Multicomponent Gas Diffusion in Porous Electrodes

Multicomponent gas transport is investigated with unprecedented precision by AC impedance analysis of porous YSZ anodesupported solid oxide fuel cells. A fuel gas mixture of H2-H2O-N2 is fed to the anode, and impedance data are measured across the range of hydrogen partial pressure (10–100%) for open circuit conditions at three temperatures (800◦C, 850◦C and 900◦C) and for 300 mA applied current at 800◦C. For the first time, analytical formulae for the diffusion resistance (Rb) of three standard models of multicomponent gas transport (Fick, Stefan-Maxwell, and Dusty Gas) are derived and tested against the impedance data. The tortuosity is the only fitting parameter since all the diffusion coefficients are known. Only the Dusty Gas Model leads to a remarkable data collapse for over twenty experimental conditions, using a constant tortuosity consistent with permeability measurements and the Bruggeman relation. These results establish the accuracy of the Dusty Gas Model for multicomponent gas diffusion in porous media and confirm the efficacy of electrochemical impedance analysis to precisely determine transport mechanisms. © The Author(s) 2015. Published by ECS. This is an open access article distributed under the terms of the Creative Commons Attribution 4.0 License (CC BY, http://creativecommons.org/licenses/by/4.0/), which permits unrestricted reuse of the work in any medium, provided the original work is properly cited. [DOI: 10.1149/2.0911506jes] All rights reserved.

[1]  Ioannis K. Kookos On the diffusion in porous electrodes of SOFCs , 2012 .

[2]  Ioannis K. Kookos,et al.  Modelling mass transport in solid oxide fuel cell anodes: a case for a multidimensional dusty gas-based model , 2008 .

[3]  W. V. Swaaij,et al.  Effects of intraparticle heat and mass transfer during devolatilization of a single coal particle , 1985 .

[4]  F. Hamdullahpur,et al.  Micro‐modeling of porous composite anodes for solid oxide fuel cells , 2012 .

[5]  C. Geankoplis,et al.  Ternary diffusion of gases in capillaries in the transition region between knudsen and molecular diffusion , 1974 .

[6]  Ellen Ivers-Tiffée,et al.  Evaluation and Modeling of the Cell Resistance in Anode-Supported Solid Oxide Fuel Cells , 2008 .

[7]  Chih‐Long Tsai,et al.  Tortuosity in anode-supported proton conductive solid oxide fuel cell found from current flow rates and dusty-gas model , 2011 .

[8]  D. Jeon,et al.  A comprehensive micro-scale model for transport and reaction in intermediate temperature solid oxide fuel cells , 2006 .

[9]  I. Celik,et al.  On modeling multi-component diffusion inside the porous anode of solid oxide fuel cells using Fick's model , 2009 .

[10]  S. Singhal,et al.  Polarization Effects in Intermediate Temperature, Anode‐Supported Solid Oxide Fuel Cells , 1999 .

[11]  R. Kee,et al.  Modeling Electrochemical Impedance Spectra in SOFC Button Cells with Internal Methane Reforming , 2006 .

[12]  L. A. Chick,et al.  Diffusion Limitations in the Porous Anodes of SOFCs , 2003 .

[13]  Chih-Long Tsai,et al.  Anode-pore tortuosity in solid oxide fuel cells found from gas and current flow rates , 2008 .

[14]  A. Virkar,et al.  Fuel Composition and Diluent Effect on Gas Transport and Performance of Anode-Supported SOFCs , 2003 .

[15]  Fausto Arpino,et al.  Numerical simulation of mass and energy transport phenomena in solid oxide fuel cells , 2009 .

[16]  Stefan-Maxwell mass transport , 2009 .

[17]  J. B. Young,et al.  Diffusion and Chemical Reaction in the Porous Structures of Solid Oxide Fuel Cells , 2006 .

[18]  E. A. Mason,et al.  Gas Transport in Porous Media: The Dusty-Gas Model , 1983 .

[19]  Wilson K. S. Chiu,et al.  A review of modeling and simulation techniques across the length scales for the solid oxide fuel cell , 2012 .

[20]  Nieck E. Benes,et al.  comparison of macro and microscopic theories describing multicomponent mass transport in microporous media , 1999 .

[21]  Rajamani Krishna,et al.  A simplified procedure for the solution of the dusty gas model equations for steady-state transport in non-reacting systems , 1987 .

[22]  W. E. Stewart,et al.  Multicomponent Diffusion of Gases in Porous Solids. Models and Experiments , 1974 .

[23]  Stefano Ubertini,et al.  Modeling solid oxide fuel cell operation: Approaches, techniques and results , 2006 .

[24]  R. Jackson,et al.  Pressure gradients in porous catalyst pellets in the intermediate diffusion regime , 1977 .

[25]  Jon M. Hiller,et al.  Three-dimensional reconstruction of a solid-oxide fuel-cell anode , 2006, Nature materials.

[26]  Martin Z. Bazant,et al.  Nonequilibrium Thermodynamics of Porous Electrodes , 2012, 1204.2934.

[27]  R. Jackson,et al.  Transport in porous catalysts , 1977 .

[28]  Mogens Bjerg Mogensen,et al.  Gas Conversion Impedance: A Test Geometry Effect in Characterization of Solid Oxide Fuel Cell Anodes , 1998 .

[29]  Edward L Cussler,et al.  Diffusion: Mass Transfer in Fluid Systems , 1984 .

[30]  Mark E. Davis,et al.  Analysis of SO2 oxidation in non-isothermal catalyst pellets using the dusty-gas model , 1982 .

[31]  Communications on the theory of diffusion and reaction — IX. Internal pressure and forced flow for reactions with volume change , 1973 .

[32]  M. Fowler,et al.  Performance comparison of Fick’s, dusty-gas and Stefan–Maxwell models to predict the concentration overpotential of a SOFC anode , 2003 .

[33]  Norman Epstein,et al.  On tortuosity and the tortuosity factor in flow and diffusion through porous media , 1989 .

[34]  Lin Ma,et al.  Comparison of the multicomponent mass transfer models for the prediction of the concentration overpotential for solid oxide fuel cell anodes , 2010 .

[35]  Nieck E. Benes,et al.  Numerical scheme for simulating multicomponent mass transport accompanied by reversible chemical reactions in porous media , 1999 .

[36]  Norberto Fueyo,et al.  Multimodal mass transfer in solid-oxide fuel-cells. , 2010 .

[37]  Norberto Fueyo,et al.  Mass transfer in hydrogen-fed anode-supported SOFCs , 2010 .

[38]  H. Chandra,et al.  Application of solid oxide fuel cell technology for power generation—A review , 2013 .

[39]  R. Krishna,et al.  The Maxwell-Stefan approach to mass transfer , 1997 .

[40]  Wilson K. S. Chiu,et al.  Nondestructive Reconstruction and Analysis of SOFC Anodes Using X-ray Computed Tomography at Sub-50 nm Resolution , 2008 .

[41]  Heterogeneous electrocatalysis in porous cathodes of solid oxide fuel cells , 2014, 1412.1548.

[42]  L. A. Chick,et al.  Factors affecting limiting current in solid oxide fuel cells or debunking the myth of anode diffusion polarization , 2011 .

[43]  Mogens Bjerg Mogensen,et al.  Gas Diffusion Impedance in Characterization of Solid Oxide Fuel Cell Anodes , 1999 .

[44]  K. Yoon,et al.  Analysis of Electrochemical Performance of SOFCs Using Polarization Modeling and Impedance Measurements , 2009 .

[45]  On the modified Stefan–Maxwell equation for isothermal multicomponent gaseous diffusion , 2006 .

[46]  M. Soroush,et al.  Mathematical modeling of solid oxide fuel cells: A review , 2011 .

[47]  J. Vohs,et al.  An Investigation of Oxygen Reduction Kinetics in LSF Electrodes , 2013 .

[48]  W. Lehnert,et al.  Structural properties of SOFC anodes and reactivity , 1998 .

[49]  Ian David Lockhart Bogle,et al.  Computers and Chemical Engineering , 2008 .

[50]  G. M. Watson,et al.  Gaseous Diffusion in Porous Media at Uniform Pressure , 1961 .