from crushed volcanic and carbonate aquifer outcrop rock in rock-leaching experiments. The leached DOC was high in 14C (75 pmc carbonate rocks, 91 pmc volcanic) suggesting that the leached DOC likely came from microbes in the rock samples. The small amount of DOC and high 14C indicates that the amount of old organic carbon in these rocks is low so there should be minimal impact on groundwater DOC 14C ages. Based on the results from this study, DOC 14C ages do not require additional corrections. Several correction models were applied to DIC 14C ages to correct for water-rock reactions along two carbonate and two volcanic flow paths and the corresponding travel times were compare to DOC 14C travel times. The DOC 14C travel times were hundreds to thousands of years shorter than uncorrected and corrected DIC 14C travel times except for the upper section of one carbonate flow path. DOC 14C travel times ranged from 400 to 5,400 years as compared to DIC 14C that ranged from modern to 20,900 years. The DIC 14C ages are greatly influenced by carbonate mineral and gas reactions and other processes such as matrix diffusion, isotope exchange, or adsorption, which are not always adequately accounted for in DIC 14C groundwater age correction models.« less

Authors:
 [1];  [1];  [1]
  1. Nevada University, Reno, NV (United States). Desert Research Institute
Publication Date:
Research Org.:
Nevada University, Reno, NV (United States). Desert Research Institute
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1287225
Report Number(s):
45268
DOE/NV/0000939-34
DOE Contract Number:
NA0000939
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Hershey, Ronald L., Fereday, Wyall, and Thomas, James M. Dissolved Organic Carbon 14C in Southern Nevada Groundwater and Implications for Groundwater Travel Times. United States: N. p., 2016. Web. doi:10.2172/1287225.
Hershey, Ronald L., Fereday, Wyall, & Thomas, James M. Dissolved Organic Carbon 14C in Southern Nevada Groundwater and Implications for Groundwater Travel Times. United States. doi:10.2172/1287225.
Hershey, Ronald L., Fereday, Wyall, and Thomas, James M. 2016. "Dissolved Organic Carbon 14C in Southern Nevada Groundwater and Implications for Groundwater Travel Times". United States. doi:10.2172/1287225. https://www.osti.gov/servlets/purl/1287225.
@article{osti_1287225,
title = {Dissolved Organic Carbon 14C in Southern Nevada Groundwater and Implications for Groundwater Travel Times},
author = {Hershey, Ronald L. and Fereday, Wyall and Thomas, James M},
abstractNote = {Dissolved inorganic carbon (DIC) carbon-14 (14C) ages must be corrected for complex chemical and physical reactions and processes that change the amount of 14C in groundwater as it flows from recharge to downgradient areas. Because of these reactions, DIC 14C can produce unrealistically old ages and long groundwater travel times that may, or may not, agree with travel times estimated by other methods. Dissolved organic carbon (DOC) 14C ages are often younger than DIC 14C ages because there are few chemical reactions or physical processes that change the amount of DOC 14C in groundwater. However, there are several issues that create uncertainty in DOC 14C groundwater ages including limited knowledge of the initial (A0) DOC 14C in groundwater recharge and potential changes in DOC composition as water moves through an aquifer. This study examines these issues by quantifying A0 DOC 14C in recharge areas of southern Nevada groundwater flow systems and by evaluating changes in DOC composition as water flows from recharge areas to downgradient areas. The effect of these processes on DOC 14C groundwater ages is evaluated and DOC and DIC 14C ages are then compared along several southern Nevada groundwater flow paths. Twenty-seven groundwater samples were collected from springs and wells in southern Nevada in upgradient, midgradient, and downgradient locations. DOC 14C for upgradient samples ranged from 96 to 120 percent modern carbon (pmc) with an average of 106 pmc, verifying modern DOC 14C ages in recharge areas, which decreases uncertainty in DOC 14C A0 values, groundwater ages, and travel times. The HPLC spectra of groundwater along a flow path in the Spring Mountains show the same general pattern indicating that the DOC compound composition does not change along this flow path. Although DOC concentration decreases from recharge-area to downgradient groundwater, the organic compounds are similar, indicating that DOC 14C is unaffected by other processes such as microbial degradation. A small amount of organic carbon was leached from crushed volcanic and carbonate aquifer outcrop rock in rock-leaching experiments. The leached DOC was high in 14C (75 pmc carbonate rocks, 91 pmc volcanic) suggesting that the leached DOC likely came from microbes in the rock samples. The small amount of DOC and high 14C indicates that the amount of old organic carbon in these rocks is low so there should be minimal impact on groundwater DOC 14C ages. Based on the results from this study, DOC 14C ages do not require additional corrections. Several correction models were applied to DIC 14C ages to correct for water-rock reactions along two carbonate and two volcanic flow paths and the corresponding travel times were compare to DOC 14C travel times. The DOC 14C travel times were hundreds to thousands of years shorter than uncorrected and corrected DIC 14C travel times except for the upper section of one carbonate flow path. DOC 14C travel times ranged from 400 to 5,400 years as compared to DIC 14C that ranged from modern to 20,900 years. The DIC 14C ages are greatly influenced by carbonate mineral and gas reactions and other processes such as matrix diffusion, isotope exchange, or adsorption, which are not always adequately accounted for in DIC 14C groundwater age correction models.},
doi = {10.2172/1287225},
journal = {},
number = ,
volume = ,
place = {United States},
year = 2016,
month = 8
}

Technical Report:

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  • Dissolved inorganic carbon (DIC) carbon-14 ( 14C) is used to estimate groundwater ages by comparing the DIC 14C content in groundwater in the recharge area to the DIC 14C content in the downgradient sampling point. However, because of chemical reactions and physical processes between groundwater and aquifer rocks, the amount of DIC 14C in groundwater can change and result in 14C loss that is not because of radioactive decay. This loss of DIC 14C results in groundwater ages that are older than the actual groundwater ages. Alternatively, dissolved organic carbon (DOC) 14C in groundwater does not react chemically with aquifermore » rocks, so DOC 14C ages are generally younger than DIC 14C ages. In addition to chemical reactions, 14C ages may also be altered by the physical process of matrix diffusion. The net effect of a continuous loss of 14C to the aquifer matrix by matrix diffusion and then radioactive decay is that groundwater appears to be older than it actually is. Laboratory experiments were conducted to measure matrix diffusion coefficients for DOC 14C in volcanic and carbonate aquifer rocks from southern Nevada. Experiments were conducted using bromide (Br-) as a conservative tracer and 14C-labeled trimesic acid (TMA) as a surrogate for groundwater DOC. Outcrop samples from six volcanic aquifers and five carbonate aquifers in southern Nevada were used. The average DOC 14C matrix diffusion coefficient for volcanic rocks was 2.9 x 10 -7 cm 2/s, whereas the average for carbonate rocks was approximately the same at 1.7 x 10 -7 cm 2/s. The average Br- matrix diffusion coefficient for volcanic rocks was 10.4 x 10 -7 cm 2/s, whereas the average for carbonate rocks was less at 6.5 x 10 -7 cm 2/s. Carbonate rocks exhibited greater variability in DOC 14C and Br- matrix diffusion coefficients than volcanic rocks. These results confirmed, at the laboratory scale, that the diffusion of DOC 14C into southern Nevada volcanic and carbonate aquifers is slower than DIC 14C. Because of the apparent sorption of 14C-labeled TMA in the experiments, matrix diffusion coefficients are likely even lower. The reasons for the higher than expected Br-/ 14C-labeled TMA are unknown. Because the molecular size of TMA is on the low end of the range in molecular size for typical humic substances, the matrix diffusion coefficients for the 14C-labeled TMA likely represent close to the maximum diffusion rates for DOC 14C in the volcanic and carbonate aquifers in southern Nevada.« less
  • Yucca Mountain (YM), Nevada, has been recommended as a deep geological repository for the disposal of spent fuel and high-level radioactive waste. If YM is licensed as a repository by the Nuclear Regulatory Commission, it will be important to identify the potential for radionuclides to migrate from underground nuclear testing areas located on the Nevada Test Site (NTS) to the hydraulically downgradient repository area to ensure that monitoring does not incorrectly attribute repository failure to radionuclides originating from other sources. In this study, we use the Death Valley Regional Flow System (DVRFS) model developed by the U.S. Geological Survey tomore » investigate potential groundwater migration pathways and associated travel times from the NTS to the proposed YM repository area. Using results from the calibrated DVRFS model and the particle tracking post-processing package MODPATH, we modeled three-dimensional groundwater advective pathways in the NTS and YM region. Our study focuses on evaluating the potential for groundwater pathways between the NTS and YM withdrawal area and whether travel times for advective flow along these pathways coincide with the prospective monitoring timeframe at the proposed repository. We include uncertainty in effective porosity, as this is a critical variable in the determination of time for radionuclides to travel from the NTS region to the YM withdrawal area. Uncertainty in porosity is quantified through evaluation of existing site data and expert judgment and is incorporated in the model through Monte Carlo simulation. Since porosity information is limited for this region, the uncertainty is quite large and this is reflected in the results as a large range in simulated groundwater travel times.« less
  • Unsaturated flow has been modeled through four cross-sections at Yucca Mountain, Nevada, for the purpose of determining groundwater particle travel times from the potential repository to the water table. This work will be combined with the results of flow modeling in the saturated zone for the purpose of evaluating the suitability of the potential repository under the criteria of 10CFR960. One criterion states, in part, that the groundwater travel time (GWTT) from the repository to the accessible environment must exceed 1,000 years along the fastest path of likely and significant radionuclide travel. Sensitivity analyses have been conducted for one geostatisticalmore » realization of one cross-section for the purpose of (1) evaluating the importance of hydrological parameters having some uncertainty (infiltration, fracture-matrix connectivity, fracture frequency, and matrix air entry pressure or van Genuchten {alpha}); and (2) examining conceptual models of flow by altering the numerical implementation of the conceptual model (dual permeability (DK) and the equivalent continuum model (ECM)). Results of comparisons of the ECM and DK model are also presented in Ho et al.« less
  • Preliminary uncertainty analyses of pre-waste-emplacement groundwater travel times are presented for a potential high-level nuclear waste repository in the deep basalts beneath the Hanford Site, Washington State. The uncertainty analyses are carried out by means of a Monte Carlo technique, which requires the uncertain inputs to be described as either random variables or spatial stochastic processes. Pre-waste-emplacement groundwater travel times are modeled in a continuous, flat-lying basalt flow top that is assumed to overlie the repository horizon. Two-dimensional, steady state groundwater flow is assumed, and transmissivity, effective thickness, and regional hydraulic gradient are considered as uncertain inputs. Groundwater travel timemore » distributions corresponding to three groundwater models are presented and compared. Limitations of these preliminary simulation results are discussed in detail.« less