Chemical Reaction Engineering
Reactor Design
Jayant M. Modak Department of Chemical Engineering Indian Institute of Science, Bangalore
Chemical Reactor Design
Objectives
q
Technological
n n n
Maximum possible product in minimum time Desired quantity in minimum time Maximum possible product in desired time Maximize profit
Economic
n
Chemical Reactor Design
Constraints
q
Market
n n
Raw materials availability quality and quantity Demand for the product Safety Pollution control Thermodynamics Stoichiometry Kinetics
Society/Legislative
n n
Technological
n n n
Chemical Reactor Design - Decisions
Type
q
of reactor
Tubular, Fixed Bed, Stirred tank, Fluidized bed Mass Flow: Batch, Continuous, Semibatch Energy: Isothermal, Adiabatic, Co/counter current
Mode
q q
Process
q
Intensification
Combining more than one type of unit operation
Tubular reactor mass balance
C j C j
+ ( Flux j ) = R j t z
+ ( uC j + J j ) = R j t z
M jC j + u M jC j + M j J j = M j R j t j j z j j f + ( u f ) = 0 t x
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Tubular reactor energy balance
1 (CTU ) + FT H + A H j J j = Q t A z j C j T (CTU ) = (CT H P ) = H j + C jCPj t t j t j t F j T ( FT H ) = H j + FjCPj z j z j z J j H j + J j H jJ j = H j z j j z j z
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Tubular reactor energy balance
J j C j 1 F j + +A H j = H j R j = H i ri z j j t A z i T T +u C jCPj u j t 4 Q = U (Tr T ) dt T T 4 + u + H i ri = U (Tr T ) C jCPj u i dt j t
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Stirred tank reactor mass and energy balance
dN j dt
= Fj 0 F je + R j
dT = F j 0 ( H j 0 H je ) + V ( H i ) ri + AKU (Tr T ) N jCPj j i j dt
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Fixed bed reactor mass balance
( BC j ) + z ( B Flux j ) = qmj t Cj ( BC j ) + z usC j Dej,s f z t f
= qmj
T T 2T 4 + us e 2 + qh = U (Tr T ) C jCPj z z dt j t
( Dej,r , C j ) 1 Y rX ( X ,Y ) = r r (e,r , T )
Psuedohomogenous model
qmj = R j qh = H i ri
i
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Heterogenous model external diffusion
qmj = K g (C j C js )gngAp = K g av (C j C js ) 3 av = (1 B ) R qh = h f av (T Ts )
h f av (T Ts ) = H i ri
i
K g av (C j C js ) = R j (C js , Ts )
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Heterogenous model internal diffusion
2 ' C 'j 1 r Dej 2 r r r ' ' ' = R j (C j , T )
2 ' T ' 1 ' r e = H i ri r 2 r r i
' qmj = Dej
C 'j r
r=R
av = R j ( C j )
qh = i ( H i ) ri
i
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Non-isothermal reactors - PFR
2.0 1.5 1.0
Adiabatic Isothermal
Concentration
0.5 0.0 2 1 0 0.0
Concentration temperature
10
20
30
40 350 325 300 4.0
0.5
1.0
1.5
2.0
2.5
3.0
3.5
Time (min)
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Non-isothermal reactors - CSTR
Concentration Temperature
340 320 300 2.0 1.5 1.0 0.5 0.0 0.0 0.2 0.4 0.6 0.8 1.0 1.2 1.4 1.6 1.8 2.0
Residence time
Non-isothermal reactors - rate
8 6
r1
1/rate
4 2 0 0.0
0.5
1.0
1.5
2.0
C10-C1
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Trajectories - Exothermic reaction
1.0
Isothermal
0.8 0.6
Xeq
Adiabatic
0.4 0.2 0.0 300 320 340 360 380 400
T
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Trajectories - Endothermic reaction
1.0 0.8 0.6
Xeq
Adiabatic Isothermal
0.4 0.2 0.0 300 320 340 360 380 400
T
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Optimal temperature trajectories
10 1
Rate
0.1
0.01 0.0
0.2
0.4
0.6
0.8
100 1.0 10
conversion
1/rate
1 0.1 0.01 0.0
0.2
0.4
0.6
0.8
1.0
conversion
Optimal temperature
500 0.9 450
0.8
400
0.7
350 300
0.6
Extent
0.5
250
0.4
200 150
0.3
0.2
100
0.1
50
450
500
550
600
650
700
Temperature K
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Thermal cracking of ethane in tubular reactor
Ethylene demands polyethylene, ethylene oxide, ethylene glycol 20 million tons per annum Main Reaction C2 H6 C2 H4 + H2 increase in number of moles so steam as inert Endothermic reaction - H 34.5 kcal/mol, high temperature for high equilibrium conversions, increasing temperatures along the length of the reactor Side reactions higher conversion yield of side products higher
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2C2 H6 C3 H8 + CH 4
Yield conversion diagram for ethane cracking
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Ethane cracking reactor
Typical operating condn L = 95 m G = 68.68 kg/m2/s P inlet 2.99 atm, outlet 1.2 atm T inlet 680, outlet 820 C Production 10000 tons/coil
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Balances
mass energy dF j
d t2 = Rj dz 4
d t2 q( z ) d t + ( H i )ri 4 i
dT 1 = dz F jC pj
j
dp 2 f du momentum = + f u2 + f u dz d t rb i dz RT F j F' 1 j u= = A A p
Simulation of ethane reactor
Hydrogenation of oil
Major demand margarine, shortenings, vanaspati Vegetable oils mixture of triglycerides - glycerol and fatty acids Fatty acids saturated (S) , monosaturated (cis, R1 and trans, R2) and diunsaturated (B). Hydrogenation to reduce odor or color, improve stability and increase melting point. Product requirements some polyunsaturated (health) and R2 ( consistency and higher melting points)
Reactions
r1 r4 C , r5 r6 CH 2
1/ 2 H2
implies selectivity of monounsaturates over saturates proportional to (CH2)1/2
Yield conversion diagrams
Balances
dC j
mass
dt k Lav CH 2 , g CH 2 ,s = RH 2 C j , CH 2 ,s
= Rj
j = B, R1 , R2 , M
) )
dCH 2 ,b
dt 0 = k S aS CH 2 ,b CH 2 ,s + RH 2
= k L a v C H 2 , g C H 2 ,b k S a S C H 2 ,b C H 2 , s
1 1 1 = + k L av k L av k S a S
Stirred tank batch reactor
Desired conversion batch time Desired production rate and batch time volume Based on volume internal design Cooling load
Q = V ( Hi )ri = AKU (T Tr )
i
Ammonia synthesis
Major
demand Fertilizer, chemicals, explosives, polyamides, pharmaceuticals; 150 million tons per annum Main reaction
1 3 N 2 + H 2 ! NH 3 , !H 298 K = "45.7 kJ / mol "1 2 2
High
pressure, low temperatures favorable Catalytic reaction iron, promoted ruthenium
Ammonia synthesis equilibrium
1.0 0.9
1.0
Ammonia Mol fraction
Ammonia Mol fraction
0.8 0.7 0.6 0.5 0.4 0.3 0.2 0.1 0.0 500
1
P = 300 atm
(A)
0.9 0.8 0.7 0.6 0.5 0.4 0.3 0.2 0.1 0.0 0
(B)
T = 473 K 523 573 623 673 723 773
200 100 50
10 3
600
700
800
900
100
200
300
Temperature (K)
Pressure (Atm)
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Ammonia synthesis - balances
mass energy us dC j dz = R j (C j ,T )
dT 4U f us c p = (Tr T ) + ( H ) r dz dt 1 d 2 dCi' r Die = Ri ( Ci' , T ' ) r 2 dr dr 1 d 2 dT ' r e = H r 2 r dr dr
catalyst
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Reactor simulation
0.7 0.6
mol fraction
0.4 0.3 0.2 0.1 0.0 0 1 2 3
H2 NH3
temperature
0.5
N2
860 840 820 800 780 760 740 720 700 680
Length (m)
Length (m)
120 100 80
rate at bulk conditions observed rate
rate
60 40 20 0 0 1 2 3 4 5
Length (m)
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Optimal temperature
500 0.9 450
0.8
400
0.7
350 300
0.6
Extent
0.5
250
0.4
200 150
0.3
0.2
100
0.1
50
450
500
550
600
650
700
Temperature K
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Fixed bed reactors
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Ammonia Multibed reactor
1.0
Conversion
0.8 0.6 0.4 0.2 0.0 400
r=0 r/ T=0 Reactor 1 Reactor 2 Reactor 3
500
600
700
800
900
Temperature
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Fixed bed reactors
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Ammonia Autothermal
300 250 200
Ttop-T1L Ttop-Tfeed 473 491 513 523 578 623
1000 900 800
150 100 50 0 400
Tfeed K
700 600 500
500
600
700
800
900
1000
400 400
500
600
700
800
900
1000
Ttop
Ttop K
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Ammonia Autothermal
800 750
0.8 0.7 0.6 0.5 0.4 0.3 0.2 0.1 0.0
Conversion
700
Conversion
650 600 550 500 0 1 2 3 4 5 6
r=0 r/ T=0
reactor heat exchanger
600
650
700
750
800
850
900
Length
Temperature
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Process intensification
Strategy
of reduction in physical size of a chemical plant while achieving given objective 30 40 years old concept, reinvented in last decade due to intense competition, scarce resources and stricter environmental norms Multifunctional reactive systems several functions are designed to occur simultaneously. Major drive in refining and petrochemicals sector
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Catalyst particle in reacting media
Type A at catalyst level Type B at interphase transport level Type C at intra-reactor level separations/heat transfer Type D inter-reactor level by combining two reactor operation with solids recirculation.
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Type A Example bifunctional catalysis
Catalytic
reforming to increase the octane
number Conversion of parafins, cyclo parafins and napthenes to aromatics and branced paraffins. Reactions involved dehydrogenation, cyclization and isomerization Pt/SiO2 catalyst
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Type B Example Gas induction reactors
DRAFT TUBE STATOR GASLIQUID DISPERSION
GAS ENTRANCE
DRAFT TUBE
STATOR GAS -LIQUID DISPERSION DISPERSING IMPELLER
SELF INDUCING IMPELLER
SUSPENDING IMPELLER
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Type C Intra-reactor operation
Energy
transfer reaction in heat exchanger Momentum transfer radial flow reactors Mass transfer reactive- distillation, absorption
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Type C Momentum transfer
High
gas flow rates ammonia synthesis, styrene from ethylbenzene, flue gas treatments
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Type C Mass transfer
Enhance
conversion in equilibrium limited reaction, prevent undesirable reaction, increase rate of product inhibited reactions
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Type C Energy transfer
CH 4 + H 2O CO + 3H 2 CH 4 + 2O2 CO2 + 2 H 2O H = 206 kJ / mol
Temperature
0.30 0.25 0.20 0.15 0.10 0.05 0.00 0 1 2 3 4 5 6
H = 803 kJ / mol
Flue gas Process
Length
840
Temperature
800 760 720 680 640 0 1 2 3 4 5 6
Flue gas Process
Length
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Type C Example styrene synthesis
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Design considerations and safety
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Multiplicity in stirred tank reactor
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Explosion in batch reactor
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Runaway/Hot spot in tubular reactor
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Runaway/Hot spot in tubular reactor
0.020
800
0.012 0.015 0.016 0.0175 0.0176 0.0181
0.012 0.015 0.016 0.0175 0.0176 0.0181
partial pressure
0.015 0.010 0.005 0.000 0.0
temperature
700
600 0.0 0.2 0.4 0.6 0.8 1.0 1.2 1.4
0.2
0.4
0.6
0.8
1.0
1.2
1.4
Length
Length
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Runaway/Hotspot in tubular reactors
0.020
Partial pressure
0.016 0.012 0.008 0.004 610 620 630
Sensitive
Insensitive
640
650
660
temperature
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q < p2 / 4 1,2 = 1, 2
'' < 0
q > p2 / 4 1,2 = i
<0
q=det (A)
q = p2 / 4
q > p2 / 4 1,2 = i
>0
2
q < p2 / 4 1,2 = 1, 2
1 > 0, 1 > 2
q < p /4 1,2 = 1, 2 > 0
p=tr (A)
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Stability analysis
A
state X=0 is said to be stable when given e>0, there exists a d>0 (0<d<e) such that if ||X (0)||<d then ||X(t)|| < e for all t>0 A state X=0 is said to be asymptotically attractive when given m>0, such that if ||X(0)|| <m then lim (t) ||X(t)|| =0 A state is asymptotically stable when stable and asymptotically attractive. A state is marginally stable when stable but not asymptotically attractive
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Examples
x2 ( y x ) + y5 dx = dt 1 + x 2 + y 2 + ( x 2 + y 2 )2 y2 ( y 2x) dy = dt 1 + x 2 + y 2 + ( x 2 + y 2 )2
1.0 0.8 0.6 0.4 0.2 0.0 0.0 0.2 0.4 0.6 0.8 1.0
dx =y dt dy = x dt
1.2 1.0 0.8 0.6 0.4 0.2 0.0 -0.2 -0.4 -0.6 -0.8 -1.0 -1.2 -1.2-1.0-0.8-0.6-0.4-0.2 0.0 0.2 0.4 0.6 0.8 1.0 1.2
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Two dimensional system - Eigen values
2 T + D = 0
T T2 1,2 = D 2 4
D=determinant(A)
T /4-D=0
Stable focus Stable node
0
Unstable focus Unstable node
T=trace(A)
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D=determinant(A)
Unstable node
= 0.1 D = 0.00971, T = 0.988
45 40 35 30 25 20 15 10 -50 0 50 100 150 200 250 300 350 0.10 0.08 0.06
T /4-D=0
= 0.0099,0.9782
Stable focus Stable node
0
Unstable focus Unstable node
T=trace(A)
alpha
beta
0.04 0.02 0.00 -50 0 50 100 150 200 250 300 350
Time
Time
0.10 0.08 0.06
beta
0.04 0.02 0.00 10 20 30 40 50
alpha
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Unstable focus
= 0.5 D = 0.248, T = 0.751
350 300 250 200 3.0 2.5 2.0
D=determinant(A)
T /4-D=0
Stable focus Stable node
0
Unstable focus Unstable node
= 0.3756 0.3276i
beta
1.5 1.0 0.5
T=trace(A)
alpha
150 100 50 0 -50 -50 0 50100 200 300 400 500 600 700 150 250 350 450 550 650 750
0.0 -50
50
100
150
200
250
300
350
Time
Time
3.0 2.5 2.0
beta
1.0 0.5 0.0 -10 0 10 20 30
beta
1.5
10 8 6 4 2 0 -2 -4 -6 -8 -10
linearized process real process
10 12 14 16 18 20
alpha
alpha
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D=determinant(A)
Stable focus
= 2.0 D = 3.99, T = 2.98 = -1.4900 1.3288i
0.80 0.75 0.70 2.1 2.0 1.9 1.8
T /4-D=0
Stable focus Stable node
0
Unstable focus Unstable node
T=trace(A)
alpha
beta
0 50 100 150 200 250 300 350
0.65 0.60 0.55 0.50 0.45 -50
1.7 1.6 1.5 1.4 -50 0 50 100 150 200 250 300 350
Time
Time
2.1 2.0 1.9 0.3 0.2
1.7 1.6 1.5 1.4 0.45 0.50 0.55 0.60 0.65 0.70 0.75 0.80
alpha
1.8
beta
0.1 0.0 -2 0 2 4 6 8 10
alpha
alpha
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D=determinant(A)
Stable node
= 2.5 D = 6.23, T = -5.21
0.65 0.60 2.5 2.4 2.3 0.55 0.50 0.45 0.40 -50 0 50 100 150 200 250 300 350
T /4-D=0
= -3.3614, -1.8525
Stable focus Stable node
0
Unstable focus Unstable node
T=trace(A)
alpha
beta
2.2 2.1 2.0 1.9 1.8 -50 0 50 100 150 200 250 300 350
Time
Time
2.5 2.4 2.3
beta
2.2 2.1 2.0 1.9 1.8 0.40 0.45 0.50 0.55 0.60 0.65
alpha
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D=determinant(A)
Limit cycle
= 1.005
1.6 1.4 1.2
T /4-D=0
D = 1.01, T = 0
1.5 1.4 1.3 1.2 1.1 1.0 0.9 0.8 0.7
= 1.003i
Stable focus Stable node
0
Unstable focus Unstable node
T=trace(A)
alpha
1.0 0.8 0.6 -50 0 50 100 150 200 250 300 350
beta
-50
50
100
150
200
250
300
350
Time
Time
1.5 1.4 1.3 1.2 1.1 1.0 0.9 0.8 0.7 0.6 0.8 1.0 1.2 1.4 1.6
beta
alpha
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Adiabatic CSTR
100 80
Heat generation Heat removal =60 s =10 s = 100 s
rate
60 40 20 0 0 1
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Adiabatic CSTR steady state multiplicity
1.0 0.8 10 8 6
Steady state 0.08996, 0.61698
temperature
Eigenvalue s 1.6710-2 , 8.6810-3 1.6710-2 7.0510-3 1.7410-2 1.6610-2
conversion
0.6 0.4 0.2 0.0
conversion temperature 2
0 40 80 120 160 200 0
0.4957 3.4 0.7628 5.2318
residence time
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Adiabatic CSTR phase plane, transient
14 12 10
Temperature
8 6 4 2 0 0.0 0.2 0.4 0.6 0.8 1.0
Conversion
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Non-ideal flow, mixing and reactions
If, we know precisely what is happening within the vessel, thus, if we have a complete velocity distribution map for the fluid in the vessel, then we should, in principle, be able to predict the behavior of a vessel as a reactor. Unfortunately, this approach is impractical, even in today s computer age. Levenspiel, Chemical Reaction Engineering, 1999. Mobil Adds Million-Dollar Benefits by Using Flow Simulation to Optimize Refinery Units, Greg Muldowney, Mobil Technology Company, 2007
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CFD modeling of bioreactors
Bioreactor
q
performance: interactive relation between biosystem and physical environment
Biotic phase: complex machinary inside cell and its regulation by external environment Abiotic phase: multiphase system with complex interactions of mass, momentum and energy leading to environmental gradients in space and time
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Anaerobic digestion
Complex polymers
Fermentative B.
HYDROLYSIS and ACIDOGENESIS
Monomers
20 76
Acidogenic B.
Volatils fatty acids (VFA), alcohols, ...
ACETOGENESIS
Acetogenic B.
Acetate
METHANOGENESIS
52
24
CO2 + H2
28
72
Homoacetogenic B. Hydrogenophilic B. Acetoclastic B.
CH4 + CO2
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CH +H O
CFD modeling of anaerobic bioreactor
Biogas out
1
0.15
Gas
0.15
1.2
Leafy biomass Treated water out water
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Waste water in
y
1.4
Results & Discussion
Vector plot for liquid velocity (m/s) (with Packed bed)
Contour plot for liquid velocity (m/s) (with Packed bed) Indian Institute of Science
PIV experiments
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Experimental verification
Contours of X-direction mean velocity (inlet NRe=7660) (a)experimental and (b ) Simulation results without packed bed
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Experimental verification
Contours of X-direction mean velocity (inlet NRe=500) (a)experimental and (b ) Simulation results with packed bed
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Improving the performance
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Non-ideal flow, mixing and reactions
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Non-ideal flow, mixing and reactions
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Non-ideal flow, mixing and reactions
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Residence time distributions
Exit
q
age distribution E(t)dt
Fraction of material in exit stream which has age between t and t+dt
Cumulative
q
residence time distribution, F(t)
Fraction of material in exit stream with age less than t
Internal
q
age distribution, I(t)dt
V 1 F (t ) = I (t ) F'
dF (t ) F (t ) = E (t ')dt ' or = E (t ), dt 0
Fraction of material within vessel which has age between t and t+dt t
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Means and moments of distribution
Mean
residence time
t = tE (t )dt
0
E (t )dt ' = tE (t )dt
0 0
Variance
= t t E (t )dt
2 0
( )
2
Skewness
s = t t E (t )dt
3 0
( )
3/ 2
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Example
0.20 0.15
1.0 0.8
E(t)
0.10 0.05 0.00 0 2 4 6 8 10 12 14
F(t)
0.6 0.4 0.2 0.0 0 2 4 6 8 10 12 14
t
0.20 0.15 0.10 0.05 0.00
t
0.8 0.6
t E(t)
0 2 4 6 8 10 12 14
I(t)
0.4 0.2 0.0
10
12
14
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Experimental determination of RTD
Convolution
t
integral
t 0
Ce (t ) = Co (t t ') E (t ')dt = Co (t ') E (t t ')dt
0
Pulse
input
E (t ) = Ce (t )
C (t ) dt
e 0
Step
input
F (t ) = Ce (t ) C0
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Determination of RTD from model
CSTR
1 E (t ) = exp ( t )
PFR
E (t ) = (t ), F (t ) = H (t )
PFR-CSTR
or CSTR-PFR
0
t <p
E (t ) = 1 t p exp t p s s
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RTD and reactions
kinetics
of the reaction the RTD of fluid in the reactor the earliness or lateness of fluid mixing in the reactor whether the fluid is a micro or macro fluid
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Example second order reaction
1.0 0.8
CSTR-PF PF-CSTR PF CSTR PF(=4) CSTR(=4 )
C/C0
0.6 0.4 0.2 0.0 0 2 4 6
10
k C0
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Macro- and Micromixing
Macromixing
in the reactor Micromixing description of how molecules of different ages interaction with each other
q
distribution of residence times
Complete segregation all molecules of same age group remain together until they exit the reactor Complete micromixing molecules of different age group are completely mixed
the
earliness or lateness of fluid mixing in the reactor whether the fluid is a micro or macro fluid
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Zero parameter models
Complete
segregation
Cs = C (t ) E (t )dt
0
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Model
dC = R(C ) C (0) = C0 dt dCs = C (t ) E (t ) Cs (0) = 0 dt Cs = C (t ) E (t )dt
0
z t= t ( 0, ) z ( 0,1) z 1 dC R (C ) = dz (1 z )2 dCs E ( z 1 z ) = C 2 dz (1 z )
dC dC dz 2 dc = = (1 z ) dt dz dt dz
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Zero parameter models
Maxiumum
mixedness
dC E ( ) = R(C ) (C10 C ) d 1 F ( )
C ( = 0) = C10
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Example second order reaction
1.0 0.8
maximum mixedness complete segregation 2 CSTRs
0.4
maximum mixedness complete segregation 2 CSTRs
C/C0
0.6 0.4 0.2 0.0 0.01 0.1 1 10 100 1000
0.0 1 10 100 1000 0.2
k C0
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Example mass transfer and reaction
0.6 0.5
1.0
Concentration
0.8 0.6 0.4 0.2 0.0 0 2 4 6
CA (r=1m) CB CA (r=100m) CB
0.4
CAe
0.3 0.2 0.1 0.0 1 10 100
maximum mixedness segregated flow
1000
10000
r( m)
10
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One parameter models
Tanks
in - series
N N t n1 nt E (t ) = exp ( N 1)! N
2 =
1 N
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One parameter models
Axial
dispersion model
1 1 = 1 (1 e Pe ) Pe Pe
2
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RTD
1.4 1.2 1.0
1
7
10
6
1 2 3 4
5 4
500
dispersion model
4 2
E(t)
E(t)
0.8 0.6 0.4 0.2 0.0 0
3 2 1
0 5 40
0 0.0
0.5
1.0
1.5
2.0
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Transient in PFR
1.0 0.8 0.6
: :
t 0 0.25 0.5 0.75
2.5
0.4 0.2 0.0 0.0
0.2
0.4
0.6
0.8
1.0
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Compartment models
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Example
1.0 0.8
1.0 0.8
ConversionA
0.4 0.2 0.0 0.0 0.2 0.4 0.6
1 CSTR 2 CSTR
YieldB
0.6
0.6 0.4 0.2
1 CSTR 2 CSTR
0.8
1.0
0.0 0.0
0.2
0.4
0.6
0.8
1.0
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Rate contours reversible reaction
1
0
0.9 0.8 0.7
0.1
0
0.6
'
0.5 0.4
0.1
0.3 0.2 0.1
0 .1
1
0
0.1 11 0 0 100
10
0 300
310
320
330
340
350
360
370
380
100 10 0 0.1 1 390 400
Temperature
Indian Institute of Science
Fludized bed catalytic convertors
Indian Institute of Science
Fluidised bed reactor
Indian Institute of Science
Solid volume fraction
Indian Institute of Science
