Electrochemical Engine Center
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1 Electrochemical Engine Center Computational Fuel Cell Research and SOFC Modeling at Penn State Chao-Yang Wang Professor of Mechanical Engineering, and Materials Science & Engineering Director, Electrochemical Engine Center (ECEC) The Pennsylvania State University University Park, PA USA Presented at NASA Solid Oxide Fuel Cell Modeling and Simulation Workshop NASA Glenn Research Center, April 11, 2003 URL: mtrl1.me.psu.edu
2 Outline Overview ECEC Computational Modeling of PEM Fuel Cells SOFC Modeling & Simulation Fuel Cell Controls Summary
3 ECEC Overview Vision: provide fuel cell science & technology for sustainable energy future Mission: organize and conduct multidisciplinary research on fuel cells and advanced batteries for vehicle propulsion, distributed power generation and portable electronics Provide experimental & computer modeling facilities for multidisciplinary graduate education (DOE s GATE & NSF GK-12 programs) Interdisciplinary team: 6-10 faculty, 5 research associates, 25 grad students, 5 undergrad assistants & 1 staff assistant Expertise areas: electrochemistry, materials science, multiphase transport, reactive flow, CFD modeling, experimental diagnostics, invehicle testing, advanced materials. Focus on design, modeling, fabrication, diagnostics and system integration of PEMFC, DMFC, and SOFC
4 ECEC Facilities (>5,000 sq ft) Fuel Cell/Battery Experimental Labs Kinetics and Thermal Transport Fuel Cell/Battery Simulation and Parallel Computing Fuel Cell Materials Research and Component Fabrication
5 H 2 /Air PEM Fuel Cells: Modeling Computer simulations are increasingly part of of the discovery and design process in the competitive field of fuel cells. ECEC vision: FC Modeling must consist of four elements: - physico-chemical model development - advanced numerical algorithms - materials characterization (to provide accurate input parameters) - experimental validation at detailed levels Current Collector Fuel Current Collector H + H + z y Fuel Air x Flow Channel Backing Layer Catalyst Layer Membrane Catalyst Layer Backing Layer Flow Channel ANODE PEM CATHODE
6 Physico-chemical Model Development Main features of ECEC models (available as in-house code, user code for STAR-CD or UDF for Fluent): - electrochemical and transport tightly coupled - fully resolve gas channels, GDL, catalyst layers & electrolyte - 3-D; steady-state and transient operation - water and proton co-transport in polymer electrolyte - accurate modeling of liquid water transport in hydrophobic GDL (ECEC s M2 model) and water management - Detailed MEA model Water Content Potential (V) Anode Membrane Cathode MEA (m) Membrane MEA (m)
7 Size of Numerical Problem: The Mesh Computational Mesh: - Through plane direction: 6-8 grid points in each of 5 distinctive regions of MEA + 10 points in each channel = Along-channel direction: points - In-plane: 10 points in channel and collector shoulder = 20 grids/flow channel Reasonable Mesh Size: 50X100X400 (for 20- channel flowfield)= 2x10 6 gridpoints! Anode outlet Cathode Inlet Cathode channel Thru plane Anode channel Anode Inlet Cathode outlet In plane Along-channel direction
8 Massively Parallel Computations ECEC has a 50-node Linux cluster (1.4GHz AMD processors) dedicated to fuel cell simulation and stack design - parallel-computing individual cells in a stack with each computer node for one cell - domain decomposition for large-scale simulation PSU clusters: Lion-XL ( GHz P4 processors), Lion-XE (256 1GHz P3 processors)
9 Massively Parallel Computations Parallel computing performance >7x speed-up with every 10 nodes roughly 300 iterations <1.5 hours for 1M comp. cell problem with 10 nodes Parallel Speed-up CPU Numbers Velocity Field (0.66 V, 0.96 A/cm 2 )
10 Ex: Large-Scale Cell Simulation 36-channel, double-pass serpentine fuel cell Cell Specifications: Anode: 2 passes are co-flow Cathode: 2 passes are counterflow Membrane: N112 A/C Stoich: 1 A/cm 2 A/C Pressure: 2.1 bars T cell : 80 o C; V cell =0.65 V A/C RH: 100%/5% Computational details: 2.56 M cell mesh, 300 iterations for convergence, 5 hours on ECEC Linux cluster using 9 processors.
11 Macro View: O 2 Distribution (mol/m 3 ) V cell =0.65 V I avg =0.91 A/cm 2 O 2 distribution in the cathode gas channels
12 Macro View: H 2 O Distribution V cell =0.65 V; I avg =0.91 A/cm 2 Anode gas channels Cathode gas channels (mol/m 3 ) (mol/m 3 ) Fully humidified H 2 in Dry air in
13 Macro View: Current Distribution V cell =0.65 V; I avg =0.91 A/cm 2 (A/m 2 ) H2 O2
14 Micro View: Current Density Profile Current Density (A/cm 2 ) V cell =0.65 V; I avg =0.91 A/cm 2 Each gridline marks the centerline of a land Z
15 16 Micro View: Water Content Profile Water cathode/gdl interface in the middle section of gas channels (V cell =0.65 V; I avg =0.91 A/cm 2 ) Water Content Each gridline marks the centerline of a land Z
16 Flooding Prediction by M2 Model Fully 3-D, two-phase, whole cell modeling and flooding prediction as function of the GDL wetting properties are available. 2-channel serpentine fuel cell Liquid Saturation Distribution at Cathode/GDL Interface (A/C RH: 100%/100%; Stoich: 1A/cm 2, V cell =0.4V, I avg =1.59 A/cm 2, GDL CA=105 o ) 1. Flooding occurs near the inlet of fully humidified cathode where current density is highest. 2. Liquid water does not transport transversely in plane, thus flooding is a localized phenomenon.
17 Flooding Prediction by M2 Model Channel Serpentine Flow Fully humidified inlets, A/C Stoich: 1 A/cm Cell Voltage [V] Power Density [W/cm 2 ] Mass Transfer limitation due to O 2 depletion Two-Phase Model Pseudo-Single Phase Model Current Density [A/cm 2 ] Mass Transfer limitation due to O 2 depletion and flooding Source: Pasaogullari & Wang, ECS Paris Mtg, April 2003.
18 Flooding Prediction by M2 Model Current Distributions w/ and w/o Flooding Pseudo Single Phase Model Two Phase Model I avg = 1.84 A/cm 2 (single phase) 1.69 A/cm 2 (two-phase) Local Current Density [A/cm 2 ] Channel Serpentine Flow Field Stoichiometry A/C: 1A/cm 2 Pressure: 1.5 atm (A/C) T cell = 80ºC V cell = 0.3 V U- turn location Distance from Inlet along Flow Path [m] Increased mass transfer due to mixing effect at the U-turn region Higher mass transfer resistance due to higher depletion of oxygen at the inlet region Source: Pasaogullari & Wang, ECS Paris Mtg, April 2003.
19 Effect of Inlet Humidity Local Current Density [A/m 2 ] %A-100%C 100%A-40%C 100%A-20%C 70%A-20%C Flooding Liquid Saturation, s Onset of liquid water 100%A-100%C 100%A-40%C 100%A-20%C 5000 Membrane Dry-out Distance along the Flow Direction [m] Distance along the Flow Direction [m] Note that M2 model can predict single-phase region in low-humidity operation, location of the onset of liquid water (unknown a priori), and two-phase region all together in one problem.
20 Effect of Stoichiometry 0.9 Same test cell as humidity case. Inlet Relative Humidity: 20% Cathode 100% Anode Test Case 1A/cm 2 : 1.0/1.0 A/C 1.4/1.4 A/C 1.8/1.8 A/C Cell Voltage [V] Symbols mark onset of liquid water Average Current Density [A/cm 2 ]
21 Effect of Stoichiometry Local CUrrent Density [A/m 2 ] Current Density 0.20 Liquid 0.4V ζ: 1A/cm ζ: 1A/cm 2 ζ: 1A/cm 2 Liquid Saturation, s ζ: 1A/cm 2 ζ: 1A/cm 2 ζ: 1A/cm Distance along the Flow Direction [m] Distance along the Flow Direction [m]
22 Materials Characterization Materials properties are required on Membranes Membrane-electrode assembly (MEA) properties including electrokinetic data for catalyst layers Gas diffusion layers (GDL) Bipolar plates Chemical reactants and products. SEM of Toray carbon paper SEM of carbon cloth
23 Materials Characterization Contact angle measurement Free surface Inserting specimen Liquid level Meniscus height Water drops on GDL surface at 70 o C Highly hydrophobic GDL Hydrophobic GDL Hydrophilic GDL
24 Experimental Validation Operation Conditions T cell =80 o C T a =T c =80 o C 1.0 Operation Conditions T cell =80 o C T a =T c =50 o C Cell Voltage (V) A/C: 100% RH Cell Voltage (V) A/C: 26% RH 0.2 Numerical Data Experimental Data 0.2 Numerical Data Experimental Data Current Density (A/cm 2 ) Current Density (A/cm 2 )
25 Is Pol Curve Sufficient for Model Validation? Consider a single-channel, 7 cm long fuel cell with Gore 18 µm membrane and operated at 80 o C and A/C stoich of 3/2 and RH of 42%/dry. Catalyst layer ionic resistance Product of specific active area and ORR exchange current density, aj o (A/m 3 ) Case 1 (ohmic polarization dominated) included 2.53x10 4 Case 2 (concentration polarization dominated) neglected 1.95x10 4 Current Density (A/m 2 ) Case 1 (ohmic polarization dominated) Case 2 (concentration polarization dominated) I 0.75V, A/cm Distance from Inlet (m) Obviously the average I-V curve is largely insufficient for validation of detailed fuel cell models. Experimental validation at the distribution level (current, species and temperature) is required!
26 Detailed Diagnostics ECEC has extensive MEA fabrication and fuel cell test facilities for experimental diagnostics and model validation. These data include not only I-V curves but also detailed distributions of current, species, and temperature as well as visualization of two-phase flow and flooding. ECEC has developed unique capabilities for current, concentration and (membrane) temperature mapping. Segmented flow plates w/ 48 separate current collection ribs for current density distribution measurement by a multi-channel potentiostat a 50cm 2 cell in testing for current and concentration mapping
27 Measured Current Distributions Current Density, A/cm Pressure H 2 /Air = 1 atm (gauge) H 2 ξ a = 1 A/cm 2, 80 o C 50%RH Air ξ c = 1 A/cm 2, 80 o C 25%RH 0.8 V 0.7 V 0.6 V 0.5 V 0.4 V Fractional Distance from Cathode Inlet
28 Measured Water Distributions 70 In Cathode Gas Channel Water Mole Fraction (%) o Ctheoretical max. 80 o Ctheoretical max. Zero cathode inlet humidity 20% mole 20% fraction mole fraction water vapor vapor at cathode anode inlet inlet 0.8 V 0.6 V 0.4 V 0.8 V 0.6 V 0.4 V Fractional Distance from Cathode Inlet Pressure A/C = 1.5 atm 100% 90 o C H 2 Anode ξ c = 1 A/cm 2 ξ a = 1 A/cm 2
29 Validation by Current Distribution Data Comparison of average polarization curves for 0.75 A/cm 2 cathode stoichiometry Voltage [V] Exp_avg Sim_avg Current Density [A/cm 2 ] But, the comparison of current distribution is far from satisfactory Current Density [A/cm 2 ] Comparison of average current density can be excellent! Simulated and measured current density distributions along the cathode path for 0.75 A/cm 2 cathode stoichiometry Lines are simulation results 0.85 V(EXP) 0.8 V(EXP) 0.75V(EXP) 0.65 V(EXP) 0.6 V(EXP) 0.5 V(EXP) 0.45 V(EXP) 0.4 V(EXP) V(SIM) V(SIM) V(SIM) 0.65 V(SIM) 0.58V(SIM) 0.51 V(SIM) 0.45 V(SIM) 0.4 V(SIM) Fractional Distance from Cathode Inlet
30 Electrode Reactions Oxidation of fuel at anode H O H 2O + e Reduction of oxidant at cathode 1 2 O2 + 2e O 2 Cell Materials Anode: Nickel / Yttria Stabilized Zirconia Cermet Cathode: Solid Oxide Fuel Cells LSM Layer: La 1-x Sr x MnO 3 Electrolyte: YSZ: Y 2 O 3 doped ZrO 2 material
31 SOFC Modeling SOFC modeling is simpler than PEMFC as there is no complex water transport and distribution issue It is a problem very similar to chemically reactive flows except that there is charge transport thru electrolyte and active layers. New numerical issues are: (1) nonlinear source terms described by Tafel kinetics; (2) multiple anodic reactions (e.g. H 2 +CO oxidation); (3) solution of two potential equations (electronic and ionic); and (4) implementation of constant total current as a boundary condition instead of a constant cell voltage; ECEC has developed a unified framework for SOFC and PEMFC modeling, with the former requiring no elaborative treatment of water transport.
32 ( κ Φ) eff + SΦ = 0 SOFC Model Equations Conservation Equation Flow Channels Porous Electrodes Source Terms Active Electrodes Electrolyte Mass Momentum ( ερ ) r + ( ρ u) = 0 t r 1 ρu 1 r r + ( ρuu) = p + + t τ ε ε S u S u µ r = u K u r = 0 u r = 0 Species ( ε c ) t k + r eff ( u ck ) = ( Dk ck ) + Sk S k sk j = n F Charge eff ( κ Φ ) + S = 0 Φ S = Φ j Heat ( ερ c T ) t P + r eff ( ρ c ) ( ) P u T = k T + ST S T = j η + T du dt 0 + i κ 2 eff S T = i κ 2 eff Electrochemical Reaction: k s k M z k = ne where M k chemical formula of species k s k stoichiometry coefficient n number of electrons transferred Source: Pasaogullari & Wang, SOFC Symposium VIII, April 2003.
33 Electrolyte-Supported SOFC Cell Dimensions (2.5 cm 2 ) Cell Length: 16 mm Anode Channel: 2x2 mm 2 Anode Electrode Thickness: 50 µm Cathode Electrode Thickness: 50 µm Cathode Channel: 2x2 mm 2 Electrolyte: 180 µm Operating Conditions Operating Temperature: 1000 o C Anode Stoichiometry: 1.5 Cathode Stoichiometry: 2.0 Cross Flow SOFC Configuration
34 Electrolyte-Supported SOFC Electrochemical, flow, transport and thermal coupled modeling in 3-dimensions Current Distribution Thermal effect is insignificant here due to small cell size
35 Electrolyte-Supported SOFC 3-D reactant concentration contours O 2 Concentration in Cathode of SOFC H 2 Concentration in Anode of SOFC
36 Geometry Anode-Supported SOFC 10-Channel Cross-Flow Anode Electrode: 1mm Cathode Electrode: 50 µm Electrolyte: 10 µm Operating Conditions 2 atm Anode/Cathode Inlet Pressure Operating Temperature: 800ºC Anode/Cathode Stoichiometry: 2 A/cm 2
37 Anode-Supported SOFC Local Current Density (A/m 2 0.7V; I avg =1.5 A/cm 2
38 Anode-Supported SOFC O 2 Concentration (mol/m 3 ) at Cathode-Interlayer Interface
39 Anode-Supported SOFC H 2 Concentration (mol/m 3 ) at Anode-Interlayer Interface
40 ECEC Fuel Cell Controls Group Chao-Yang Wang Dynamic Modeling Christopher Rahn Sensors Matthew Mench Asok Ray Diagnostics Control System Design Sean Brennan Automotive Systems
41 Summary Multidisciplinary computational fuel cell research encompasses: (1) physicochemical model development, (2) numerical algorithm development, (3) materials characterization, and (4) model validation at detailed levels. PEMFC model is mature for use in product design and optimization. Considerable capabilities are available: fully coupled electrochemical/ flow modeling, 3-D, water and heat management, cathode flooding, CO poisoning, cold start, etc. ECEC also has developed an electrochemical-transport coupled model for SOFC in commercial CFD packages. Fuel cell control strategies are studied and integrated at early stages to enable design for high performance, design for robust controls, or design for high reliability.
42 Acknowledgements ECEC Team, and former graduates and associates U.S. DOE, DOD, DOT, NSF, Sandia, Argonne, NETL Many industries worldwide
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