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Characterizing Reactive Transport Behavior in a Three-Dimensional Discrete Fracture Network

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Abstract

While several studies have linked network and in-fracture scale properties to conservative transport behavior in subsurface fractured media, studies on reactive transport cases remain relatively underdeveloped. In this study, we explore the behavior of an irreversible kinetic reaction during the interaction of two solute plumes, one consisting of species A and the other species B. When the plumes converge, these species react kinetically to form a new species C via \(A+B\xrightarrow {k} C\). This reactive system is studied using a three-dimensional discrete fracture network (DFN) model coupled with reactive Lagrangian particle tracking. We find that the interplay of network topology and chemical properties of the reactive solutes controls reactive transport processes. The network topology drives species A and B together, and the chemical properties dictate whether and how quickly a reaction occurs. Results demonstrate that reactions are most likely to occur in high-velocity fractures that make up the network backbone. The interplay between species’ chemical properties and transport is characterized by a non-dimensional Damköhler (Da) number. We show that the spatial distribution of reactions is sensitive to Da, which subsequently influences late-time tailing behavior in outlet breakthrough time distributions. The results of this study provide initial insights into how an irreversible reaction occurs during transport in a fracture network, using a methodology that can be applied to study reactive transport in a wide range of fractured media environments and contexts.

Article Highlights

  • Discrete Fracture Network models are used to study reactive transport behavior.

  • We consider the irreversible chemical reaction A + B → C

  • Reactions primarily occur in the network backbone and reaction locations are sensitive to chemical properties.

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Acknowledgements

D.B’s portion of this work was supported by the US Army Research Office under Contract/Grant number W911NF-18-1-0338. M.R.S. and J.D.H. thank the Department of Energy (DOE) Basic Energy Sciences program (LANLE3W1) for support. M.R.S. would like to thank the Center for Nonlinear Studies for support. M.R.S. and J.D.H. also gratefully acknowledge support from the LANL LDRD program office Grant Number #20180621ECR. Los Alamos National Laboratory is operated by Triad National Security, LLC, for the National Nuclear Security Administration of US Department of Energy (Contract No. 89233218CNA000001). dfnWorks is open source software and can be obtained at https://github.com/lanl/dfnWorks LA-UR-20-26548.

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Authors and Affiliations

  1. FTS International LLC, Dulles, VA, USA

    Thomas Sherman

  2. Division of Environmental Research, CRCL Solutions LLC, Louisville, KY, USA

    Thomas Sherman & Daniel Vassallo

  3. Energy Geosciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Guillem Sole-Mari

  4. Department of Civil and Environmental Engineering, Universitat Politècnica de Catalunya, Barcelona, Spain

    Guillem Sole-Mari

  5. Computational Earth Science Group (EES-16), Earth and Environmental Sciences Division, Los Alamos National Laboratory, Los Alamos, NM, 87545, USA

    Jeffrey Hyman & Matthew R. Sweeney

  6. Center for Nonlinear Studies, Theoretical Division, Los Alamos National Laboratory, Los Alamos, NM, 87545, USA

    Matthew R. Sweeney

  7. Department of Civil and Environmental Engineering and Earth Sciences, University of Notre Dame, Notre Dame, IN, USA

    Daniel Vassallo & Diogo Bolster

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  1. Thomas Sherman
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Sherman, T., Sole-Mari, G., Hyman, J. et al. Characterizing Reactive Transport Behavior in a Three-Dimensional Discrete Fracture Network. Transp Porous Med 146, 307–327 (2023). https://doi.org/10.1007/s11242-021-01568-4

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