CFD Modelling of TBR 2

CFD MODELING OF TRICKLE BED REACTORS: Hydro-processing Reactor
Prashant R. Gunjal, Amit Arora and Vivek V. Ranade

Industrial Flow Modeling Group National Chemical Laboratory Pune 411008 Email: vvranade@ifmg.ncl.res.in
OUTLINE
Trickle Bed Reactors

Applications/ flow regimes Experiments
CFD Modeling of Trickle Bed Reactors

Inter-phase momentum exchange/ capillary terms Estimation of fraction of liquid suspended in gas phase
Simulating Hydro-processing Reactor

Reaction kinetics/ other sub-models Influence of reactor scale
Concluding Remarks
TRICKLE BED REACTORS Wide Applications

Hydro-de-sulfurization Hydro-cracking/ hydro-treating Hydrogenation/ oxidation Waste water treatment
Key Characteristics
Close to plug flow/ Low liquid hold-up Suitable for slow reactions Poor heat transfer/ possibility of mal-distribution Difficult scale-up
TRICKLE BED REACTORS

Liquid Gas
Gas & Liquid Flow through Void Space = 26-48 %
FLUID DYNAMICS OF TBR
Characterization of Packed Bed Wetting of Solid Surface by Liquid , P, L, , RTD Mal-distribution, Channeling & Mixing Flow Regimes & Global Flow Characteristics
FLOW REGIMES
EXPERIMENTS AT NCL
Pressure Indicator
101
Hydrodynamics
Pressure Drop Liquid Hold-up
Column with 3mm or 6mm Glass Beads

Data Acquisition
Conductivity Probes
Residence Time Distribution
Liquid Distribution at Inlet

Uniform Non-uniform
From Compressor
Separator Conductivity Probe
Pump
Liquid Tank
Experimental Parameters
Bed Diameter: Particle Diameter: Liquid Velocity: Gas Velocity: Tracer : 0.1 & 0.2 m 3 & 6 mm < 24 mm/ s < 0.50 m/ s NaCl
TYPICAL PRESSURE DROP DATA

35 30
Pressure gradient, KPa/m
Trickle flow regime
Pulse flow regime
25 20 15 10 5 0 0
10 20 Liquid Flow Rate, Kg/m 2s
30
PUBLISHED EXPERIMENTAL DATA

2 1.8 1.6 1.4 1.2 1 0.8 0.6 0.4 0.2 0 0 5 10 15 20 25 Liquid Velocity VL, (Kg/m2s)
2 L= ? Trickle Flow 1 3 L L Spray Flow
1. Szady and Sundersan (1991) 2. Rao et. al (1983) 3. Specchia and Baldi (1977)
Superficial Gas Velocity Vg, (m/s)
Pulse Flow L= ? L=L Bubbly Flow
MODELING OF MACROSCOPIC FLOW
Bed Porosity: Scale of Scrutiny

Bed diameter/ length: overall Intermediate scale: Gaussian distribution Smaller than particle diameter: Bi-modal distribution
Approach Used:
Experimentally measured or estimated radial variation of axially averaged bed porosity Specify porosity by drawing a sample assuming Gaussian distribution with specified variance
CHARACTERIZATION OF PACKED BED Radial Variation of Porosity: Mueller (1991)

(r ) = B + (1 B )J o (ar * )e br 12.98 for 2.61 D/d P 13.0 a = 8.243 (D/d P 3.156 ) a = 7.383 2.932 for 13.0 D/d P (D/d P 9.864 )
0.724 b = 0.304 D/d P r * = r/D and J o is zero th order Bessel Function

CHARACTERIZATION OF PACKED BED Muellers Correlation

Three data sets from literature
0.8 0.7 0.6 0.5
Szady and Sundersan (1991) Rao et.al. (1983) Spacchia and Baldi (1977)
Our experiments
0.7 0.6 0.5
D=0.194m, dp=3mm D=0.194m, dp=6mm
Porosity
0 0.2 0.4 0.6 0.8 1
Porosity
0.4 0.3 0.2 0.1 0 0 0.2 0.4 0.6 0.8 1
0.4 0.3 0.2 0.1 0
Dimensionless Radius
VARIATION OF BED POROSITY

0.56
With std dev=0
With std dev=5%
With std dev=10%
r/R
0.70
Selection of appropriate value is not straight forward: RTD may help

CFD MODEL Multi-fluid Model (Eulerian-Eulerian) Continuity Equation

K K + K KU K = 0 t
Momentum Balance Equation

( K KU K ) + ( K K U KU K ) = K P + t ( K U ) + K K g + FK , R (U k U R )
CFD MODEL Inter-phase Coupling Terms (Attou & Ferschneider, 2000)

FGL E (1 ) 2 = G 1 2 2G G d p L (1 G )
0.667
E 2 P (U G U L )(1 G ) L + Gd p (1 G )
0.667
0.333
FGS
E (1 ) 2 = G 1 2 2G G d p
S (1 G )
E U (1 G ) S + 2 P G Gd p (1 G )

0.333
E1 s 2 E2 PU G S FLS = L 2 2 + d Ld p L p
CFD MODEL Capillary Terms

1 1 PG PL = 2 d d 2 1
Attou and Ferschneider (2000)

1 PG PL = 2 1 G
0.333
0.5416 G F d P L
PG PL 2 5.416 s = z z 3 d p 1 G
2 / 3
1 1 G
G s s z + (1 )2 z G
G F L
CFD MODEL Capillary Terms

F G L = 1 + 88.1 G L for
G < 0.025 L
Extent of Wetting, f (Jiang et al., 2002)

PG PL = (1 f ) Pc
Scalar Transport
K K Ci + K KU K Ci = ( K K Di.mCi ) + Si t
SIMULATED RESULTS
Distributions within the bed
45 40 35
No n-prewetted B ed
P rewetted B ed
Contours of Liquid Hold-up
30 25 20 1 5 1 0 5 0 0 0.02 0.04 0.06 0.08 0.1 V e lo c it y M a gnit ude , m / s e c
35 30 25 20 1 5 1 0 5
No n-prewetted B ed P rewetted B ed
Pre-wetted
Un-wetted
0 0 0.1 0.2 Liquid Holdup 0.3
VL= 6 mm/ s, VG=0.22 m/ s, D=0.114 m, dP= 3 mm, =5%
SIMULATED RESULTS
Column Diameter = 0.114 m
Particle Diameter = 3 mm, VG=0.22 m/ s
SIMULATED RESULTS
VG= 0.22 m /s, D = 0.114 m
VG= 0.22 m /s, D = 0.194 m
GAS-LIQUID FLOW IN TBR Estimation of Frictional Pressure Drop & Fraction of Liquid Supported by Gas
Solid
P P = f ( LL g ) L GL L GL Q L L
Liquid Gas
Fraction of Liquid Hold-up Supported by Gas Phase < 1
Simulate at two values of g (9.7, 9.9 m/s2)

Pf L = P P g1 g2 L 2 L 1 g1 g 2
L = P P L 2 L 1 L (g 1 g 2 )
SIMULATED RESULTS
14
Pressure Gradient KPa/m
12 10 8 6
Saez and Corbonell (1985)-Exp. data Szady and Sundersan (1991)-Increase in liquid Szady and Sundersan (1991)-decrease in liquid CFD Simulations w ithout Capillary Force CFD Simulations
Calibrate Model Parameters from P

0.60
Holub et. al. (1993) -Experimental data Szady and Sundersan (1991)-Exp. Data CFD Results Supported Liquid Saturation
0.50
L
4 2 0 0.00
Liquid Saturation and
0.40
0.30
0.20
0.40
0.60
-1 2
0.80
1.00
Liquid Flow Rate x10 , Kg/m s
0.20
Can Predict Total and Supported Liquid Volume Fraction
0.10
0.00 0.00
0.20
0.40 0.60 0.80 -1 2 Liquid Flow Rate x10 , kg/m s
1.00
Operating conditions:VG=0.22m/s, D/dp =55, dp=3mm, Std. Dev.=5%, E1=215, E2=1.75
SIMULATED RESULTS
50
Pressure Drop, (KPa/m)
40 30 20
CFD Results Experimental Data
Data of Spachio & Baldi (1977)

0.5
L
10 0 0 0.2 0.4 0.6 0.8 1

Gas Flow Rate, (Kg/m 2s)
0.4
Liquid Saturation- CFD Results Supported Liquid Saturation Liquid Saturation- Exp. Data
0.3
0.2
As gas velocity increases, more & more liquid is supported by gas
0.1
0 0 0.2 0.4 0.6 Gas Mass Velocity, kg/m2s 0.8 1
Operating conditions: VL=2.8x10-3 m/s, dp=3mm, D/dp=30, Std. Dev.=5%, E1=500, E2=3
SIMULATED RESULTS
200 Pressure Drop, (KPa/m) 160 120 80
L
Experimental Data CFD Results
Data of Rao et al. (1983)

0.2
40
0.16
Liquid Saturation- CFD Results Supported Liquid Saturation Liquid Saturation Exp. Data
0 0 2 4 6 8 Gas Mass Velocity, (kg/m2s)
0.12
0.08
As gas velocity increases, more & more liquid is supported by gas
0.04
0 0 2 4 6 8
Gas mass velocity, Kg/m2s
Operating conditions:VL=1x10-3m/s, D/dp =15.4, dp=3mm, Std. Dev.=5%, E1=215, E2=3.4
RESIDENCE TIME DISTRIBUTION

0.12 0.1 0.08 E(t), sec
-1
1 2 1 2 2
Pre-wetted Bed Non Pre-wetted Bed
Simulation Results Experimental Results
0.06 0.04
0.02 0 0 20 40 60 Time, (sec) 80 100 120
Operating conditions: VL=2.06x10-3m/s VG=0.22m/s, D/dp =18, dp=6mm, Std. Dev.=5%, E1=180, E2=1.75
MODELING OF HYDRO-PROCESSING REACTOR
Reaction and Kinetics (Chowdhury et al. 2002)

Hydro-desulfurisation (HDS)
Ar S + 2H2 Ar + H2S
rHDS =
0 56 6 k c L ,.H 2 c 1 .,S L
1 + K Ad c L ,H 2 S
De-aromatisation of Mono-, Di- and Poly- Aromatics

Mono Ar + 3H2 Napthenes Di Ar + 2H2 Mono Ar Tri Ar + H2 Di Ar
rMono = kMonoCMono + k _ MonoCNaph rDi = k Di C Di + k _ Di C Mono

rPoly = k Poly C Poly + k _ Poly C Di
SIMPLIFICATIONS/ ASSUMPTIONS
Pressure drop is insignificant compared to the operating pressure Trickle bed reactor is operated isothermally (efficient heat transfer) Ideal gas law is applicable Liquid phase reactants are non-volatile (negligible vapor pressure) Gas-liquid mass transfer is the limiting resistance. The catalyst particles are completely wetted
MODEL EQUATIONS
Mass Balance of Species i
k k Ck , i t + ( k kU k Ck ., i ) = ( k k Di , mCk , i ) + k k Si , k
Source Terms for Gas Phase

C S i = K GLi a GL Gi C Li Hi
Source Terms for Liquid Phase

j= nr CGi C Li + B rij S i = K GLi aGL Hi j=1
S i = B rij
j=1
j= nr
MODEL EQUATIONS Mass Transfer Coefficient (From Goto & Smith, 1975)
L G ki aL = 1 L DiL L
L DL L i
1/ 2
Solubility of Hydrogen/ H2S (Korsten et al. 1996)

Hi =
H2
N i . L
: molar gas volume

a 0 = 0.559729 a 1 = 0.42947 10 3 a 2 = 3.07539 10 3 a 3 = 1.94593 10 6 a 4 = 0.835783
T 1 = a 0 + a 1T + a 2 + a 3T 2 + a 4 . 2 20 20
H S = exp(3.3670 0.008470 .T )
2
CASE STUDIES Gas and Liquid Superficial Velocities Increase with Scale Wetting gets Better with Scale
Parameters Reactor Diameter, m Bed Length Particle Diameter, m Bed Porosity LHSV, h-1 Operating Pressure, Mpa Operating Temperature, K Initial H2S Conc., v/v % Laboratory Scale Reactor (Chowdhury et al. 2002) 0.019 0.5 m 0.0024 0.50 1-5 20-28 573-693 0.5-8 Commercial Scale Reactor (Bhaskar et al. 2004) 3.8 16 m 0.0015 0.36 1-5 20-80 573-693 0.5-8
KINETICS/ OIL COMPOSITION From Chowdhury et al. (2002)

Kinetic Constants
K Ad , m3/kmol
Values 50000 2.5 X 1012 exp(-19384/T) 6.04 X 102 exp(-12414/T) 8.5 X 102 exp(-12140/T) 2.66 X 105 exp(-15170/T) Percentage 1.67 2.59 8.77 17.96 19.25
K, Dimensionless k*mono, m3/kg.s k*Di, m3/kg.s k*poly, m3/kg.s Component Ar-S % Poly-Ar % Di-Ar % Mono-Ar % Naphthenes %
SIMULATED RESULTS-1
100
90
75
Varying Porosity
Conversion, Ar-S %
Ar-S Exp
50
Conversion, x
Uniform Porosity
60
30
25
0 573
0
583 593 603 613 623 633 643 653
Temp, K
Initial H2S Conc Gas Phase ( %, V/V)
Temperature
Initial Concentration of H2S
(P=4 MPa, LHSV=2.0 h-1, QGNTP/QL=200 m3/m3, TR=320oC, yH2S=1.4% ) Symbols denote experimental data of Chowdhury et al. (2002)
SIMULATED RESULTS-2
90 80 70 Conversion, % 60 50 40 30 20 10 0 573 593 613 Temperature, K 633 653
60
Ar-P total total poly

50
A r-D
A r-M
A r-Di-Expt
Conversion, %
A r-Mono-Exp
40
30
20
10
0 573 593 613 633 653
Temperature, K
(P=4 MPa, LHSV=2.0 h-1, QGNTP/QL=200 m3/m3, yH2S=1.4%) Symbols denote experimental data of Chowdhury et al. (2002)
SIMULATED RESULTS-3
60
Total-Ar
50
Ar-Poly Ar-Di Ar-Mono
Conversion, %
40 30 20 10 0 2 2.4 2.8 3.2 3.6

-1
LHSV, h
(P=4 MPa, TR=320 oC, QGNTP/QL=200 m3/m3, yH2S=1.4%, filled symbols are for experimental data of Chowdhury et al., 2002)
INFLUENCE OF REACTOR SCALE
1.6
35 1.6 7
1.4
30
1.4
Dimensionless Solid Hold-up
25 1 20 0.8 15 0.6 10
1.2 5 1 4 0.8 3 0.6 2
0.4
Solid hold-up Local Axial Velocity
0.4
Solid hold-up Local Axial Velocity
0.2
5 0.2 0 0 0.2 0.4 0.6 0.8 1
0 0 0.2 0.4 0.6 0.8 1
Laboratory (LHSV=3)
Industrial (LHSV=2)
(P=4 MPa, TR=320 oC, QGNTP/QL=300 m3/m3)
Dimensionless Local Axial Velocity
1.2
Dimensionless Local Axial Velocity
Dimensionless Solid Hold-up
100
12000 Outlet Conc. Ar-S, ppm 10000 8000 6000 4000 2000
Lab S c ale Reactor
Com m ercial Reactor
Conversion, %
75
Lab-scale Reactor Commercial Reactor
50
25 573
0
593 613 633 653
573
593
Temperature, K
613 633 Temperature, K
653
(Plab & com=4 & 4.4 MPa, LHSVlab=2.0 h-1, QGNTP/QL=200 m3/m3, yH2S=1.4%)
100 80 Conversion, % 60 40 20 0 -20 573

Poly-Ar Total Poly-Ar-Commercial Total-Commercial
100 95 90 Conversion, % 85 80 75 70 65 60 55 50
593 613 Temperature, K 633 653
Ar-S-Lab Scale Ar-S-Commercial
2.5
3 LHSV, h-1
3.5
(Plab & com=4 & 4.4 MPa, LHSVlab & com=2.0 & 3.0 h-1, (QGNTP/QL)lab & com= 200 & 300 m3/m3, yH2S=1.4%)
(Plab & com=4 & 4.4 MPa, Temperature= 593 K, (QGNTP/QL)lab & com= 200 & 300 m3/m3, yH2S=1.4%)

120
100
Poly-Ar
90 80
Poly-Ar Di-Ar Mono-Ar Total
100
Di-Ar
Mono-Ar
Total
Conversion, %
Conversion, %
80
70 60 50 40 30 20
60
40
20
10
0 2 3 4 5 Pressure, MPa 6 7 8
0 2 2.5 3 -1 LHSV, h 3.5 4
(QGNTP/QL)lab & com= 200 & 300 m3/m3 T=593 K LHSVlab & com=2.0 & 3.0 h-1 ,yH2S=1.4%
Plab & com=4 & 4.4 Mpa, T=593 K yH2S=1.4% (QGNTP/QL)lab & com= 200 & 300 m3/m3
Continuous lines: commercial; Dotted lines: laboratory scale
CONCLUDING REMARKS Macroscopic CFD Model Reasonably Simulates Gasliquid Flow in Trickle Beds
Liquid hold-up Residence time distribution May be used to estimate fraction of suspended liquid
Further Work is Needed for Understanding Wetting/ Hysteresis to Make Further Progress Despite Limitations, CFD Models can be Used to Understand Key Issues in Reactor Engineering Including Scale-up & Scale-down
MODELING OF MESO-SCALE FLOWS Single Phase Flow through Packed Bed

Unit cell approach Simple cubic, FCC, rhombohedral .. Inertial flow structures, pressure drop, heat transfer
Interaction of Liquid Drop/ Film with Solid Surface

Regimes of interaction Dynamic contact angle/ surface characteristics VOF simulations Insight into capillary forces???
SINGLE PHASE FLOW Single Phase Flow through Packed Bed

Periodic Flow Periodic Flow
Wall Wall Wall
Operating Parameters
Cell Length Fluid Particle Reynolds Number 28mm, 3mm Water 12-6000
SINGLE PHASE FLOW

5
Experiments:
0
Suekane et al. AIChE J., 49, 1
4.5
Simulations
SINGLE PHASE FLOW

3
Experiment al Simulat ion-28mm Simulat ion-3mm
4
Experiment al
Simulat ion-28mm
Simulat ion-3mm
Vz/Vmean
Vz/Vmean
0 -1
5
Experimental
-1
-0.5
x/r
0.5
-1
-0.5
0.5
x/r
5
Experimental
4 3
Simulation-28mm Simulation-3mm
4 3 2 1 0 -1
Simulation-28mm Simulation-3mm
Vz/Vmean
2 1 0 -1 -1 -0.5 0 x/r 0.5 1
Vz/Vmean
-1
-0.5
x/r
0.5
SINGLE PHASE FLOW
Vz=8.66mm /s
S
Max arrow length : A=0.26 mm/s B=0.29 mm/s C=0.44 mm/s
A: z/r=0.14 (experimental)
B: z/r=0.28 (experimental)
C: z/r=0.42 (experimental)
SINGLE PHASE FLOW Inertial Flow Structures were Captured Accurately by CFD Models Velocity Distribution in Unit Cells Resembles that in a Packed Bed Ergun Parameters may be Obtained through Unit Cell Approach for Semi-structured Packed Bed Unit Cell Approach may be Extended to Simulate Two Phase Flows to Understand Wetting
LIQUID SPREADING ON SOLID SURFACES

Monitor Computer
Light Diffuser
Drop Rest on Flat Plate
Light
8.79mm 1mm
10.4mm
Drop Flow Over Pellet
CCD Camera
DROP IMPACT ON SOLID SURFACE
DROP IMPACT ON SOLID SURFACE
FLAT SURFACE
t=0ms
t=45ms
t=0ms t=36ms
(a)
(d)
t=10ms
t=45ms
t=16ms
t=48ms
(b) (e) t=25ms
t=210ms
t=20ms
t=240ms
(c) (f)
DYNAMICS OF DROP IMPACT
MODELS FOR INTERPHASE COUPLING?
Drop Shape at 12 ms
Wall Shear Stress on Solid Surface, red~100 Pa
Shear Strain on Gas-liquid Interface


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CFD MODELING OF TRICKLE BED REACTORS: Hydro-processing Reactor

Prashant R. Gunjal, Amit Arora and Vivek V. Ranade

Trickle Bed Reactors

CFD Modeling of Trickle Bed Reactors

Simulating Hydro-processing Reactor

TRICKLE BED REACTORS Wide Applications

TRICKLE BED REACTORS

Gas & Liquid Flow through Void Space = 26-48 %

CFD Modeling of Trickle Bed Reactors

FLUID DYNAMICS OF TBR

CFD Modeling of Trickle Bed Reactors

CFD Modeling of Trickle Bed Reactors

Column with 3mm or 6mm Glass Beads

Liquid Distribution at Inlet

Separator Conductivity Probe

CFD Modeling of Trickle Bed Reactors

TYPICAL PRESSURE DROP DATA

10 20 Liquid Flow Rate, Kg/m 2s

CFD Modeling of Trickle Bed Reactors

PUBLISHED EXPERIMENTAL DATA

Superficial Gas Velocity Vg, (m/s)

Pulse Flow L= ? L=L Bubbly Flow

CFD Modeling of Trickle Bed Reactors

MODELING OF MACROSCOPIC FLOW

Bed Porosity: Scale of Scrutiny

CHARACTERIZATION OF PACKED BED Radial Variation of Porosity: Mueller (1991)

0.724 b = 0.304 D/d P r * = r/D and J o is zero th order Bessel Function

CHARACTERIZATION OF PACKED BED Muellers Correlation

0.4 0.3 0.2 0.1 0 0 0.2 0.4 0.6 0.8 1

0.4 0.3 0.2 0.1 0

CFD Modeling of Trickle Bed Reactors

VARIATION OF BED POROSITY

With std dev=0

With std dev=5%

With std dev=10%

Selection of appropriate value is not straight forward: RTD may help

CFD MODEL Multi-fluid Model (Eulerian-Eulerian) Continuity Equation

Momentum Balance Equation

CFD Modeling of Trickle Bed Reactors

CFD MODEL Inter-phase Coupling Terms (Attou & Ferschneider, 2000)

CFD Modeling of Trickle Bed Reactors

CFD MODEL Capillary Terms

Attou and Ferschneider (2000)

CFD Modeling of Trickle Bed Reactors

CFD MODEL Capillary Terms

Extent of Wetting, f (Jiang et al., 2002)

Contours of Liquid Hold-up

30 25 20 1 5 1 0 5 0 0 0.02 0.04 0.06 0.08 0.1 V e lo c it y M a gnit ude , m / s e c

0 0 0.1 0.2 Liquid Holdup 0.3

VL= 6 mm/ s, VG=0.22 m/ s, D=0.114 m, dP= 3 mm, =5%

CFD Modeling of Trickle Bed Reactors

Column Diameter = 0.114 m

Particle Diameter = 3 mm, VG=0.22 m/ s

CFD Modeling of Trickle Bed Reactors

VG= 0.22 m /s, D = 0.114 m

VG= 0.22 m /s, D = 0.194 m

CFD Modeling of Trickle Bed Reactors

Fraction of Liquid Hold-up Supported by Gas Phase < 1

Simulate at two values of g (9.7, 9.9 m/s2)

CFD Modeling of Trickle Bed Reactors

Calibrate Model Parameters from P

Liquid Saturation and

Liquid Flow Rate x10 , Kg/m s