The filamentary structure of mixing fronts and its control on reaction kinetics in porous media flows

The mixing dynamics resulting from the combined action of diffusion, dispersion, and advective stretching of a reaction front in heterogeneous flows leads to reaction kinetics that can differ by orders of magnitude from those measured in well-mixed batch reactors. The reactive fluid invading a porous medium develops a filamentary or lamellar front structure. Fluid deformation leads to an increase of the front length by stretching and consequently a decrease of its width by compression. This advective front deformation, which sharpens concentration gradients across the interface, is in competition with diffusion, which tends to increase the interface width and thus smooth concentration gradients. The lamella scale dynamics eventually develop into a collective behavior through diffusive coalescence, which leads to a disperse interface whose width is controlled by advective dispersion. We derive a new approach that quantifies the impact of these filament scale processes on the global mixing and reaction kinetics. The proposed reactive filament model, based on the elementary processes of stretching, coalescence, and fluid particle dispersion, provides a new framework for predicting reaction front kinetics in heterogeneous flows.

[1]  M. Dentz,et al.  Transport‐controlled reaction rates under local non‐equilibrium conditions , 2007 .

[2]  Timothy D. Scheibe,et al.  A smoothed particle hydrodynamics model for reactive transport and mineral precipitation in porous and fractured porous media , 2007 .

[3]  Colin Neal,et al.  Universal fractal scaling in stream chemistry and its implications for solute transport and water quality trend detection , 2013, Proceedings of the National Academy of Sciences.

[4]  E. Villermaux,et al.  Mixing by random stirring in confined mixtures , 2008, Journal of Fluid Mechanics.

[5]  Patrick J. Fox,et al.  A pore‐scale numerical model for flow through porous media , 1999 .

[6]  B. Jamtveit,et al.  Reaction enhanced permeability during retrogressive metamorphism , 2008 .

[7]  S. Whitaker The method of volume averaging , 1998 .

[8]  J. Ottino The Kinematics of Mixing: Stretching, Chaos, and Transport , 1989 .

[9]  C. Harvey,et al.  Reactive transport in porous media: a comparison of model prediction with laboratory visualization. , 2002, Environmental science & technology.

[10]  Lincoln Paterson,et al.  Role of Convective Mixing in the Long-Term Storage of Carbon Dioxide in Deep Saline Formations , 2005 .

[11]  Olivier Bour,et al.  Persistence of incomplete mixing: a key to anomalous transport. , 2011, Physical review. E, Statistical, nonlinear, and soft matter physics.

[12]  François Renard,et al.  Self‐organization during reactive fluid flow in a porous medium , 1998 .

[13]  Application of the finite-size Lyapunov exponent to particle tracking velocimetry in fluid mechanics experiments. , 2005, Physical review. E, Statistical, nonlinear, and soft matter physics.

[14]  J. Jiménez,et al.  Fractal interfaces and product generation in the two‐dimensional mixing layer , 1991 .

[15]  Tanguy Le Borgne,et al.  Stretching, coalescence, and mixing in porous media. , 2013, Physical review letters.

[16]  P. Meakin,et al.  Fracture patterns generated by diffusion controlled volume changing reactions. , 2006, Physical review letters.

[17]  Scott Fendorf,et al.  Processes conducive to the release and transport of arsenic into aquifers of Bangladesh. , 2005, Proceedings of the National Academy of Sciences of the United States of America.

[18]  Daniel M. Tartakovsky,et al.  On breakdown of macroscopic models of mixing-controlled heterogeneous reactions in porous media , 2009 .

[19]  E. Villermaux,et al.  How vortices mix , 2003, Journal of Fluid Mechanics.

[20]  Roman Stocker,et al.  Gyrotaxis in a steady vortical flow. , 2011, Physical review letters.

[21]  Alexandre M Tartakovsky,et al.  Flow intermittency, dispersion, and correlated continuous time random walks in porous media. , 2013, Physical review letters.

[22]  Tanguy Le Borgne,et al.  Mixing and reaction kinetics in porous media: an experimental pore scale quantification. , 2014, Environmental science & technology.

[23]  Emmanuel Villermaux,et al.  Mixing by porous media , 2012 .

[24]  Mathieu Sebilo,et al.  Long-term fate of nitrate fertilizer in agricultural soils , 2013, Proceedings of the National Academy of Sciences.

[25]  Timothy D. Scheibe,et al.  EFFECTS OF INCOMPLETE MIXING ON MULTICOMPONENT REACTIVE TRANSPORT , 2009 .

[26]  Tanguy Le Borgne,et al.  Lagrangian statistical model for transport in highly heterogeneous velocity fields. , 2008, Physical review letters.

[27]  E Villermaux,et al.  Mixing as an aggregation process. , 2001, Physical review letters.

[28]  H. Herzog,et al.  Lifetime of carbon capture and storage as a climate-change mitigation technology , 2012, Proceedings of the National Academy of Sciences.

[29]  J. Bear Dynamics of Fluids in Porous Media , 1975 .

[30]  Peter K. Kitanidis,et al.  The concept of the Dilution Index , 1994 .

[31]  Emmanuel Villermaux,et al.  A nonsequential turbulent mixing process , 2010 .

[32]  W. Ranz Applications of a stretch model to mixing, diffusion, and reaction in laminar and turbulent flows , 1979 .

[33]  Dennis A. Lyn,et al.  Experimental study of a bimolecular reaction in Poiseuille Flow , 1998 .

[34]  Emilio Hernández-García,et al.  Chemical and Biological Processes in Fluid Flows: A Dynamical Systems Approach , 2009 .

[35]  Andreas Englert,et al.  Mixing, spreading and reaction in heterogeneous media: a brief review. , 2011, Journal of contaminant hydrology.

[36]  A. Wit Fingering of Chemical Fronts in Porous Media , 2001 .