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

Jemison, Noah E.; Bizjack, Matthew T.; Johnson, Thomas M.; Druhan, Jennifer L.

doi:10.1016/j.gca.2019.10.031

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

Journal Article · Mon Nov 09 00:00:00 EST 2020 · Geochimica et Cosmochimica Acta

DOI:https://doi.org/10.1016/j.gca.2019.10.031· OSTI ID:1735894

^[1]; Bizjack, Matthew T. ^[2]; Johnson, Thomas M. ^[3]; ^[3]

Univ. of Illinois at Urbana-Champaign, IL (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Univ. of Illinois at Urbana-Champaign, IL (United States); Geosyntec Consultants, Chicago, IL (United States)
Univ. of Illinois at Urbana-Champaign, IL (United States)

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.

View Accepted Manuscript (DOE)

Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC). Biological and Environmental Research (BER)

Grant/Contract Number:: 89233218CNA000001; SC0006755

OSTI ID:: 1735894

Alternate ID(s):: OSTI ID: 1775795

Report Number(s):: LA-UR--19-21464

Journal Information:: Geochimica et Cosmochimica Acta, Journal Name: Geochimica et Cosmochimica Acta Vol. 269; ISSN 0016-7037

Publisher:: Elsevier; The Geochemical Society; The Meteoritical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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

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