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Title: Pore-scale study of multiphase reactive transport in fibrous electrodes of vanadium redox flow batteries

Abstract

The electrode of a vanadium redox flow battery generally is a carbon fibre-based porous medium, in which important physicochemical processes occur. In this work, pore-scale simulations are performed to study complex multiphase flow and reactive transport in the electrode by using the lattice Boltzmann method (LBM). Four hundred fibrous electrodes with different fibre diameters and porosities are reconstructed. Both the permeability and diffusivity of the reconstructed electrodes are predicted and compared with empirical relationships in the literature. Reactive surface area of the electrodes is also evaluated and it is found that existing empirical relationship overestimates the reactive surface under lower porosities. Further, a pore-scale electrochemical reaction model is developed to study the effects of fibre diameter and porosity on electrolyte flow, V II/V III transport, and electrochemical reaction at the electrolyte-fibre surface. Finally, evolution of bubble cluster generated by the side reaction is studied by adopting a LB multiphase flow model. Effects of porosity, fibre diameter, gas saturation and solid surface wettability on average bubble diameter and reduction of reactive surface area due to coverage of bubbles on solid surface are investigated in detail. It is found that gas coverage ratio is always lower than that adopted in the continuummore » model in the literature. Furthermore, the current pore-scale studies successfully reveal the complex multiphase flow and reactive transport processes in the electrode, and the simulation results can be further upscaled to improve the accuracy of the current continuum-scale models.« less

Authors:
 [1];  [2];  [2]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [3]
  1. Xi'an Jiaotong Univ., Shaanxi (China); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Xi'an Jiaotong Univ., Shaanxi (China)
  3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1374359
Report Number(s):
LA-UR-17-25691
Journal ID: ISSN 0013-4686
Grant/Contract Number:
AC52-06NA25396
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Electrochimica Acta
Additional Journal Information:
Journal Volume: 248; Journal Issue: C; Journal ID: ISSN 0013-4686
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 25 ENERGY STORAGE; Energy Sciences

Citation Formats

Chen, Li, He, YaLing, Tao, Wen -Quan, Zelenay, Piotr, Mukundan, Rangachary, and Kang, Qinjun. Pore-scale study of multiphase reactive transport in fibrous electrodes of vanadium redox flow batteries. United States: N. p., 2017. Web. doi:10.1016/j.electacta.2017.07.086.
Chen, Li, He, YaLing, Tao, Wen -Quan, Zelenay, Piotr, Mukundan, Rangachary, & Kang, Qinjun. Pore-scale study of multiphase reactive transport in fibrous electrodes of vanadium redox flow batteries. United States. doi:10.1016/j.electacta.2017.07.086.
Chen, Li, He, YaLing, Tao, Wen -Quan, Zelenay, Piotr, Mukundan, Rangachary, and Kang, Qinjun. 2017. "Pore-scale study of multiphase reactive transport in fibrous electrodes of vanadium redox flow batteries". United States. doi:10.1016/j.electacta.2017.07.086.
@article{osti_1374359,
title = {Pore-scale study of multiphase reactive transport in fibrous electrodes of vanadium redox flow batteries},
author = {Chen, Li and He, YaLing and Tao, Wen -Quan and Zelenay, Piotr and Mukundan, Rangachary and Kang, Qinjun},
abstractNote = {The electrode of a vanadium redox flow battery generally is a carbon fibre-based porous medium, in which important physicochemical processes occur. In this work, pore-scale simulations are performed to study complex multiphase flow and reactive transport in the electrode by using the lattice Boltzmann method (LBM). Four hundred fibrous electrodes with different fibre diameters and porosities are reconstructed. Both the permeability and diffusivity of the reconstructed electrodes are predicted and compared with empirical relationships in the literature. Reactive surface area of the electrodes is also evaluated and it is found that existing empirical relationship overestimates the reactive surface under lower porosities. Further, a pore-scale electrochemical reaction model is developed to study the effects of fibre diameter and porosity on electrolyte flow, VII/VIII transport, and electrochemical reaction at the electrolyte-fibre surface. Finally, evolution of bubble cluster generated by the side reaction is studied by adopting a LB multiphase flow model. Effects of porosity, fibre diameter, gas saturation and solid surface wettability on average bubble diameter and reduction of reactive surface area due to coverage of bubbles on solid surface are investigated in detail. It is found that gas coverage ratio is always lower than that adopted in the continuum model in the literature. Furthermore, the current pore-scale studies successfully reveal the complex multiphase flow and reactive transport processes in the electrode, and the simulation results can be further upscaled to improve the accuracy of the current continuum-scale models.},
doi = {10.1016/j.electacta.2017.07.086},
journal = {Electrochimica Acta},
number = C,
volume = 248,
place = {United States},
year = 2017,
month = 7
}

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  • In the subsurface fluids play a critical role by transporting dissolved minerals, colloids and contaminants (sometimes over long distances), by mediating dissolution and precipitation processes and enabling chemical transformations in solution and at mineral surfaces. Although the complex geometries of fracture apertures, fracture networks and pore spaces may make it difficult to accurately predict fluid flow in saturated (single-phase) subsurface systems, well developed methods are available. The simulation of multiphase fluid flow in the subsurface is much more challenging because of the large density and/or viscosity ratios found in important applications (water/air in the vadose zone, water/oil, water/gas, gas/oil andmore » water/oil/gas in oil reservoirs, water/air/non-aqueous phase liquids (NAPL) in contaminated vadose zone systems and gas/molten rock in volcanic systems, for example). In addition, the complex behavior of fluid-fluid-solid contact lines, and its impact on dynamic contact angles, must also be taken into account, and coupled with the fluid flow. Pore network models and simple statistical physics based models such as the invasion percolation and diffusion-limited aggregation models have been used quite extensively. However, these models for multiphase fluid flow are based on simplified models for pore space geometries and simplified physics. Other methods such a lattice Boltzmann and lattice gas models, molecular dynamics, Monte Carlo methods, and particle methods such as dissipative particle dynamics and smoothed particle hydrodynamics are based more firmly on first principles, and they do not require simplified pore and/or fracture geometries. However, they are less (in some cases very much less) computationally efficient that pore network and statistical physics models. Recently a combination of continuum computation fluid dynamics, fluid-fluid interface tracking or capturing and simple models for the dependence of contact angles on fluid velocity at the contact line has been used to simulate multiphase fluid flow in fracture apertures, fracture networks and pore spaces. Fundamental conservation principles - conservation of momentum, and conservation of mass (or conservation of volume for incompressible fluids) and conservation of energy, as well as symmetries (Galilean invariance and isotropy) are central to the physics of fluids and the models used to simulate them. In molecular and mesoscale models observance of these conservation principles and symmetries at the microscopic level leads to macroscopic fluid dynamics that can be represented by the Navier Stokes equation. The remarkable fact that the flow of all simpe fluids, irrespective of their chemical nature, can be described by the Navier-Stokes equation is a result of these conservation principles and symmetries acting on the molecular level.« less
  • In the subsurface fluids play a critical role by transporting dissolved minerals, colloids and contaminants (sometimes over long distances), by mediating dissolution and precipitation processes and enabling chemical transformations in solution and at mineral surfaces. Although the complex geometries of fracture apertures, fracture networks and pore spaces may make it difficult to accurately predict fluid flow in saturated (single-phase) subsurface systems, well developed methods are available. The simulation of multiphase fluid flow in the subsurface is much more challenging because of the large density and/or viscosity ratios found in important applications (water/air in the vadose zone, water/oil, water/gas, gas/oil andmore » water/oil/gas in oil reservoirs, water/air/non-aqueous phase liquids (NAPL) in contaminated vadose zone systems and gas/molten rock in volcanic systems, for example). In addition, the complex behavior of fluid-fluid-solid contact lines, and its impact on dynamic contact angles, must also be taken into account, and coupled with the fluid flow. Pore network models and simple statistical physics based models such as the invasion percolation and diffusion-limited aggregation models have been used quite extensively. However, these models for multiphase fluid flow are based on simplified models for pore space geometries and simplified physics. Other methods such a lattice Boltzmann and lattice gas models, molecular dynamics, Monte Carlo methods, and particle methods such as dissipative particle dynamics and smoothed particle hydrodynamics are based more firmly on first principles, and they do not require simplified pore and/or fracture geometries. However, they are less (in some cases very much less) computationally efficient that pore network and statistical physics models. Recently a combination of continuum computation fluid dynamics, fluid-fluid interface tracking or capturing and simple models for the dependence of contact angles on fluid velocity at the contact line has been used to simulate multiphase fluid flow in fracture apertures, fracture networks and pore spaces. Fundamental conservation principles - conservation of momentum, and conservation of mass (or conservation of volume for incompressible fluids) and conservation of energy, as well as symmetries (Galilean invariance and isotropy) are central to the physics of fluids and the models used to simulate them. In molecular and mesoscale models observance of these conservation principles and symmetries at the microscopic level leads to macroscopic fluid dynamics that can be represented by the Navier Stokes equation. The remarkable fact that the flow of all simpe fluids, irrespective of their chemical nature, can be described by the Navier-Stokes equation is a result of these conservation principles and symmetries acting on the molecular level.« less