Hydrodesulfurization of Dibenzothiophene in a Micro Trickle Bed Catalytic Reactor under Operating Conditions from Reactive Distillation
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J. C. García-Martínez
Abstract
The hydrodesulfurization (HDS) of dibenzothiophene (DBT) is investigated over a commercial NiMoP/γ-Al2O3 catalyst in a micro trickled bed reactor (Micro-TBR) at operating conditions of a reactive distillation (RD) column. An analysis with and without reaction is carried out to have a first understanding on the complex interaction between kinetics and transport phenomena. A set of well-accepted criteria is evaluated to elucidate the presence of heat and mass transport limitations. Residence time distribution (RTD) experiments are performed to evaluate axial dispersion through the estimation of axial dispersion coefficient (Daxial,L) from a convection-dispersion model. Experiments with reaction are carried out using hydrogen and DBT as feedstock at reaction temperatures from 533 to 599 K, pressures from 1.5 to 2.5 MPa and inlet molar flow of DBT from 4 to 12×10–8 mol.s–1. A pseudo heterogeneous model accounting for mass transport limitations is used to describe experiments under reaction conditions. The main findings can be summarized as follows: most of RD operating conditions lead to the presence of interfacial mass transport limitations at both interfaces L-S and G-L; convection-dispersion model is able to describe satisfactorily RTD observations, suggesting that axial dispersion phenomena are negligible; conversion of DBT ranges from ca. 22 to 90% having a selectivity to by-product molecules from 30 to 80%, respectively; and the pseudo heterogeneous reaction model describes observations adequately obtaining activation energies ranging from 49 to 62 kJ mol–1 at pressures from 1.5 to 2.5 MPa, respectively. Estimated activation energies are comparatively lower than the activation energies reported in literature for the conventional HDS process, i.e. 40–160 kJ.mol–1, thereby suggesting an apparent catalytic energy savings by using RD technology.
Acknowledgments
Julio Cesar gratefully acknowledges CONACyT (México) for the grant with registry No. 179608 and IMP for the catalyst provided for the experiments.
Nomenclature
Roman Letters
- aB
interfacial area related to gas interface, m–1
- aL
interfacial area related to liquid interface, m–1
- as
interfacial area related to solid interface, m–1
- CL
tracer concentration at the exit of the vessel, kg.m–3
- C
tracer concentration, kg.m–3
- C0
inlet tracer concentration, kg.m–3
- Ci,G
concentration of the component i-th in gas phase, mol.m–3
- C i,L
concentration of component i-th in liquid phase, mol.m–3
- Ci,S
concentration of the component i-th in solid phase, mol.m–3
- Ck,n
n-th experimental response, mol.m–3
n-th predicted responses, mol.m–3
- dp
particle diameter, m
- dpi
inert particle diameter
- dr
reactor diameter, m
- Daxial,L
axial dispersion coefficient, m2.s–1
diffusion coefficient of component i-th in gas phase, m2.s–1
diffusion coefficients of component i-th in liquid phase, m2.s–1
- Deff
effective diffusion coefficient of component i-th into the catalyst particle, m2.s–1
- E
exit age distribution of the fluid, s–1
- Eθ
dimensionless exit age distribution, -/-
- Ea
activation energy, kJ.mol–1
- hi
heat transfer coefficient, W.m–2.K–1
- H
Henry’s constant based on solubility of component i-th in hexadecane, –/–
- Ki
adsorption constant of component i, m3.mol–1
- keff
bed effective radial conductivity, W.m–1.K–1
- kGL
overall interfacial mass transfer coefficient at the interface L-S, m.s–1
- kLS
overall interfacial mass transfer coefficient at the interface L-S, m.s–1
- kL
interfacial mass transfer coefficient at the liquid interface, m.s–1
- kp
effective thermal conductivity of the particle, W.m–1.K–1
- ks
interfacial mass transfer coefficients at solid interface, m.s–1
- L
reactor length
- M
mass of tracer into the fluid entering the reactor, kg
- nresp
number of responses
- QL
volumetric flow rate of the liquid phase, m3.s–1
- R
gas ideal constant, J.mol–1.K–1
- ri
apparent reaction rate of i-th component, mol.m–3.s–1
- t
time, s
- tavg
average residence time, s
- ti
tracer injection time, s
- Tr
reactor temperature, K
- uG
inlet superficial velocity of gas phase, m.s–1
- uL
inlet superficial velocity of the liquid phase, m.s–1
- V
reactor volume, m3
- wn
weight factor assigned to the n-th response
- z
axial dimension, m
Greek Letters
fraction of species adsorbed on catalyst active sites
- νn
stoichiometric coefficient of the i-th component
- ρG
density of gas fluid, kg.m–3
- ρL
density of liquid fluid, kg.m–3
- μG
dynamic viscosity of gas phase, kg.m–1.s–1
- μL
dynamic viscosity of liquid phase, kg.m–1.s–1
- ΔHr
reaction enthalpy, kJ.mol–1
Abbreviations
- ULSD
ultra-low-sulfur diesel
- HDS
hydrodesulfurization
- HYD
hydrogenation
- DDS
direct desulfurization
- RD
reactive distillation
- Micro-TBR
micro trickle bed catalytic reactor
- DBT
dibenzothiophene
- T
thiophene
- BT
benzothiophene
- 4,6-DMDBT
4,6-dymetildibenzothiophene
- DMDBT
dymetildibenzothiophene
- BP
biphenyl
- THDBT
tetrahydrodibenzothiophene
- CHB
cyclohexylbenzene
- BCH
bicyclohexyl. RTD, residence time distribution
- GC
gas chromatography
- FID
flame ionization detector
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©2016 by De Gruyter
Artikel in diesem Heft
- Frontmatter
- Editorial
- In Honour of Professor Serge Kaliaguine
- Research Articles
- Core/Shell Nanostructured Materials for Sustainable Processes
- Photodegradation Efficiencies in a Photo-CREC Water-II Reactor Using Several TiO2 Based Catalysts
- Hydrotreatment of Light Cycle Oil Over a Dispersed MoS2 Catalyst
- Hybrid Ionic Liquid-Chitosan Membranes for CO2 Separation: Mechanical and Thermal Behavior
- Photo-oxidation of Tributyltin, Dibutyltin and Monobutyltin in Water and Marine Sediments
- Contribution of Pd Membrane to Dehydrogenation of Isobutane Over a New Mesoporous Cr/MCM-41 Catalyst
- Self Diffusivity of n-Dodecane and Benzothiophene in ZSM-5 Zeolites. Its Significance for a New Catalytic Light Diesel Desulfurization Process
- Staggered Grid Finite Volume Approach for Modeling Single Particle Char Gasification
- High Efficiency CeCu Composite Oxide Catalysts Improved via Preparation Methods for Propyl Acetate Catalytic Combustion in Air
- Hydrodesulfurization of Dibenzothiophene in a Micro Trickle Bed Catalytic Reactor under Operating Conditions from Reactive Distillation
- Surface Modification of the ZnO Nanoparticles with γ-Aminopropyltriethoxysilane and Study of Their Photocatalytic Activity, Optical Properties and Antibacterial Activities
- One-Pot Isomerization of n-Alkanes by Super Acidic Solids: Sulfated Aluminum-Zirconium Binary Oxides
- Photocatalytic Decomposition of Metoprolol and Its Intermediate Organic Reaction Products: Kinetics and Degradation Pathway
Artikel in diesem Heft
- Frontmatter
- Editorial
- In Honour of Professor Serge Kaliaguine
- Research Articles
- Core/Shell Nanostructured Materials for Sustainable Processes
- Photodegradation Efficiencies in a Photo-CREC Water-II Reactor Using Several TiO2 Based Catalysts
- Hydrotreatment of Light Cycle Oil Over a Dispersed MoS2 Catalyst
- Hybrid Ionic Liquid-Chitosan Membranes for CO2 Separation: Mechanical and Thermal Behavior
- Photo-oxidation of Tributyltin, Dibutyltin and Monobutyltin in Water and Marine Sediments
- Contribution of Pd Membrane to Dehydrogenation of Isobutane Over a New Mesoporous Cr/MCM-41 Catalyst
- Self Diffusivity of n-Dodecane and Benzothiophene in ZSM-5 Zeolites. Its Significance for a New Catalytic Light Diesel Desulfurization Process
- Staggered Grid Finite Volume Approach for Modeling Single Particle Char Gasification
- High Efficiency CeCu Composite Oxide Catalysts Improved via Preparation Methods for Propyl Acetate Catalytic Combustion in Air
- Hydrodesulfurization of Dibenzothiophene in a Micro Trickle Bed Catalytic Reactor under Operating Conditions from Reactive Distillation
- Surface Modification of the ZnO Nanoparticles with γ-Aminopropyltriethoxysilane and Study of Their Photocatalytic Activity, Optical Properties and Antibacterial Activities
- One-Pot Isomerization of n-Alkanes by Super Acidic Solids: Sulfated Aluminum-Zirconium Binary Oxides
- Photocatalytic Decomposition of Metoprolol and Its Intermediate Organic Reaction Products: Kinetics and Degradation Pathway
