Numerical Modelling of the Original and Advanced Version of the TEMKIN-Reactor for Catalysis Experiments in Laboratory Scale

Similar documents
3 rd Generation Stabilized Front End Selective Hydrogenation Catalysts Enhance Operational Stability and Maximize Ethylene Gain

Computational Fluid Dynamic Study On The Decomposition Of Methane Gas Into Hydrogen And Solid Carbon In A Packed Bed Fluid Catalytic Cracking Reactor

INTRODUCTION TO CATALYTIC COMBUSTION

Chemical Reaction Engineering - Part 16 - more reactors Richard K. Herz,

ADVANCES IN OLEFIN PURIFICATION VIA CATALYSIS AND SORBENT MATERIALS

Two-dimensional mathematical modeling of oxidative coupling of methane in a membrane reactor

Modeling of Packed Bed Reactors: Hydrogen Production By the Steam Reforming of Methane and Glycerol

Rajeev K. Garg, V.K. Srivastava, V.V. Krishnan Department of Chemical Engineering, Indian Institute of Technology, Hauz Khas, New Delhi , India

Vacuum Gas Carburizing with Acetylene - Gas Phase Modeling of a Bench Scale Reactor

Nirma University Institute of Technology Chemical Engineering Department, Handouts -RRP- CRE-II. Handouts

Transient modeling of chemical vapor infiltration of methane using multi-step reaction and deposition models

Dehydrogenation of Propane to Propylene Over Pt-Sn/Al 2 O 3 Catalysts: The influence of operating conditions on product selectivity

Chemical Reaction Engineering

Structural and Catalytic Investigation of Active-Site Isolation in Pd-Ga Intermetallic Compounds

Modeling of Packed Bed Reactors: Hydrogen Production by the Steam Reforming of Methane and Glycerol

Dehydrogenation of propane with selective hydrogen combustion: A mechanistic study by transient analysis of products

NPTEL. Chemical Reaction Engineering II - Video course. Chemical Engineering. COURSE OUTLINE

To increase the concentration of product formed in a PFR, what should we do?

Methane Oxidation Reactions

Mass Balance MATHEMATICAL MODEL FOR THERMAL CRACKING OF HYDROCARBONS ETHANE CRACKING

Be prepared to discuss the quantitative comparison method in the oral exam.

Stoichiometric Reactor Simulation Robert P. Hesketh and Concetta LaMarca Chemical Engineering, Rowan University (Revised 4/8/09)

Carbon2Chem. Modeling the Catalytic Conversion of Steel Mill Gases. Stefan Schlüter, Fraunhofer UMSICHT, Oberhausen (Germany) Fraunhofer UMSICHT

Lecture (9) Reactor Sizing. Figure (1). Information needed to predict what a reactor can do.

Adsorption (Ch 12) - mass transfer to an interface

close to performances of the turbine gas meters designed for custody transfer measurements.

Structural and Catalytic Investigation of Active-Site Isolation in Pd-Ga Intermetallic Compounds

Chemical Reactor flnolysis

SRC SUPER RADIANT COIL

Effects of Different Processing Parameters on Divinylbenzene (DVB) Production Rate

Oxygenate Formation from n-butane Oxidation at Short Contact Times: Different Gauze Sizes and Multiple Steady States 1

2Fe 2 O 3 +3H 2 S FeS+FeS x +S+3H 2 O

Development, Application and Understanding of Synthetic Tools!

Fast Determination of Impurities in Propane- Propylene Streams Using a Pulsed Flame Photometric Detector (PFPD) and a New Capillary.

Multiscale Modeling of Carbon Nanotube Synthesis in a Catalytic Chemical Vapor Deposition Reactor

Simulation study of membrane supported oxidation of methane with simultaneous steam reforming using O 2 - selective Perowskite hollow fibres

TABLE OF CONTENT. Chapter 4 Multiple Reaction Systems 61 Parallel Reactions 61 Quantitative Treatment of Product Distribution 63 Series Reactions 65

CFD study of gas mixing efficiency and comparisons with experimental data

A First Course on Kinetics and Reaction Engineering Unit 12. Performing Kinetics Experiments

Chemical Reaction Engineering Lecture 5

Notes on reaction-diffusion cases with effectiveness factors greater than one! Richard K. Herz,

How sulphur really forms on the catalyst surface

PCE126 Chemical Reaction Engineering & Applied Chemical Kinetics

Modelling Thermal Time-of-Flight Sensor for Flow Velocity Measurement

Part A: Operando FT-IR Studies of heterogeneous catalytic reactions: pitfalls and benefits.

Modeling of the Unsteady State Methanol Synthesis at the Level of Catalyst Pellet

Modeling Of Carbon Deposit From Methane Gas On Zeolite Y Catalyst Activity In A Packed Bed Reactor

A First Course on Kinetics and Reaction Engineering Example 1.2

DETAILED MODELLING OF SHORT-CONTACT-TIME REACTORS

Comparison between Honeycomb and Fin Heat Exchangers

Steady-State and Dynamic Systems for Diffusion Parameters Determination: Advantages and Disadvantages

The Seeding of Methane Oxidation

Introduction. Mathematical model and experimental

HANDBOOK SECOND EDITION. Edited by

H 0 r = -18,000 K cal/k mole Assume specific heats of all solutions are equal to that of water. [10]

Overview of Reacting Flow

Chemical Reactions and Chemical Reactors

International Journal of ChemTech Research CODEN (USA): IJCRGG ISSN: Vol.8, No.6, pp , 2015

Mathematical Investigation and CFD Simulation of Monolith Reactors: Catalytic Combustion of Methane

By Rogéria Amaral and Sébastien Thomas

Modeling of a Fluid Catalytic Cracking (FCC) Riser Reactor

Engineering. Green Chemical. S. Suresh and S. Sundaramoorthy. and Chemical Processes. An Introduction to Catalysis, Kinetics, CRC Press

An Introduction to COMSOL Multiphysics v4.3b & Subsurface Flow Simulation. Ahsan Munir, PhD Tom Spirka, PhD

Non-oxidative methane aromatization in a catalytic membrane reactor

Exercise 1. Material balance HDA plant

A mini review on the chemistry and catalysis of the water gas shift reaction

The School For Excellence 2018 Unit 3 & 4 Chemistry Topic Notes Page 1

Multiple Reactions. ChE Reactive Process Engineering

SUPPLEMENT TO CHAPTER 7 7S.1 LOCATING THE SEPARATION SECTION WITH RESPECT TO THE REACTOR SECTION

Oxygen-Containing Contaminants and Steam Cracking: Understanding their Impact Using COILSIM1D

Erratum to: High speed mixture fraction and temperature imaging of pulsed, turbulent fuel jets auto igniting in high temperature, vitiated co flows

CATALYTIC COMBUSTION OF HYD RO GEN/ AIR IN MICROCHANNEL REACTOR

TRANSALKYLATION OF DIISOPROPYLBENZENE WITH BENZENE IN SUPERCRITICAL CARBON DIOXIDE

Supplementary Information. The role of copper particle size in low pressure methanol synthesis via CO 2 hydrogenation over Cu/ZnO catalysts

Modelling and Simulation of hydrogen storage device for fuel cell using COMSOL Multiphysics

ChE 344 Chemical Reaction Engineering Winter 1999 Final Exam. Open Book, Notes, CD ROM, Disk, and Web

Review: Nonideal Flow in a CSTR

Alkylation process, Feedstocks, reactions, products, catalysts and effect of process variables.

IDEAL REACTORS FOR HOMOGENOUS REACTION AND THEIR PERFORMANCE EQUATIONS

Hydrogen addition to the Andrussow process for HCN synthesis

Possibilities and Limits for the Determination of. Adsorption Data Pure Gases and Gas Mixtures

ENZYME SCIENCE AND ENGINEERING PROF. SUBHASH CHAND DEPARTMENT OF BIOCHEMICAL ENGINEERING AND BIOTECHNOLOGY IIT DELHI

Compact Multi-Fuel Autothermal Reforming Catalytic Reactor for H 2 Production

Kinetic Characterisation of Zeolite Catalysts Using Cracking, Alkylation and Other Chemical Reactions

CHEMICAL ENGINEERING DEPARTMENT Equipments and List of Experiments in each Laboratory

Kinetics of Catalytic Cracking of Kerosene to Ethylene on CaO-Promoted Z5 Nano-Catalyst

Kinetic Analysis and Development of a Complete Catalytic Oxidation of Methane Experiment for Unit Operations II

Effects of Ethane Partial Pressure on the Apparent Rate Expressions of Oxidative Couplin... Page 1 of 16

Identification in closed-loop, MISO identification, practical issues of identification

Deep Desulfurization of Diesel using a Single-Phase Micro-reactor

Hydrogenation of CO Over a Cobalt/Cerium Oxide Catalyst for Production of Lower Olefins

COMSOL Multiphysics Simulation of 3D Single- hase Transport in a Random Packed Bed of Spheres

Vapor-hydrate phases equilibrium of (CH 4 +C 2 H 6 ) and (CH 4 +C 2 H 4 ) systems

AE 205 Materials and Energy Balances Asst. Prof. Dr. Tippabust Eksangsri. Chapter 4 Stoichiometry and MB with Reactions

Relative Conversion of Lower Alkanes in Their Simultaneous Partial Gas-Phase Oxidation

(1) This reaction mechanism includes several undesired side reactions that produce toluene and benzene:

Hydrogen production by decomposition of ethane-containing methane over carbon black catalysts

Mechanistic Study of Selective Catalytic Reduction of NOx with C2H5OH and CH3OCH3 over Ag/Al2O3 by in Situ DRIFTS

Catalyst Characterization Using Thermal Conductivity Detector *

Introduction to the course ``Theory and Development of Reactive Systems'' (Chemical Reaction Engineering - I)

Transcription:

Numerical Modelling of the Original and Advanced Version of the TEMKIN-Reactor for Catalysis Experiments in Laboratory Scale D. Götz, M. Kuhn, P. Claus TU Darmstadt, Ernst-Berl-Institute for Technical and Makromolekular Chemistry, Alarich-Weiss-Straße 8, D-64287 Darmstadt, Germany 17.09.2014 TU Darmstadt Ernst-Berl-Institute Prof. Dr. P. Claus Dominik Götz, M.Sc.

Laboratory Scale Reactors Testing of Egg-shell Catalysts Plug Flow Reactor (PFR) Simple build-up Requirements for ideal behaviour: Reactor radius / pellet radius: min. 10 Reactor length / pellet length: min. 30 High catalyst amounts and feed streams cost-intensive TEMKIN reactor Original: TEMKIN AND COWORKERS Advanced version: CLAUS AND COWORKERS Smaller catalyst amounts and feed streams needed Complex mass, momentum and heat transport! M. Temkin et al., Kulkova, Kinet. Katal 1969, 10, 461-463. M. Kuhn, M. Lucas, P. Claus, Chemie Ingenieur Technik, 2014. Patent, DE200920003014, 2009. 17.09.2014 TU Darmstadt Ernst-Berl-Institute Prof. Dr. P. Claus Dominik Götz, M.Sc. 1

Selective Hydrogenation of Acetylene Ethylene production in a steam cracker Acetylene impurities in ethylene stream Poisoning of downstream processes Selective hydrogenation using Pd-Ag/Al 2 O 3 egg shell catalysts tail-end process crack gases CO 2, H 2 S A. Borodzinki, Catal Rev 2006, 48, 91-144. CH 4,H 2, CO H 2 /CO dryer H 2 /CO C 3+ Ethylene Ethane 17.09.2014 TU Darmstadt Ernst-Berl-Institute Prof. Dr. P. Claus Dominik Götz, M.Sc. 2

Selective Hydrogenation of Acetylene Ethylene production in a steam cracker Acetylene impurities in ethylene stream Poisoning of downstream processes Selective hydrogenation using Pd-Ag/Al 2 O 3 egg shell catalysts tail-end process crack gases CO 2, H 2 S A. Borodzinki, Catal Rev 2006, 48, 91-144. CH 4,H 2, CO H 2 /CO dryer H 2 /CO C 3+ Ethylene Ethane Commercial industrial catalyst 17.09.2014 TU Darmstadt Ernst-Berl-Institute Prof. Dr. P. Claus Dominik Götz, M.Sc. 2

Selective Hydrogenation of Acetylene Ethylene production in a steam cracker Acetylene impurities in ethylene stream Poisoning of downstream processes Selective hydrogenation using Pd-Ag/Al 2 O 3 egg shell catalysts tail-end process crack gases acetylene r 1 r 2 CO 2, H 2 S r A. Borodzinki, 3 Catal Rev 2006, 48, 91-144. CH 4,H 2, CO H 2 /CO dryer H 2 /CO ethylene (target product) ethane C 3+ C 4 H x Ethylene Ethane Commercial industrial catalyst Kinetics from PFR experiments Two different active sites AS1 and AS2 due to carbon and hydrocarbon deposits Ethylene can only adsorb and react at the bigger active sites Reactions spatially separated r 1 = r 2 = r 3 = 1 2 k 1 p A p H2 2 1 + K A,13 p A k 2p Ey p H2 1 + K A,2 p A 2 1 2 k 3 p A p H2 2 1 + K A,13 p A active site AS 1 AS 2 AS 1 A. Pachulski, R. Schödel, P. Claus, Applied Catalysis A: General 2012, 445-446, 107-120. 17.09.2014 TU Darmstadt Ernst-Berl-Institute Prof. Dr. P. Claus Dominik Götz, M.Sc. 2

Modelling in COMSOL Multiphysics Distinguishing between different domains Free gas flow (cyan) Modelling of laminar fluid flow coupled with heat and species transport 17.09.2014 TU Darmstadt Ernst-Berl-Institute Prof. Dr. P. Claus Dominik Götz, M.Sc. 3

Modelling in COMSOL Multiphysics Distinguishing between different domains Free gas flow (cyan) Modelling of laminar fluid flow coupled with heat and species transport Inert support (white) Modelling of species and heat transport in porous media (no convection) 17.09.2014 TU Darmstadt Ernst-Berl-Institute Prof. Dr. P. Claus Dominik Götz, M.Sc. 3

Modelling in COMSOL Multiphysics Distinguishing between different domains Free gas flow (cyan) Modelling of laminar fluid flow coupled with heat and species transport Inert support (white) Modelling of species and heat transport in porous media (no convection) Catalytically active shell (red) Modelling of species and heat transport in porous media including reaction kinetics 17.09.2014 TU Darmstadt Ernst-Berl-Institute Prof. Dr. P. Claus Dominik Götz, M.Sc. 3

Modelling in COMSOL Multiphysics Distinguishing between different domains Free gas flow (cyan) Modelling of laminar fluid flow coupled with heat and species transport Inert support (white) Modelling of species and heat transport in porous media (no convection) Catalytically active shell (red) Modelling of species and heat transport in porous media including reaction kinetics Reactor body (not shown) Modelling of heat transport 17.09.2014 TU Darmstadt Ernst-Berl-Institute Prof. Dr. P. Claus Dominik Götz, M.Sc. 3

Validation Experimental setup Pulse tagging experiments Pulse injection by pneumatic 6-port valve Pulse detection via sensor unit of a thermal mass flow controller Catalysis experiments 4 reactor modules in series in a temperated aluminium block Typical industrial reaction conditions GHSV = 4000 h -1 Pressure = 11 bar Temperature = 45 C Hydrogen, acetylene, propane (internal standard): 1 Vol-% each; ethylene: 30 Vol-%; argon: 67 Vol-%, Online-gas chromatography connectors between reactor modules details published in M. Kuhn, M. Lucas, P. Claus, Chemie Ingenieur Technik, 2014. 17.09.2014 TU Darmstadt Ernst-Berl-Institute Prof. Dr. P. Claus Dominik Götz, M.Sc. 4

Validation Pulse Tagging Experiments Good agreement between simulated and measured pulse experiments Diffusion into the porous pellets leads to increasing residence times 17.09.2014 TU Darmstadt Ernst-Berl-Institute Prof. Dr. P. Claus Dominik Götz, M.Sc. 5

Validation Pulse Tagging Experiments Good agreement between simulated and measured pulse experiments Diffusion into the porous pellets leads to increasing residence times Simple reactor models fail due to complex mass transfer 17.09.2014 TU Darmstadt Ernst-Berl-Institute Prof. Dr. P. Claus Dominik Götz, M.Sc. 5

Validation Catalysis Experiments PFR results differ from TEMKIN results 17.09.2014 TU Darmstadt Ernst-Berl-Institute Prof. Dr. P. Claus Dominik Götz, M.Sc. 6

Validation Catalysis Experiments PFR results differ from TEMKIN results Different densities of the two active sites e.g. due to hotspots in PFR 17.09.2014 TU Darmstadt Ernst-Berl-Institute Prof. Dr. P. Claus Dominik Götz, M.Sc. 6

Validation Catalysis Experiments PFR results differ from TEMKIN results Different densities of the two active sites e.g. due to hotspots in PFR Adjustment of active site densities AS1 and AS2 Good agreement between experiment and simulation 17.09.2014 TU Darmstadt Ernst-Berl-Institute Prof. Dr. P. Claus Dominik Götz, M.Sc. 6

Performance Evaluation Original vs Advanced Version Thermal conditions inside the reactor Good heat transfer via pellet holders Nearly ideal isothermal behaviour 17.09.2014 TU Darmstadt Ernst-Berl-Institute Prof. Dr. P. Claus Dominik Götz, M.Sc. 7

Performance Evaluation Original vs Advanced Version Thermal conditions inside the reactor Good heat transfer via pellet holders Nearly ideal isothermal behaviour Mass transfer under reaction conditions Slow mass transfer due to dead zones Original version: Large dead zones before and after each catalyst pellet Advanced version: Only small dead zones after each catalyst pellet 17.09.2014 TU Darmstadt Ernst-Berl-Institute Prof. Dr. P. Claus Dominik Götz, M.Sc. 7

flow Performance Evaluation Benefits from Numerical Simulations Quick check and optimisation for new reactor or catalyst geometries 17.09.2014 TU Darmstadt Ernst-Berl-Institute Prof. Dr. P. Claus Dominik Götz, M.Sc. 8

flow Performance Evaluation Benefits from Numerical Simulations Quick check and optimisation for new reactor or catalyst geometries Checking the interaction between mass transport and kinetics under reaction conditions 17.09.2014 TU Darmstadt Ernst-Berl-Institute Prof. Dr. P. Claus Dominik Götz, M.Sc. 8

flow Conclusions Good agreement between experiment and simulation Simulations clearly confirms the benefits of our advanced reactor version COMSOL Multiphysics is a powerful tool for the development of new laboratory reactor systems 17.09.2014 TU Darmstadt Ernst-Berl-Institute Prof. Dr. P. Claus Dominik Götz, M.Sc. 9

Thank you for your attention! - Catalysis - Chemical Reaction Engineering - New Technologies - with the Claus group http://www.chemie.tu-darmstadt.de/claus/ 17.09.2014 TU Darmstadt Ernst-Berl-Institute Prof. Dr. P. Claus Dominik Götz, M.Sc. 10

2024 © sciencedocbox.com Privacy Policy | Terms of Service | Feedback