Steam Reforming in a Packed Bed Membrane Reactor
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1 Steam Reforming in a Packed Bed Membrane Reactor Nico Jurtz, Prof. Matthias Kraume Technische Universität Berlin Chair for Chemical and Process Engineering nico.jurtz@tu-berlin.de
2 Outline Motivation Modeling Basics of modeling packed-bed reactors Basics of modeling membranes Validation of reaction mechanism Case study PBR vs. PBCMR Reaction rate coefficients Concentration and temperature field Reactor performance Outlook Folie 2
3 Motivation Hydrogen is the most important compound of chemical and petrochemical industries Steam Reforming of Methane (SRM) is the most used and economic process for the large scale production of hydrogen and synthesis gas 50% of world wide hydrogen production is produced via SRM In terms of process intensification fixed-bed membrane reactors may increase the yield by shifting the chemical equilibrium towards the product side - Le Chatelier's Principle Computational Fluid Dynamics (CFD) is a valuable tool for the understanding and design of that reactor type World-wide H 2 production [10 9 Nm 3 ] Source: Folie 3
4 What is needed? Membrane flux (Itoh et al.): E a A e RT J H2 = p δ f p p E a = kj mol A = mol m s Pa 0.5 δ = 5μm F mem/geom = 2 3-step mechanism (Xu et al.): R1: CH 4 + H 2 O CO + 3H 2 R2: CO + H 2 O CO 2 + H 2 R3: CH 4 + 2H 2 O CO 2 + 4H 2 Itoh et al., Handbook of membrane reactors. 2013, J. Xu, G.F. Froment, AIChE J. 1989, 35, CH 4, H 2 O CO 2, CO, H 2 N 2, H 2 R 1 = k p p CH 4 p H2 O p H 3 2 p CO 1 H2 K e1 DEN 2 R 2 = k 2 p H2 r i = ν i R j j i J H2 p CO p H2 O p H 2 p CO2 K e2 1 DEN 2 R 3 = k p p 2 CH 4 p H2 O p H 4 2 p CO2 1 H2 K e3 DEN 2 DEN = 1 + K CO p CO + K H2 p H2 + K CH4 p CH4 + K H 2 Op H2 O p H2 N 2 Folie 4
5 Modeling Packed Bed Reactors
6 Modeling Packed Bed Reactors Workflow: 1. Discrete-Element-Methode (DEM) for packing generation 2. Create geometry of packing based on DEM results 3. Meshing (local flattening at contacts) 4. CFD Simulation Folie 6
7 Fundamentals of Chemical Kinetics Brutto equation Limited insights CH 4 + H 2 O CO + 3H 2 Lumped kinetics Some parameters can be studied Limited to experimental setup (p,t, composition) Fluid dynamic effects (mass transport limitations) are often lumped into the kinetics Elementary step mechanism Detailed insights Transferable to other types of reactor Very complexe, high calculation times All relevant steps has to be taken into account large systems Folie 7
8 Implementation of Chemical Kinetics Currently no User-defined Reaction Rate available for Surface Chemistry Model Define reaction rate expressions via field functions Use of Wall Boundary Species Flux option Heat of reaction is calculated through enthalpy difference BUT: Kinetic mechanism is not thermodynamic consistent Use constant and equal specific heat for all species Use Wall Boundary Heat Flux option Folie 8
9 Modeling Membrane Reactors
10 ሶ ሶ ሶ Modeling Transmembrane Flux Mass transfer through membrane is proportional to some driving force Membrane specific characteristics are lumped into one coefficient (permeance or permeability) Temperature dependency of permeability can be modeled by Arrhenius-type equation A mapping approach on conformal interfaces is used to calculate the driving force Concentration profile within the membrane c f Porous support c f,m Active layer c d,m Semi-permeable membrane c d,bulk Permeate Reduced concentration at membrane m i ~Δμ i m i ~Δc i m i ~Δp i Folie 10
11 Examples of membrane modeling Gas separation membrane 10 bar 10 bar 40 bar Folie 11
12 Relative Recovery Dextran [-] Examples of membrane modeling Tubular membrane reactor Radial Position of the Pipe [m] 0.15 Folie 12
13 Examples of membrane modeling Flat sheet membrane Increasing Pressure Velocity Inlet: u 0 =0.2m/s c NaCl =2g/l Feed Side Pressure Outlet Permeate Side Membrane Folie 13 Baffle
14 PBR + MBR = PBCMR
15 Mole Fraction [-] Mole Fraction [-] SRM in Annulus Packed Bed Reactor - Validation Models: Heated wall 60kW/m 2 Catalyst particles Turbulence: Realizable k- P PBR : 1.5bar Radiation Surface-to-surface T in,pbr : 973K EoS Ideal Gas u in,pbr : 7.75m/s Transport properties: Chapmen-Enskog : 0.8 Heat Transfer: CHT H 2 O/CH 4 ratio: Mole Outlet CH4 H2O H2 CO CO2 Kuroki 2009 Current Study Axial Concentration Profile Axial Position [m] CH4Series1 H2OSeries2 H2 Series3 Folie 15
16 Process Intensification Packed Bed Membrane Reactor Adiabatic wall Semi-permeable membrane Catalyst particles P PBR : T in,pbr : u in,pbr : 3.1bar 750K 0.12m/s : 0.8 H 2 O/CH 4 ratio: 3.5 P M : 0.1bar Sweep ratio: 1.04 Folie 16
17 PBR PBCMR Reaction Rate Coefficients R1: CH 4 + H 2 O CO + 3H 2 R2: CO + H 2 O CO 2 + H 2 Rate Coefficient [mol/kg-cat s] Folie 17
18 PBR PBCMR Reaction Rate Coefficient and Membrane Flux R3: CH 4 + 2H 2 O CO 2 + 4H 2 Rate Coefficient [mol/kg-cat s] Folie 18
19 PBR PBCMR Temperature and Concentration Field Folie 19
20 Conversion [%] Yield [%] Conclusion and Outlook % % Outlook: 8 8 Use of Detailed Chemistry Variation of operating parameters 6 6 Operating temperature Operating pressure Transmembrane pressure 4 4 Sweep ratio Co- vs. Counter-Current 2 2 Extend bed length 0 0 PBR PBCMR Folie 20
21 Thanks Thanks for your attention! Acknowledgement: This work is part of the Cluster of Excellence Unifying Concepts in Catalysis coordinated by the Technische Universität Berlin. Financial support by the Deutsche Forschungsgemeinschaft (DFG) within the framework of the German Initiative for Excellence is gratefully acknowledged (EXC 314). Folie 21
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