Exploring The Fundamentals In Catalytic Partial Oxidation Of Methane: The Interaction Between Diffusion And Reaction In A Packed Bed Reactor

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1 Exploring The Fundamentals In Catalytic Partial Oxidation Of Methane: The Interaction Between Diffusion And Reaction In A Packed Bed Reactor Songjun Liu; Ana Obradović; Joris W. Thybaut; Guy B. Marin Laboratory for Chemical Technology, Ghent University 1

2 Introduction Syngas production route 0 H 298 Kj mol Steam reforming (SR): CH 4 + H 2 O = CO + 3H CO + H 2 O = CO 2 + H 2-41 Catalytic partial oxidation (CPO): Direct route: CH O 2 = CO + 2H 2-38 Indirect route: CH 4 + 2O 2 = CO 2 + 2H 2 O -802 CH 4 + H 2 O = CO + 3H Homogeneous reactions High velocity Limiting Advantages of CPO: Autothermal operation High catalytic reaction rate: short residence time (1-10 ms) high throughput ideal H2/CO ratio: 2/1 High reactivity Aim: Study the diffusion-reaction interaction by a packed bed reactor model: External and internal diffusions Surface and homogeneous reactions

3 Introduction Reactor model development Model validation & baseline case Reactor performance at various configurations Conclusion Acknowledgement Outline 3

4 Packed bed reactor model Assumptions: Sphere particles and cylindrical tubes around particles No axial diffusion and conduction No pressure drop Ideal gas Microkinetics: CPO on Rhodium [2] : 6 gas species, 12 surface species, 36 reactions CH 4 Homogeneous combustion (Reduced GRI30) [3] : 32 species, 196 reversible reactions Reactor scale Interstitial cylinder diameter: Pellet scale [1] Kechagiopoulos, Panagiotis N., Joris W. Thybaut, and Guy B. Marin. Industrial & Engineering Chemistry Research 53.5 (2013): [2] Dalle Nogare, D., Degenstein, N. J., Horn, R., Canu, P., & Schmidt, L. D. (2011). Journal of catalysis, 277(2), [3] Gregory P. Smith, David M. Golden, Michael Frenklach, Nigel W. Moriarty, Boris Eiteneer, Mikhail Goldenberg, C. Thomas Bowman, Ronald K. Hanson, Soonho Song, William C. Gardiner, Jr., Vitali V. Lissianski, and Zhiwei Qin 4

5 Governing equations Interstitial phase: Convection, external diffusion, homogeneous reactions C i,g t C i,c t = (u gc i,g ) z T g = (u gt g ) t z = D e,i ξ 2 ξ + D m,i r + α g r r Nsp,g i ξ2 C i,c ξ r r T g r r C i,g r + R i,g Intraparticle phase: internal diffusion, homogeneous reactions, surface reactions R i,g H i,g /(ρ g Cp g ) + a c R i,s + ε c R i,g Boundary conditions: z = 0 0 < r < d v 2 : C i,g = C i,0, T g = T 0 r = 0 C i,g r = 0, T g r = 0 r = d v 2 0 = a g D m,i C i,g r + a cd e,i C i,c ξ T g 0 = a g λ g + a T s r cλ e ξ T s = α e t ξ 2 Surface intermediates: θ i,s t (ε c = R i,s Γ θ i,s = 1 ξ ξ2 T s ξ Nsp,g Nsp,s i R i,g H i,g + a c i R i,s H i,s )/(ρ s Cp s ) ξ = 0 C i,c ξ = 0, T s ξ = 0 ξ = d p 2 : C i,g = C i,c, T g = T s 5

6 Solution Reactor coordinate: Backward difference 115 points unevenly distributed Pellet coordinate: Orthogonal collocation (for symmetry problem) Collocation points: >> interstitial : 6 >> intraparticle :11 6

7 Introduction Reactor model development Model validation & baseline case Reactor performance at various configurations Conclusion Acknowledgement Outline 7

8 Model validation & baseline case Baseline conditions >> Inlet Temperature = 500 C >> Pressure = 1 atm >> CH 4 /O 2 /N 2 = 2/1/4 >> W/F CH4,0 = kg s mol -1, V/F tot,0 = m 3 s mol -1 >> Catalyst diameter = 0.4 mm >> Catalyst density = kg/m 3 >> Rh specific surface area = 0.2 m 2 /g >> Catalyst porosity/tortuosity = 0.4/4.0 >> Bed porosity = 0.42 (loose packing) >> Reactor length/diameter = 20mm/15mm 8

9 Model validation This work: Mole fractions profile along axial coordinate (radial positon: center of interstitial phase) Qualitatively validated Literature results: spatial profiles of experimental and modeling compositions in foam reactor [1] [1] Dalle Nogare, D., Degenstein, N. J., Horn, R., Canu, P., & Schmidt, L. D. (2011). Journal of catalysis, 277(2),

10 Temperature & mole fractions: reactants High solid conductivity 10

11 Mole fractions: major products High diffusivity Kinetically favorable: Steam reforming, WGS x CO 2 reforming, reverse WGS 11

12 Surface coverages 12

13 Mole fractions: Radicals Conclusions for baseline case: strong diffusion limitations in both inter- and intra- particle phase Steam reforming is kinetically favored, CO 2 consumption is kinetically unfavorable, homogeneous reactions are negligible at atmosphere pressure 13

14 Introduction Reactor model development Model validation & baseline case Reactor performance at various configurations Conclusion Acknowledgement Outline 14

15 Reactor performance cases: 1. Increase reactivity Rh specific surface area: 0.2, 0.6, 1.0 m 2 /g 2. Increase particle diameter (increase diffusion distance) Catalyst particle diameter: 0.4, 0.8, 1.2 mm 3. Industrial condition Particle diameter: 1.2 mm Pressure: 10:5:30 bar 15

16 Rh specific surface area: 0.2, 0.6, 1.0 m 2 /g Rh specific surface area High loading: Steam reforming: kinetics & transport limited Oxidation: transport limited H2/CO:

17 Particle diameter: 0.4, 0.8, 1.2 mm bed porosity: 0.42, 0.44, 0.45 Interstitial tube diameter: 0.193, 0.419, mm Particle diameter H2/CO:

18 Particle diameter 1.2 mm Pressure: 10:5:30 bar High pressure (1) A.Bitsch-Larson; R. Horn; L.D. Schmidt, Applied Catalysis A: General 348 (2008), H2/CO:

19 Conclusion 1. An adiabatic packed bed reactor was developed and validated. Strong diffusion limitations were confirmed in both inter- and intra-particle phase 2. High catalyst loading has little impact on reactor performance in the highly diffusion limited reactor. 3. The diffusion limitations are largely enhanced for larger particles, lower the efficiency of catalytic bed. 4. Homogeneous combustion at elevated pressure changes the reaction path, results in a more complicated coupling of homogeneous reactions, mass and heat transfer and surface reactions. 19

20 Acknowledgement European Research Council FP7/ /ERC grant agreement n China Scholarship Council Thank you for your attention Laboratory for Chemical Technology Ghent University 20

21 CPO on Rh kinetics 21

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