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Title: Mass-transfer limitation for nitrate removal in a uranium-contaminated aquifer at Oak Ridge, TN

Abstract

A field test on in situ subsurface bioremediation of uranium(VI) is underway at the Y-12 National Security Complex in the Oak Ridge Reservation, Oak Ridge, TN. Nitrate has a high concentration at the site, which prevents U(VI) reduction, and thus must be removed. An acidic-flush strategy for nitrate removal was proposed to create a treatment zone with low levels of accessible nitrate. The subsurface at the site contains highly interconnected fractures surrounded by matrix blocks of low permeability and high porosity and is therefore subject to preferential flow and matrix diffusion. To identify the heterogeneous mass transfer properties, we performed a novel forced-gradient tracer test, which involved the addition of bromide, the displacement of nitrate, and the rebound of nitrate after completion of pumping. The simplest conceptualization consistent with the data is that the pore-space consists of a single mobile domain, as well as a fast and a slowly reacting immobile domain. The slowly reacting immobile domain (shale matrix) constitutes over 80% of the pore volume and acts as a long-term reservoir of nitrate. According to simulations, the nitrate stored in the slowly interacting immobile domain in the fast flow layer, at depths of about 12.2-13.7 m, will be reducedmore » by an order of magnitude over a period of about a year. By contrast, the mobile domain rapidly responds to flushing, and a low average nitrate concentration can be maintained if the nitrate is removed as soon as it enters the mobile domain. A field-scale experiment in which the aquifer was flushed with acidic solution confirmed our understanding of the system. For the ongoing experiments on microbial U(VI) reduction, nitrate concentrations must be low in the mobile domain to ensure U(VI) reducing conditions. We therefore conclude that the nitrate leaching out of the immobile pore space must continuously be removed by in situ denitrification to maintain favorable conditions.« less

Authors:
 [1];  [2];  [1];  [2];  [2];  [2];  [2];  [1];  [1]
  1. Stanford University
  2. ORNL
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
986459
DOE Contract Number:  
DE-AC05-00OR22725
Resource Type:
Journal Article
Journal Name:
Environmental Science & Technology
Additional Journal Information:
Journal Volume: 39; Journal Issue: 21; Journal ID: ISSN 0013-936X
Country of Publication:
United States
Language:
English
Subject:
45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEFENSE; 99 GENERAL AND MISCELLANEOUS//MATHEMATICS, COMPUTING, AND INFORMATION SCIENCE; AQUIFERS; BIOREMEDIATION; DENITRIFICATION; DIFFUSION; FIELD TESTS; FRACTURES; LEACHING; MASS TRANSFER; NATIONAL SECURITY; NITRATES; OAK RIDGE RESERVATION; PERMEABILITY; POROSITY; PUMPING; REMOVAL

Citation Formats

Luo, Jian, Cirpka, Olaf, Wu, Weimin, Fienen, Michael, Mehlhorn, Tonia L, Jardine, Philip M, Watson, David B, Criddle, Craig, and Kitanidis, Peter K. Mass-transfer limitation for nitrate removal in a uranium-contaminated aquifer at Oak Ridge, TN. United States: N. p., 2005. Web. doi:10.1021/es050195g.
Luo, Jian, Cirpka, Olaf, Wu, Weimin, Fienen, Michael, Mehlhorn, Tonia L, Jardine, Philip M, Watson, David B, Criddle, Craig, & Kitanidis, Peter K. Mass-transfer limitation for nitrate removal in a uranium-contaminated aquifer at Oak Ridge, TN. United States. https://doi.org/10.1021/es050195g
Luo, Jian, Cirpka, Olaf, Wu, Weimin, Fienen, Michael, Mehlhorn, Tonia L, Jardine, Philip M, Watson, David B, Criddle, Craig, and Kitanidis, Peter K. 2005. "Mass-transfer limitation for nitrate removal in a uranium-contaminated aquifer at Oak Ridge, TN". United States. https://doi.org/10.1021/es050195g.
@article{osti_986459,
title = {Mass-transfer limitation for nitrate removal in a uranium-contaminated aquifer at Oak Ridge, TN},
author = {Luo, Jian and Cirpka, Olaf and Wu, Weimin and Fienen, Michael and Mehlhorn, Tonia L and Jardine, Philip M and Watson, David B and Criddle, Craig and Kitanidis, Peter K},
abstractNote = {A field test on in situ subsurface bioremediation of uranium(VI) is underway at the Y-12 National Security Complex in the Oak Ridge Reservation, Oak Ridge, TN. Nitrate has a high concentration at the site, which prevents U(VI) reduction, and thus must be removed. An acidic-flush strategy for nitrate removal was proposed to create a treatment zone with low levels of accessible nitrate. The subsurface at the site contains highly interconnected fractures surrounded by matrix blocks of low permeability and high porosity and is therefore subject to preferential flow and matrix diffusion. To identify the heterogeneous mass transfer properties, we performed a novel forced-gradient tracer test, which involved the addition of bromide, the displacement of nitrate, and the rebound of nitrate after completion of pumping. The simplest conceptualization consistent with the data is that the pore-space consists of a single mobile domain, as well as a fast and a slowly reacting immobile domain. The slowly reacting immobile domain (shale matrix) constitutes over 80% of the pore volume and acts as a long-term reservoir of nitrate. According to simulations, the nitrate stored in the slowly interacting immobile domain in the fast flow layer, at depths of about 12.2-13.7 m, will be reduced by an order of magnitude over a period of about a year. By contrast, the mobile domain rapidly responds to flushing, and a low average nitrate concentration can be maintained if the nitrate is removed as soon as it enters the mobile domain. A field-scale experiment in which the aquifer was flushed with acidic solution confirmed our understanding of the system. For the ongoing experiments on microbial U(VI) reduction, nitrate concentrations must be low in the mobile domain to ensure U(VI) reducing conditions. We therefore conclude that the nitrate leaching out of the immobile pore space must continuously be removed by in situ denitrification to maintain favorable conditions.},
doi = {10.1021/es050195g},
url = {https://www.osti.gov/biblio/986459}, journal = {Environmental Science & Technology},
issn = {0013-936X},
number = 21,
volume = 39,
place = {United States},
year = {Thu Sep 01 00:00:00 EDT 2005},
month = {Thu Sep 01 00:00:00 EDT 2005}
}