Tomographic Reservoir Imaging with DNA-Labeled Silica Nanotracers: The First Field Validation.

This study presents the first field validation of using DNA-labeled silica nanoparticles as tracers to image subsurface reservoirs by travel time based tomography. During a field campaign in Switzerland, we performed short-pulse tracer tests under a forced hydraulic head gradient to conduct a multisource-multireceiver tracer test and tomographic inversion, determining the two-dimensional hydraulic conductivity field between two vertical wells. Together with three traditional solute dye tracers, we injected spherical silica nanotracers, encoded with synthetic DNA molecules, which are protected by a silica layer against damage due to chemicals, microorganisms, and enzymes. Temporal moment analyses of the recorded tracer concentration breakthrough curves (BTCs) indicate higher mass recovery, less mean residence time, and smaller dispersion of the DNA-labeled nanotracers, compared to solute dye tracers. Importantly, travel time based tomography, using nanotracer BTCs, yields a satisfactory hydraulic conductivity tomogram, validated by the dye tracer results and previous field investigations. These advantages of DNA-labeled nanotracers, in comparison to traditional solute dye tracers, make them well-suited for tomographic reservoir characterizations in fields such as hydrogeology, petroleum engineering, and geothermal energy, particularly with respect to resolving preferential flow paths or the heterogeneity of contact surfaces or by enabling source zone characterizations of dense nonaqueous phase liquids.

[1]  P. Bayer,et al.  Field validation of thermal tracer tomography for reconstruction of aquifer heterogeneity , 2017 .

[2]  M Todd Walter,et al.  Hydrological tracers using nanobiotechnology: proof of concept. , 2012, Environmental science & technology.

[3]  J. Selker,et al.  Neutrally buoyant tracers in hydrogeophysics: Field demonstration in fractured rock , 2017 .

[4]  Robert N Grass,et al.  Silica-Encapsulated DNA-Based Tracers for Aquifer Characterization. , 2018, Environmental science & technology.

[5]  Stefan Uhlenbrook,et al.  Using multiple artificial DNA tracers in hydrology , 2011 .

[6]  P. Blum,et al.  Thermal tracer testing in a sedimentary aquifer: field experiment (Lauswiesen, Germany) and numerical simulation , 2014, Hydrogeology Journal.

[7]  W. Illman,et al.  Three-dimensional imaging of aquifer and aquitard heterogeneity via transient hydraulic tomography at a highly heterogeneous field site , 2018 .

[8]  S. Greenhalgh,et al.  Zonation for 3D aquifer characterization based on joint inversions of multimethod crosshole geophysical data , 2010 .

[9]  M. Saar,et al.  Quantifying magmatic, crustal, and atmospheric helium contributions to volcanic aquifers using all stable noble gases: Implications for magmatism and groundwater flow , 2005 .

[10]  P. Bayer,et al.  Travel-time-based thermal tracer tomography , 2016 .

[11]  S. Smith,et al.  Single-molecule studies of DNA mechanics. , 2000, Current opinion in structural biology.

[12]  Liping Pang,et al.  Tracking effluent discharges in undisturbed stony soil and alluvial gravel aquifer using synthetic DNA tracers. , 2017, The Science of the total environment.

[13]  Albert J. Valocchi,et al.  Validity of the local equilibrium assumption for modeling sorbing solute transport through homogeneous soils , 1985 .

[14]  Mary P Anderson,et al.  Heat as a Ground Water Tracer , 2005, Ground water.

[15]  James J. Butler,et al.  Pumping tests in networks of multilevel sampling wells: Motivation and methodology , 1999 .

[16]  Robert N Grass,et al.  Magnetically recoverable, thermostable, hydrophobic DNA/silica encapsulates and their application as invisible oil tags. , 2014, ACS nano.

[17]  C. V. Theis The relation between the lowering of the Piezometric surface and the rate and duration of discharge of a well using ground‐water storage , 1935 .

[18]  P. Bayer,et al.  Time-lapse pressure tomography for characterizing CO2 plume evolution in a deep saline aquifer , 2015 .

[19]  Gregoire Mariethoz,et al.  Smart pilot points using reversible‐jump Markov‐chain Monte Carlo , 2016 .

[20]  J. Vanderzalm,et al.  Unraveling the complexities of the velocity dependency of E. coli retention and release parameters in saturated porous media. , 2017, The Science of the total environment.

[21]  Junfeng Zhu,et al.  Analysis of tracer tomography using temporal moments of tracer breakthrough curves , 2009 .

[22]  P. Bayer,et al.  A new sequential procedure for hydraulic tomographic inversion , 2013 .

[23]  Thomas Ptak,et al.  Tracer tests for the investigation of heterogeneous porous media and stochastic modelling of flow and transport—a review of some recent developments , 2004 .

[24]  Robert N Grass,et al.  Reversible DNA encapsulation in silica to produce ROS-resistant and heat-resistant synthetic DNA 'fossils' , 2013, Nature Protocols.

[25]  P. Smart,et al.  An evaluation of some fluorescent dyes for water tracing , 1977 .

[26]  B. Vinther,et al.  Memory effect in deuterium analysis by continuous flow isotope ratio measurement , 2006 .

[27]  Thom Bogaard,et al.  Development of a methodology for the application of synthetic DNA in stream tracer injection experiments , 2013 .

[28]  C. A. Mora,et al.  DNA‐Based Sensor Particles Enable Measuring Light Intensity in Single Cells , 2016, Advanced materials.

[29]  C. E. Jacob,et al.  A generalized graphical method for evaluating formation constants and summarizing well‐field history , 1946 .

[30]  Walter A Illman,et al.  Hydraulic/partitioning tracer tomography for DNAPL source zone characterization: small-scale sandbox experiments. , 2010, Environmental science & technology.

[31]  M. Saar,et al.  Effects of permeability fields on fluid, heat, and oxygen isotope transport in extensional detachment systems , 2013 .

[32]  Lucia Aquilanti,et al.  A DNA tracer used in column tests for hydrogeology applications , 2013, Environmental Earth Sciences.

[33]  M. Saar,et al.  Process length scales and longitudinal damping in karst conduits , 2012 .

[34]  Tammo S. Steenhuis,et al.  Quantifying Preferential Flow by Breakthrough of Sequentially Applied Tracers Silt Loam Soil , 2000 .

[35]  Heileen Hsu-Kim,et al.  Influence of dissolved organic matter on the environmental fate of metals, nanoparticles, and colloids. , 2011, Environmental science & technology.

[36]  M. Saar,et al.  Depth dependence of permeability in the Oregon cascades inferred from hydrogeologic, thermal, seismic, and magmatic modeling constraints , 2004 .

[37]  Peter Aleström,et al.  Synthetic DNA tracers: examples of their application in water related studies. , 2000 .

[38]  T. Schuetz,et al.  Multi-tracer experiments to characterise contaminant mitigation capacities for different types of artificial wetlands , 2011 .

[39]  S. Haldorsen,et al.  Use of Synthetic DNA as New Tracers for Tracing Groungwater Flow and Multiple Contaminants , 2001 .

[40]  N. Weisbrod,et al.  The use of fluorescent dyes as tracers in highly saline groundwater , 2008 .

[41]  S. Walsh,et al.  Macroscale lattice‐Boltzmann methods for low Peclet number solute and heat transport in heterogeneous porous media , 2010 .

[42]  Wendelin J. Stark,et al.  Silica particles with encapsulated DNA as trophic tracers , 2015, Molecular ecology resources.

[43]  P. Kitanidis,et al.  Hydraulic conductivity imaging from 3‐D transient hydraulic tomography at several pumping/observation densities , 2013 .

[44]  Martin O. Saar,et al.  Review: Geothermal heat as a tracer of large-scale groundwater flow and as a means to determine permeability fields , 2011 .

[45]  W. Stark,et al.  Tracking Trace Amounts of Submicrometer Silica Particles in Wastewaters and Activated Sludge Using Silica-Encapsulated DNA Barcodes , 2014 .

[46]  Steve W. Lyon,et al.  Using concurrent DNA tracer injections to infer glacial flow pathways , 2015 .

[47]  B. Lowery,et al.  Bromide and chloride tracer application to determine sufficiency of plot size and well depth placement to capture preferential flow and solute leaching , 2016 .

[48]  S. Davis,et al.  Ground‐Water Tracers — A Short Review , 1980 .

[49]  Matthew M. Winkler,et al.  DNA-labeled clay: A sensitive new method for tracing particle transport , 1998 .

[50]  Niklas Linde,et al.  3D crosshole ERT for aquifer characterization and monitoring of infiltrating river water , 2011 .

[51]  Tian-Chyi J. Yeh,et al.  Hydraulic/partitioning tracer tomography for characterization of dense nonaqueous phase liquid source zones , 2007 .

[52]  Cheng-Haw Lee,et al.  Time to Change the Way We Collect and Analyze Data for Aquifer Characterization , 2007, Ground water.

[53]  H. Gvirtzman,et al.  A 3‐D hydrologic transport model of a water recharge system using carbamazepine and chloride as tracers , 2014 .

[54]  J. Kirchner,et al.  Catchment-scale advection and dispersion as a mechanism for fractal scaling in stream tracer concentrations , 2001 .

[55]  Hiromitsu Saegusa,et al.  Hydraulic tomography in fractured granite: Mizunami Underground Research site, Japan , 2009 .

[56]  Samuel Diem,et al.  Räumliche Charakterisierung der hydraulischen Leitfähigkeit in alluvialen Schotter-Grundwasserleitern: Ein Methodenvergleich , 2010 .

[57]  M. Weiler,et al.  Tracking water pathways in steep hillslopes by δ18O depth profiles of soil water , 2014 .

[58]  Shibo Wang,et al.  Wettability phenomena at the CO2-brine-mineral interface: implications for geologic carbon sequestration. , 2013, Environmental science & technology.

[59]  Peiling Yang,et al.  A DNA Tracer System for Hydrological Environment Investigations. , 2018, Environmental science & technology.

[60]  M. Saar,et al.  Three thousand years of extreme rainfall events recorded in stalagmites from Spring Valley Caverns, Minnesota , 2010 .

[61]  M. Field Assessing Aquatic Ecotoxicological Risks Associated with Fluorescent Dyes Used for Water-Tracing Studies , 2005 .

[62]  Arturo A. Keller,et al.  Transport of colloids in saturated porous media: A pore‐scale observation of the size exclusion effect and colloid acceleration , 2003 .

[63]  Thermal damping and retardation in karst conduits , 2014 .

[64]  G. Böhm,et al.  A laboratory study of tracer tomography , 2013, Hydrogeology Journal.

[65]  Scott C Alexander,et al.  Improved Characterization of Small “u” for Jacob Pumping Test Analysis Methods , 2012, Ground water.

[66]  Akhil Datta-Gupta,et al.  Asymptotic solutions for solute transport: A formalism for tracer tomography , 1999 .

[67]  C. Leibundgut,et al.  Tracers in Hydrology , 2009 .

[68]  Peter Aleström,et al.  DNA tracers with information capacity and high detection sensitivity tested in groundwater studies , 1999 .

[69]  Peter Dietrich,et al.  Rapid field application of hydraulic tomography for resolving aquifer heterogeneity in unconsolidated sediments , 2013 .

[70]  Walter A. Illman,et al.  Three‐dimensional transient hydraulic tomography in a highly heterogeneous glaciofluvial aquifer‐aquitard system , 2011 .