- Access by Xinjiang University
Effects of incomplete mixing on reactive transport in flows through heterogeneous porous media
Phys. Rev. Fluids 2, 114501 – Published 8 November, 2017
DOI: https://doi.org/10.1103/PhysRevFluids.2.114501
Abstract
The phenomenon of incomplete mixing reduces bulk effective reaction rates in reactive transport. Many existing models do not account for these effects, resulting in the overestimation of reaction rates in laboratory and field settings. To date, most studies on incomplete mixing have focused on diffusive systems; here, we extend these to explore the role that flow heterogeneity has on incomplete mixing. To do this, we examine reactive transport using a Lagrangian reactive particle tracking algorithm in two-dimensional idealized heterogeneous porous media. Contingent on the nondimensional Peclet and Damköhler numbers in the system, it was found that near well-mixed behavior could be observed at late times in the heterogeneous flow field simulations. We look at three common flow deformation metrics that describe the enhancement of mixing in the flow due to velocity gradients: the Okubo-Weiss parameter , the largest eigenvalue of the Cauchy-Green strain tensor , and the finite-time Lyapunov exponent . Strong mixing regions in the heterogeneous flow field identified by these metrics were found to correspond to regions with higher numbers of reactions, but the infrequency of these regions compared to the large numbers of reactions occurring elsewhere in the domain imply that these strong mixing regions are insufficient in explaining the observed near well-mixed behavior. Since it was found that reactive transport in these heterogeneous flows could overcome the effects of incomplete mixing, we also search for a closure for the mean concentration. The conservative quantity , where , was found to predict the late time scaling of the mean concentration, i.e., .
Physics Subject Headings (PhySH)
Article Text
References (58)
- P. Guerra, C. Gonzalez, C. Escauriaza, G. Pizarro, and P. Pasten, Incomplete mixing in the fate and transport of arsenic at a river affected by acid drainage, Water Air Soil Pollut. 227, 73 (2016).
- S. A. Levin and L. A. Segel, Hypothesis for origin of planktonic patchiness, Nature 259, 659 (1976).
- F. J. Molz and M. A. Widdowson, Internal inconsistencies in dispersion-dominated models that incorporate chemical and microbial kinetics, Water Resour. Res. 24, 615 (1988).
- M. Taillefert and J.-F. Gaillard, Reactive transport modeling of trace elements in the water column of a stratified lake: Iron cycling and metal scavenging, J. Hydrol. 256, 16 (2002).
- T. Tel, A. de Moura, C. Grebogi, and G. Karolyi, Chemical and biological activity in open flows: A dynamical system approach, Phys. Rep. 413, 91 (2005).
- C. M. Gramling, C. F. Harvey, and L. C. Meigs, Reactive transport in porous media: A comparison of model prediction with laboratory visualization, Environ. Sci. Technol. 36, 2508 (2002).
- V. Kapoor, C. T. Jafvert, and D. A. Lyn, Experimental study of a bimolecular reaction in Poiseuille flow, Water Resour. Res. 34, 1997 (1998).
- E. Monson and R. Kopelman, Observation of Laser Speckle Effects and Nonclassical Kinetics in an Elementary Chemical Reaction, Phys. Rev. Lett. 85, 666 (2000).
- E. Monson and R. Kopelman, Nonclassical kinetics of an elementary reaction-diffusion system showing effects of a speckled initial reactant distribution and eventual self-segregation: Experiments, Phys. Rev. E 69, 021103 (2004).
- D. S. Raje and V. Kapoor, Experimental study of bimolecular reaction kinetics in porous media, Environ. Sci. Technol. 34, 1234 (2000).
- G. Chiogna and A. Bellin, Analytical solution for reactive solute transport considering incomplete mixing within a reference elementary volume, Water Resour. Res. 49, 2589 (2013).
- Y. Edery, H. Scher, and B. Berkowitz, Particle tracking model of bimolecular reactive transport in porous media, Water Resour. Res. 46, W07524 (2010).
- Y. Edery, A. Guadagnini, H. Scher, and B. Berkowitz, Reactive transport in disordered media: Role of fluctuations in interpretation of laboratory experiments, Adv. Water Resour. 51, 86 (2013).
- X. Sanchez-Vila, D. Fernàndez-Garcia, and A. Guadagnini, Interpretation of column experiments of transport of solutes undergoing an irreversible bimolecular reaction using a continuum approximation, Water Resour. Res. 46, W12510 (2010).
- D. Bolster, P. de Anna, D. A. Benson, and A. M. Tartakovsky, Incomplete mixing and reactions with fractional dispersion, Adv. Water Resour. 37, 86 (2012).
- A. M. Tartakovsky, P. de Anna, T. Le Borgne, A. Balter, and D. Bolster, Effect of spatial concentration fluctuations on effective kinetics in diffusion-reaction systems, Water Resour. Res. 48, W02526 (2012).
- Z. Alhashmi, M. J. Blunt, and B. Bijeljic, Predictions of dynamic changes in reaction rates as a consequence of incomplete mixing using pore scale reactive transport modeling on images of porous media, J. Contam. Hydrol. 179, 171 (2015).
- D. Ding, D. A. Benson, A. Paster, and D. Bolster, Modeling bimolecular reactions and transport in porous media via particle tracking, Adv. Water Resour. 53, 56 (2013).
- C. Knutson, A. Valocchi, and C. Werth, Comparison of continuum and pore-scale models of nutrient biodegradation under transverse mixing conditions, Adv. Water Resour. 30, 1421 (2007).
- K. U. Mayer, S. G. Benner, and D. W. Blowes, Process-based reactive transport modeling of a permeable reactive barrier for the treatment of mine drainage, J. Contam. Hydrol. 85, 195 (2006).
- C. I. Steefel, D. J. DePaulo, and P. C. Lichtner, Reactive transport modeling: An essential tool and a new research approach for the Earth sciences, Earth Planet. Sci. Lett. 240, 539 (2005).
- D. T. Gillespie, Stochastic simulation of chemical kinetics, Annu. Rev. Phys. Chem. 58, 35 (2007).
- A. Paster, D. Bolster, and D. A. Benson, Connecting the dots: Semi-analytical and random walk numerical solutions of the diffusion-reaction equation with stochastic initial conditions, J. Comput. Phys. 263, 91 (2014).
- K. Kang and S. Redner, Scaling Approach for the Kinetics of Recombination Processes, Phys. Rev. Lett. 52, 955 (1984).
- A. A. Ovchinnikov and Ya. B. Zeldovich, Role of density fluctuations in bimolecular reaction kinetics, Chem. Phys. 28, 215 (1978).
- D. Toussaint and F. Wilczek, Particle—Antiparticle annihilation in diffusive motion, J. Chem. Phys. 78, 2642 (1983).
- S. A. Rice, Diffusion-Limited Reactions, Comprehensive Chemical Kinetics Vol. 25 (Elsevier, Amsterdam, 1985).
- E. Kotomin and V. Kuzovkov, Modern Aspects of Diffusion-Controlled Reactions: Cooperative Phenomena in Bimolecular Processes, Comprehensive Chemical Kinetics Vol. 34 (Elsevier, Amsterdam, 1996).
- J. D. Murray, Mathematical Biology: I. An Introduction (Springer, New York, 2002).
- D. Becherer and M. Schweizer, Classical solutions to reaction-diffusion systems for hedging problems with interacting Itô and point processes, Ann. Appl. Probab. 15, 1111 (2005).
- J. Fort and V. Mendéz, Reaction-diffusion waves of advance in the transition to agricultural economics, Phys. Rev. E 60, 5894 (1999).
- C.-Z. Li and K.-G. Löfgren, Renewable resources and economic sustainability: A dynamic analysis with heterogeneous time preferences, J. Environ. Econ. Manag. 40, 236 (2000).
- F. Schweitzer, Brownian Agents and Active Particles: Collective Dynamics in the Natural and Social Sciences (Springer, Berlin/Heidelberg, 2007).
- M. Dentz, T. Le Borgne, A. Englert, and B. Bijeljic, Mixing, spreading and reaction in heterogeneous media: A brief review, J. Contam. Hydrol. 120-121, 1 (2011).
- F. P. J. de Barros, M. Dentz, J. Koch, and W. Nowak, Flow topology and scalar mixing in spatially heterogeneous flow fields, Geophys. Res. Lett. 39, L08404 (2012).
- T. Le Borgne, M. Dentz, and E. Villermaux, Stretching, Coalescence, and Mixing in Porous Media, Phys. Rev. Lett. 110, 204501 (2013).
- S. W. Weeks and G. Sposito, Mixing and stretching efficiency in steady and unsteady groundwater flows, Water Resour. Res. 34, 3315 (1998).
- D. Bolster, M. Dentz, and T. Le Borgne, Hypermixing in linear shear flow, Water Resour. Res. 47, W09602 (2011).
- N. B. Engdahl, T. R. Ginn, and G. E. Fogg, Scalar dissipation rates in nonconservative transport systems, J. Contam. Hydrol. 149, 46 (2013).
- T. Le Borgne, M. Dentz, D. Bolster, J. Carrera, J.-R. de Dreuzy, and P. Davy, Non-Fickian mixing: Temporal evolution of the scalar dissipation rate in heterogeneous porous media, Adv. Water Resour. 33, 1468 (2010).
- P. K. Kitanidis, The concept of the dilution index, Water Resour. Res. 30, 2011 (1994).
- P. de Anna, J. Jimenez-Martinez, H. Tabuteau, R. Turuban, T. Le Borgne, M. Derrien, and Y. Méheust, Mixing and reaction kinetics in porous media: An experimental pore scale quantification, Environ. Sci. Technol. 48, 508 (2014).
- N. B. Engdahl, D. A. Benson, and D. Bolster, Predicting the enhancement of mixing-driven reactions in nonuniform flows using measures of flow topology, Phys. Rev. E 90, 051001 (2014).
- N. Kleinfelter, M. Moroni, and J. H. Cushman, Application of the finite-size Lyapunov exponent to particle tracking velocimetry in fluid mechanics experiments, Phys. Rev. E 72, 056306 (2005).
- A. Paster, T. Aquino, and D. Bolster, Incomplete mixing and reactions in laminar shear flow, Phys. Rev. E 92, 012922 (2015).
- D. A. Benson and M. M. Meerschaert, Simulation of chemical reaction via particle tracking: Diffusion-limited versus thermodynamic rate-limited regimes, Water Resour. Res. 44, W12201 (2008).
- A. Paster, D. Bolster, and D. A. Benson, Particle tracking and the diffusion-reaction equation, Water Resour. Res. 49, 1 (2013).
- D. A. Benson, T. Aquino, D. Bolster, N. Engdahl, C. V. Henri, and D. Fernàndez-Garcia, A comparison of Eulerian and Lagrangian transport and nonlinear reaction algorithms, Adv. Water Resour. 99, 15 (2017).
- D. A. Benson and D. Bolster, Arbitrarily complex chemical reactions on particles, Water Resour. Res. 52, 1 (2016).
- D. Bolster, A. Paster, and D. Benson, A particle number conserving Lagrangian method for mixing-driven reactive transport, Water Resour. Res. 52, 1 (2016).
- R. Ababou and L. W. Gelhar, in Dynamics of Fluids in Hierarchical Porous Media, edited by J. H. Cushman (Academic Press, San Diego, CA, 1990), Chap. 14.
- B. Zinn and C. F. Harvey, When good statistical models of aquifer heterogeneity go bad: A comparison of flow, dispersion, and mass transfer in connected and multivariate Gaussian hydraulic conductivity fields, Water Resour. Res. 39, 1051 (2003).
- A. Paster and D. Bolster, The effect of initial spatial correlations on late time kinetics of bimolecular irreversible reactions, Physica A 391, 4654 (2012).
- M. De Simoni, J. Carrera, X. Sánchez-Vila, and A. Guadagnini, A procedure for the solution of multicomponent reactive transport problems, Water Resour. Res. 41, W11410 (2005).
- G. Zumofen, J. Klafter, and M. F. Shlesinger, Breakdown of Ovchinnikov-Zeldovich Segregation in the Reaction under Levy Mixing, Phys. Rev. Lett. 77, 2830 (1996).
- G. Chiogna, M. Rolle, A. Bellin, and O. A. Cirpka, Helicity and flow topology in three-dimensional anisotropic porous media, Adv. Water Resour. 73, 134 (2014).
- G. Chiogna, O. A. Cirpka, M. Rolle, and A. Bellin, Helical flow in three-dimensional nonstationary anisotropic heterogeneous porous media, Water Resour. Res. 51, 261 (2015).
- O. A. Cirpka, G. Chiogna, M. Rolle, and A. Bellin, Transverse mixing in three-dimensional nonstationary anisotropic heterogeneous porous media, Water Resour. Res. 51, 241 (2015).