Geophysical monitoring and reactive transport modeling of ureolytically-driven calcium carbonate precipitation

Ureolytically-driven calcium carbonate precipitation is the basis for a promising in-situ remediation method for sequestration of divalent radionuclide and trace metal ions. It has also been proposed for use in geotechnical engineering for soil strengthening applications. Monitoring the occurrence, spatial distribution, and temporal evolution of calcium carbonate precipitation in the subsurface is critical for evaluating the performance of this technology and for developing the predictive models needed for engineering application. In this study, we conducted laboratory column experiments using natural sediment and groundwater to evaluate the utility of geophysical (complex resistivity and seismic) sensing methods, dynamic synchrotron x-ray computed tomography (micro-CT), and reactive transport modeling for tracking ureolytically-driven calcium carbonate precipitation processes under site relevant conditions. Reactive transport modeling with TOUGHREACT successfully simulated the changes of the major chemical components during urea hydrolysis. Even at the relatively low level of urea hydrolysis observed in the experiments, the simulations predicted an enhanced calcium carbonate precipitation rate that was 3-4 times greater than the baseline level. Reactive transport modeling results, geophysical monitoring data and micro-CT imaging correlated well with reaction processes validated by geochemical data. In particular, increases in ionic strength of the pore fluid during urea hydrolysis predicted by geochemical modeling were successfully captured by electrical conductivity measurements and confirmed by geochemical data. The low level of urea hydrolysis and calcium carbonate precipitation suggested by the model and geochemical data was corroborated by minor changes in seismic P-wave velocity measurements and micro-CT imaging; the latter provided direct evidence of sparsely distributed calcium carbonate precipitation. Ion exchange processes promoted through NH4+ production during urea hydrolysis were incorporated in the model and captured critical changes in the major metal species. The electrical phase increases were potentially due to ion exchange processes that modified charge structure at mineral/water interfaces. Our study revealed the potential of geophysical monitoring for geochemical changes during urea hydrolysis and the advantages of combining multiple approaches to understand complex biogeochemical processes in the subsurface.

[1]  K. A. Winfield.  Spatial variability of sedimentary interbed properties near the Idaho Nuclear Technology and Engineering Center at the Idaho National Engineering and Environmental Laboratory, Idaho , 2003 .

[2]  A. Demond,et al.  Packing of Sands for the Production of Homogeneous Porous Media , 1996 .

[3]  André Revil,et al.  Induced polarization signatures of cations exhibiting differential sorption behaviors in saturated sands , 2011 .

[4]  P. Maurice,et al.  Microbially Mediated Calcium Carbonate Precipitation: Implications for Interpreting Calcite Precipitation and for Solid-Phase Capture of Inorganic Contaminants , 2001 .

[5]  L. Pyrak‐Nolte,et al.  Microbial‐induced heterogeneity in the acoustic properties of porous media , 2009 .

[6]  G. E. Archie.  The electrical resistivity log as an aid in determining some reservoir characteristics , 1942 .

[7]  Yousif K. Kharaka,et al.  A Compilation of Rate Parameters of Water-Mineral Interaction Kinetics for Application to Geochemical Modeling , 2004 .

[8]  Bärbel Tiemeyer,et al.  Artificially Drained Catchments—From Monitoring Studies towards Management Approaches , 2010 .

[9]  Yuxin Wu,et al.  On the complex conductivity signatures of calcite precipitation , 2010 .

[10]  A. Lasaga.  Kinetic theory in the earth sciences , 1998 .

[11]  L. Wendt,et al.  Evaluating the potential of native ureolytic microbes to remediate a 90Sr contaminated environment. , 2010, Environmental science & technology.

[12]  M. Mercedes Maroto-Valer,et al.  Investigation of Carbon Sequestration via Induced Calcite Formation in Natural Gas Well Brine , 2006 .

[13]  C. E. Cowan,et al.  Sorption of divalent metals on calcite , 1991 .

[14]  Y. Personna,et al.  Spectral induced polarization and electrodic potential monitoring of microbially mediated iron sulfide transformations , 2008 .

[15]  G. Sposito.  The Gapon and the Vanselow Selectivity Coefficients , 1977 .

[16]  R. Lavecchia,et al.  Kinetic Study of Enzymatic Urea Hydrolysis in the pH Range 4-9 , 2003 .

[17]  Stuart R. Stock,et al.  MicroComputed Tomography: Methodology and Applications , 2008 .

[18]  W. W. Wood,et al.  Aqueous geochemistry and diagenesis in the eastern Snake River Plain aquifer system, Idaho , 1986 .

[19]  Andrew C. Mitchell,et al.  The coprecipitation of Sr into calcite precipitates induced by bacterial ureolysis in artificial groundwater: Temperature and kinetic dependence , 2005 .

[20]  E. Curti.  Coprecipitation of radionuclides with calcite: estimation of partition coefficients based on a review of laboratory investigations and geochemical data , 1999 .

[21]  Sébastien Sauvé,et al.  Toxicity interaction of metals (Ag, Cu, Hg, Zn) to urease and dehydrogenase activities in soils , 2007 .

[22]  Y. Furukawa,et al.  Geochemical Transactions , 2007 .

[23]  Andreas Kemna,et al.  Geophysical monitoring of coupled microbial and geochemical processes during stimulated subsurface bioremediation. , 2009, Environmental science & technology.

[24]  B. C. Martinez,et al.  Forward and Inverse Bio-Geochemical Modeling of Microbially Induced Calcite Precipitation in Half-Meter Column Experiments , 2011 .

[25]  J. DeJong,et al.  Microbially Induced Cementation to Control Sand Response to Undrained Shear , 2006 .

[26]  G. Schwarz.  A THEORY OF THE LOW-FREQUENCY DIELECTRIC DISPERSION OF COLLOIDAL PARTICLES IN ELECTROLYTE SOLUTION1,2 , 1962 .

[27]  Susan S. Hubbard,et al.  Low-frequency electrical response to microbial induced sulfide precipitation , 2005 .

[28]  Frederick S. Colwell,et al.  Calcium Carbonate Precipitation by Ureolytic Subsurface Bacteria , 2000 .

[29]  C. Noiriel,et al.  Hydraulic Properties and Microgeometry Evolution Accompanying Limestone Dissolution by Acidic Water , 2005 .

[30]  Phil Long,et al.  Geophysical monitoring of hydrological and biogeochemical transformations associated with Cr(VI) bioremediation. , 2008, Environmental science & technology.

[31]  Victoria S. Whiffin,et al.  Microbial Carbonate Precipitation as a Soil Improvement Technique , 2007 .

[32]  Vernon R. Phoenix,et al.  Kinetics of calcite precipitation induced by ureolytic bacteria at 10 to 20°C in artificial groundwater , 2004 .

[33]  J. Berryman,et al.  Linear dynamics of double-porosity dual-permeability materials. I. Governing equations and acoustic attenuation. , 2003, Physical review. E, Statistical, nonlinear, and soft matter physics.

[34]  J. Berryman,et al.  Elastic moduli of cemented sphere packs , 1999 .

[35]  Jani C. Ingram,et al.  Strontium incorporation into calcite generated by bacterial ureolysis , 2002 .

[36]  Karsten Pruess,et al.  TOUGHREACT Version 2.0: A simulator for subsurface reactive transport under non-isothermal multiphase flow conditions , 2011, Comput. Geosci..

[37]  Frederick S. Colwell,et al.  Subscribed Content Calcium Carbonate Precipitation by Ureolytic Subsurface Bacteria , 2000 .

[38]  S. Hubbard,et al.  Pore‐scale spectral induced polarization signatures associated with FeS biomineral transformations , 2007 .

[39]  L. Slater,et al.  On the low‐frequency electrical polarization of bacterial cells in sands , 2005 .

[40]  C. Oldenburg,et al.  A mechanistic treatment of the dominant soil nitrogen cycling processes: Model development, testing, and application , 2008 .

[41]  Yuxin Wu,et al.  Electrical properties of iron-sand columns : Implications for induced polarization investigation and performance monitoring of iron-wall barriers , 2005 .

[42]  R. C. Bartholomay.  Mineralogical correlation of surficial sediment from area drainages with selected sedimentary interbeds at the Idaho National Engineering Laboratory, Idaho , 1990 .

[43]  Keith W. Jones,et al.  Synchrotron computed microtomography of porous media: Topology and transports. , 1994, Physical review letters.

[44]  Estella A. Atekwana,et al.  In-situ apparent conductivity measurements and microbial population distribution at a hydrocarbon-contaminated site , 2004 .

[45]  G. R. Olhoeft,et al.  Low-frequency electrical properties. , 1985 .

[46]  K. Williams,et al.  Feedbacks between hydrological heterogeneity and bioremediation induced biogeochemical transformations. , 2009, Environmental science & technology.

[47]  D. Lesmes,et al.  Influence of pore fluid chemistry on the complex conductivity and induced polarization responses of Berea sandstone , 2001 .

[48]  J. Wong,et al.  An electrochemical model of the induced‐polarization phenomenon in disseminated sulfide ores , 1979 .

[49]  R. Smith,et al.  Cation Exchange on Vadose Zone Research Park Subsurface Sediment, Idaho National Laboratory , 2010 .

[50]  Y. Fujita,et al.  Stimulation of microbial urea hydrolysis in groundwater to enhance calcite precipitation. , 2008, Environmental science & technology.

[51]  K. Williams,et al.  Geophysical imaging of stimulated microbial biomineralization. , 2005, Environmental science & technology.

[52]  M. P. Eastman,et al.  The coprecipitation of Sr2+ with calcite at 25°C and 1 atm , 1986 .

[53]  Clifton C. Casey,et al.  Geophysical Monitoring of a Field‐Scale Biostimulation Pilot Project , 2006, Ground water.