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Title: Influence of physical and chemical hydrology on bioremediation of a U-contaminated aquifer informed by reactive transport modeling incorporating 238U/235U ratios

Abstract

Microbially-catalyzed reductive immobilization of aqueous uranium (U) as a solid phase has been proposed as a U remediation technique. Both laboratory and field experiments have demonstrated that this reduction reaction alters the 238U/235U ratio, producing a 238U-enriched U(IV) solid. In contrast, other major U reactive transport processes fractionate these isotopes much less. This suggests the potential to quantify the extent of bioreduction occurring in groundwater containing U using the 238U/235U ratio, which would substantially improve upon current practices largely relying on U concentration measurements alone. Current reactive transport models for uranium dynamics include only concentration measurements, which are strongly influenced by highly coupled reactive transformation and aqueous transport processes. The complex physical and chemical behavior of U potentially compromises such quantitative analysis of U storage and release. Here we report the first numerical reactive transport model which explicitly incorporates variations in the 238U/235U ratio of U and demonstrates improved interpretation of the principal chemical reactions and groundwater transport processes affecting the subsurface mobility and distribution of this widespread contaminant.Recent U bioreduction studies performed in a contaminated aquifer in Rifle, Colorado, USA applied Rayleigh distillation models to interpret U stable isotope fractionation observed as a result of acetate amendment. These simplifiedmore » models were unable to resolve the spatiotemporal pattern of U isotope fractionation recorded in the aqueous solutes. Here, we employ the multi-component, isotope-enabled CrunchTope reactive transport software to interpret these measured U isotope ratios, and demonstrate accurate reproduction of observed trends in both geochemistry and 238U/235U ratios for two consecutive years of field experiments. Overall, our results indicate that accurately modeling both the U concentration and isotope ratio distributions greatly constrains the parameter space of the model. We find that the transport properties of U in the Rifle aquifer are governed by the presence of low-permeability regions, which the isotopes are uniquely sensitive to. When U reduction is spatially constrained by these low-permeability regions, the shift in the 238U/235U ratio becomes more muted. Accurate modeling of observed U isotope ratios thus provides a powerful means to better understand bioremediation, and the current study serves to advance the application of this novel method.« less

Authors:
ORCiD logo [1];  [2];  [3]; ORCiD logo [3]
+ Show Author Affiliations
  1. Univ. of Illinois at Urbana-Champaign, IL (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Univ. of Illinois at Urbana-Champaign, IL (United States); Geosyntec Consultants, Chicago, IL (United States)
  3. Univ. of Illinois at Urbana-Champaign, IL (United States)
Publication Date:
Research Org.:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC). Biological and Environmental Research (BER); USDOE
OSTI Identifier:
1735894
Alternate Identifier(s):
OSTI ID: 1775795
Report Number(s):
LA-UR-19-21464
Journal ID: ISSN 0016-7037
Grant/Contract Number:  
89233218CNA000001; SC0006755
Resource Type:
Accepted Manuscript
Journal Name:
Geochimica et Cosmochimica Acta
Additional Journal Information:
Journal Volume: 269; Journal ID: ISSN 0016-7037
Publisher:
Elsevier; The Geochemical Society; The Meteoritical Society
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 238U/235U; groundwater contamination; remediation; reactive transport modeling; aquifer heterogeneity

Citation Formats

Jemison, Noah E., Bizjack, Matthew T., Johnson, Thomas M., and Druhan, Jennifer L. Influence of physical and chemical hydrology on bioremediation of a U-contaminated aquifer informed by reactive transport modeling incorporating 238U/235U ratios. United States: N. p., 2020. Web. doi:10.1016/j.gca.2019.10.031.
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Jemison, Noah E., Bizjack, Matthew T., Johnson, Thomas M., & Druhan, Jennifer L. Influence of physical and chemical hydrology on bioremediation of a U-contaminated aquifer informed by reactive transport modeling incorporating 238U/235U ratios. United States. https://doi.org/10.1016/j.gca.2019.10.031
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Jemison, Noah E., Bizjack, Matthew T., Johnson, Thomas M., and Druhan, Jennifer L. Mon . "Influence of physical and chemical hydrology on bioremediation of a U-contaminated aquifer informed by reactive transport modeling incorporating 238U/235U ratios". United States. https://doi.org/10.1016/j.gca.2019.10.031. https://www.osti.gov/servlets/purl/1735894.
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@article{osti_1735894,
title = {Influence of physical and chemical hydrology on bioremediation of a U-contaminated aquifer informed by reactive transport modeling incorporating 238U/235U ratios},
author = {Jemison, Noah E. and Bizjack, Matthew T. and Johnson, Thomas M. and Druhan, Jennifer L.},
abstractNote = {Microbially-catalyzed reductive immobilization of aqueous uranium (U) as a solid phase has been proposed as a U remediation technique. Both laboratory and field experiments have demonstrated that this reduction reaction alters the 238U/235U ratio, producing a 238U-enriched U(IV) solid. In contrast, other major U reactive transport processes fractionate these isotopes much less. This suggests the potential to quantify the extent of bioreduction occurring in groundwater containing U using the 238U/235U ratio, which would substantially improve upon current practices largely relying on U concentration measurements alone. Current reactive transport models for uranium dynamics include only concentration measurements, which are strongly influenced by highly coupled reactive transformation and aqueous transport processes. The complex physical and chemical behavior of U potentially compromises such quantitative analysis of U storage and release. Here we report the first numerical reactive transport model which explicitly incorporates variations in the 238U/235U ratio of U and demonstrates improved interpretation of the principal chemical reactions and groundwater transport processes affecting the subsurface mobility and distribution of this widespread contaminant.Recent U bioreduction studies performed in a contaminated aquifer in Rifle, Colorado, USA applied Rayleigh distillation models to interpret U stable isotope fractionation observed as a result of acetate amendment. These simplified models were unable to resolve the spatiotemporal pattern of U isotope fractionation recorded in the aqueous solutes. Here, we employ the multi-component, isotope-enabled CrunchTope reactive transport software to interpret these measured U isotope ratios, and demonstrate accurate reproduction of observed trends in both geochemistry and 238U/235U ratios for two consecutive years of field experiments. Overall, our results indicate that accurately modeling both the U concentration and isotope ratio distributions greatly constrains the parameter space of the model. We find that the transport properties of U in the Rifle aquifer are governed by the presence of low-permeability regions, which the isotopes are uniquely sensitive to. When U reduction is spatially constrained by these low-permeability regions, the shift in the 238U/235U ratio becomes more muted. Accurate modeling of observed U isotope ratios thus provides a powerful means to better understand bioremediation, and the current study serves to advance the application of this novel method.},
doi = {10.1016/j.gca.2019.10.031},
journal = {Geochimica et Cosmochimica Acta},
number = ,
volume = 269,
place = {United States},
year = {Mon Nov 09 00:00:00 EST 2020},
month = {Mon Nov 09 00:00:00 EST 2020}
}
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