Modern Methods in Heterogeneous Catalysis Research

TRANSPORT PHENOMENA
10/31/08 Giulio Lolli
 Outline
2

Part I - Theory
Why Transport?
Fundamental equations

Unified approach to transport phenomena

Boundary Layer approach

Dimensionless numbers

Part II - Practice
Example: Methanol Synthesis

Transport Phenomena 10/31/08

 Further Reading
3

Part I
Bird, Steward, Lightfoot
Transport Phenomena
Asano Welty
Mass Transport Fundamentals of M,H&M Transfer
Part II
Handout
Web: Document DB # 15375
Perrys Chemical Engineering Handbook

Transport Phenomena 10/31/08

4 Part I
Theory

Transport Phenomena 10/31/08

 Why Transport? Catalytic Process
5

Thermodynamic
Reaction Equilibrium
Phase equilibrium:
adsorption/desorption
Kinetic
Reaction Kinetic
Transport
Reactants/Product to/
from the active sites
Heat to/from the
Transport Phenomena 10/31/08
active site
 Transport Phenomena
6

Type of transport What is transferred

Specific direction x
Momentum Transport Kinetic Energy
!uy T CA
!xy = qx = k jA,x =Law
Newtons DA
nx x x x

st
Heat Transport Thermal Energy

1 Law (Fluxes)
T CA
qx = k jA,x = DA Fouriers Law
x x
!
T! Mass
!Transport
= ! u ! Chemical
!q = k T j!A =Energy
! A
DA C
) CA
jA,x = DA Ficks Law
! =
! Ax

!
!q = k T j!A = DA C! A
2nd Law (variation in space-time)
Transport Phenomena 10/31/08
 !xy = qx
x
First Law of
Specific direction x
transport
7
st
Specific direction x
!xy =
!uy 1 q =Law
k
x
T (Fluxes)
j = D A,x A
CA
x
!uy x
T xA
C
!xy = qx = k jA,x = DA
x x x
1st Law (Fluxes)
!! !u
st
1 Law (Fluxes)
!
T! = !
!u

T!q ==kT
!
! j! ! A
= DA C
!q =
A
!
T! = !
!u !
!q = k T ! A
j!A = DA C
! =
! A
! =
! A ! =
! A
2nd Law (variation in space-time)
2nd Law (variation in space-time)
D!u !
= 2!u+!g p
nd Transport Phenomena

Dt
D!
u 2 !
= !u+!g p 2 Law (variation in sp
10/31/08
Dt
 Math 101- Gradient
8
Math 101 Nabla, Gradient

S
x x
! ! S
= y S = y

S
z z

Math 102 Divergence, Laplacian

S
x x Vx Vy Vz
! ! S ! !
= y S = y V = + +
x y z
S
z z
Transport Phenomena 10/31/08
2 2 2
2 S S S
 = !u+!g p
! =
! A Dt
Second
nd
Law of Transport
2 Law (variation in space-time)
9
DT 2
= !u+!g C = k T +u
D!u Navier-Stokes
2 !
p p
Dt Dt
DT nd
2 Fouriers
Cp
Dt
2
DCA
= k T + rH u rxn
2
DC A = D A C A +A r
Dt
= D C + r
A
2
Dt
A A 2 Fick nd

D
Dt
2
= D 2
=
Fundamental equations of the system
Dt
D!u !
= 2!u+!g p
Dt
Fundamental equations
Transport Phenomena 10/31/08
 ! ! S
= y S = y

Math 102 Divergence & Laplace

z
S
z

10 Math 102 Divergence, Laplacian

S
x x Vx Vy Vz
! ! S ! !
= y S = y V = + +
x y z
S
z z

2 2 2
2 ! ! S S S
S = S = 2
+ 2 + 2
x y z
Math 103 Substantial Derivative

S
x x Vx Vy Vz
! ! S ! !
= y S = y V = + +
Transportx y 10/31/08
Phenomena z
S
 z z

2 2 2
S S S
Math 103 Substantial Derivative
2 ! !
S = S =
x 2
+ 2 + 2
y z
11
Math 103 Substantial Derivative

S
x x Vx Vy Vz
! ! S ! !
= y S = y V = + +
x y z
S
z z

2 2 2
2 ! ! S S S
S = S = 2
+ 2 + 2
x y z

DS S ! S S S S
= + !u S = + ux + uy + uz
Dt t t x y z

Transport Phenomena 10/31/08

 = 2
Dt
Equations of Motion
12
Fundamental equations of the system

D!u 2 !
= !u+!g p
Dt
DT 2
Cp = k T +u rHrxn
Dt
DCA 2
= DA CA +A r
Dt
! (!u) = 0

Transport Phenomena 10/31/08
 Example
13

Start-up in circular tube r

Cylindrical coordinates
z
Only vz(r) 0

Example: startup in circular tube only uz (r) != 0

! "
uz u
!!z 1 uz
+ uz! = p + r
t ! z r r r

In S.S. conditions (/t = Transport

0) Phenomena 10/31/08
 Example
Example: startup in circular tube only u (r) != 0 z
14
! "
uz u
!!z 1 uz
+ uz! = p + r
t ! z r r r r

In S.S. conditions (/t = 0) z

! "
uz p
r = r
r r

uz p r"2 A" uz
r" = + " B.C. = f inite r=0
r 2 "r r
p r2
uz = +B B.C. uz = 0 r=R
4
p # 2 2
$ Transport Phenomena 10/31/08
uz = R r
4

r

1.0

0
0.0001
0.001
0.01
0.05
0.1

vz/vmax(r=0)
0.2
0.5 0.5
infinite

0.0
-1.0 -0.8 -0.6 -0.4 -0.2 0.0 0.2 0.4 0.6 0.8 1.0
r/R

15 Transport Phenomena 10/31/08

 Numerical Solution
16

Finite elements approach

Software packages

Fluent

CFD

Physics

Set up the correct problem and boundary conditions

Many times is not necessary to know the exact T,C,v

of every single point in your system

Transport Phenomena 10/31/08

 Boundary Layer
17

All the phenomena happen in the boundary layer

Everything
outside the boundary layer is in equilibrium
and constant
The boundary layer is very thin
The size of the boundary layer () is smaller than the
characteristic size of the system
Order of magnitude approach
Taylor series
Transport Phenomena 10/31/08
 Reynolds Number
18

Boundary layer approach

Reinolds Number

D"u
= 2"u
Dt
!! !! ux
u
u

2
u
Re =

x
! "2


ux
= 1/Re Re =
x ux
Prandtl Number
Transport Phenomena 10/31/08
 ux
= 1/Re Re =
x ux
Prandtls Number
Prandtl Number
19

uT = uT /

DT
Cp = k2 T
1/2 Dt
T
!
T! !
T !
Cp uT k 2
x T
T k
Cp u
x
2
T Cp
! "3
T k
Pr =


Cp
k
T Cp
P r1/3 Pr =
Transport Phenomena 10/31/08
k
 Dt
!
T! !
!
T
Schmidts Number
Cp uT
x
k 2
T
Cp
20 T
Cp u 2
k
Pr =
! "3
x T
k
T k
Re1/2
Cp
C
T Cp
P r1/3 Pr =
k
As usual everything is
Schmidt Number
the same DA
C Sc = D

A
Sc1/3 Sc =

Transport Phenomena 10/31/08

 Nusselts Number
21

Considering the
Considering the fluxes:
fluxes:

T T
k T
qq =
= k
x
= hT
= hT
x
!!
T!
! ! k!
! T
hh!
T
T k
TT
hx
hx xx KA x x
NNuu =
=
Sh =
kk TT
!"#$ !"#$
!"#$ !"#$ DA C
!"#$
1/2
!"#$
Re1/2
Re 1/3
Prr1/3 Re1/2 Sc1/3
P
In general
In general Transport Phenomena 10/31/08
 Sherwoods Number
22

Considering the
Considering the fluxes:
fluxes:

T C
k T
qq =
= k
x
= hT
= hT
x
!!
T!
! ! k!
! T
hh!
T
T k
TT
hx
hx xx KA x x
NNuu =
=
Sh =
kk TT
!"#$ !"#$
!"#$ !"#$ DA C
!"#$
1/2
!"#$
Re1/2
Re 1/3
Prr1/3 Re1/2 Sc1/3
P
In general
In general Transport Phenomena 10/31/08
 hx x
Nu =
k T
In General
!"#$ !"#$
Re1/2 P r1/3
23 In general

hx 1/3 KA x
Nu = = f (Re) P r Sh = = f (Re) Sc1/3
k DA


Re 1/2
Plate in laminar flow






2 + Re1/2 Sphere in laminar flow
f (Re) =

0.8

0.005Re Packed bed in turbulent flow

Extension to macroscopic balances

) *
Transport Phenomena 10/31/08 *
Q = q dA = A U T 1/U = 1/h + s /k
 Extension to Macroscopic Balances
24

Transport Phenomena 10/31/08

 hx 1/3 KA x
Nu = = f (Re) P r Sh = = f (Re) Sc1/3
Overall Transfer Coefficient
k DA
25


Re 1/2
Plate in laminar flow






2 + Re1/2 Sphere in laminar flow
f (Re) =

0.8

0.005Re Packed bed in turbulent flow

Extension to macroscopic balances

) * *
Q = q dA = A U T 1/U = 1/hi + si /ki
A

1/U = 1/hint + s/kmetal + 1/hext

Transport Phenomena 10/31/08
 Nu = = f (Re) P r
k
hx KA x
Nu = = f (Re) P r1/3 Sh = = f (Re) Sc1/3
Log-Mean Temperature Difference
k D



A
Re 1/2
Plate


26



Re 1/2 2 + Re1/2
Plate in laminar flow Sphere

f (Re) =



2 + Re1/2
0.8

Sphere in laminar flow
0.005Re Packed
f (Re) =




0.005Re 0.8 flow
Packed bed in turbulent





Extension to macroscopic balanc
)
Extension to macroscopic balances
Q = q dA = A U T
) A
* *
Q = q dA = A U T 1/U = 1/hi + si /ki
A 1/U = 1/hint + s/kmetal + 1/hext
T1 T2
1/U = 1/hint + s/kmetal + 1/hext Tln =
ln (T1 /T2 )
Transport Phenomena 10/31/08
 Conclusions
27

Momentum, Heat and Mass Transfer

Highly inter-correlated
Similar physical principles
Similar driving force
Similar mathematical formulas

2ndorder PDE numerical solutions

Highly dependent from fluid-dynamic properties

Simplifications
Boundary layer
Dimensionless numbers

Transport Phenomena 10/31/08

28 PART II
Methanol Synthesis

Transport Phenomena 10/31/08

 Methanol Production
29

Produced from SynGas

Catalyst Cu/ZnO-Al2O3
Equilibrium limited
P = 50 100 bar
T = 200 300 C

Main Commodity
20 Million ton/year
Typical plant size is 1 Million ton/year
12 m3/s

Transport Phenomena 10/31/08

 Catalyst specs
30
KATALCO 51-8
Methanol Synthesis Catalyst

Product Benefits Long life as a result of the optimized formulation incorporating a patented
use of a fourth component MgO
Low operating temperatures minimize the catalyst sintering rate
High catalyst selectivity gives very low impurities in the crude product
Close approach to equilibrium is achieved and maintained
Easy to reduce and start-up

Product Uses Synthesis of methanol from H2, CO and CO2 mixtures arising from steam
reforming of hydrocarbons, coal gasification or POx
General KATALCO 51-8 is a copper catalyst on a ZnO-Al2O3 support with a MgO
Description promoter
Physical Properties (Typical) Chemical Composition (Typical)
KATALCO 51-8
Form Cylindrical pellet CuO: 64 wt%
Diameter 5.4 mm Al2 O3 : 10 wt%
Length 5.2 mm ZnO: 24 wt%
Bulk Density 1250 kg/m 3 MgO: 2 wt%
Crush Strength 80 kgf
(axial)
Shipping & Avoid contact with skin and clothing. Avoid breathing dust. Do not take
Handling internally. Please refer to the relevant Material Safety Data Sheet for
further information.
KATALCO 51-8 catalyst is available in non-returnable polythene lined
mild steel drums or bulk bags for easy loading.

Transport Phenomena 10/31/08

 Reactor types
31

Transport Phenomena 10/31/08

 Multi-Bed Reactor
32
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Transport Phenomena 10/31/08
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Transport Phenomena 10/31/08
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Transport Phenomena 10/31/08
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1/U 1/hi =>:)
+ :V=:;6D@)si /ki CD77
Nusselt
A ) and Sherwood Numbers BDA=5;7 \
I) *
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)
Q = q dA = A U T ) 1/U = 1/hi + si /ki
1/U = 1/hint &A2'+"s/kmetal + 1/hext
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Transport Phenomena 10/31/08
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External Limitations
)
38
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Transport Phenomena 10/31/08
)
 Heat Exchanger
39

1st bed 580 490 K

35 MW power to take out
Boiling water to produce low pressure steam
!"#$%&'()*+',"-#) )
16 kg/s steam produced
!

Shell tube heat exchanger: 2 (5cm) tubes

6:96

hout=220 W/m2K 6:27

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)DEBFGHBG)@HGC)IAE>JKLDHGFM
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10/31/08
 Evaporation/condensation
5-22 HEAT AND MASS TRANSFER
40

For example, vapori

radiation and conve
result of heat absorb
the disengaging sur
Pr water 7
when the superheat
also occurs from falli
flashing of liquids su
Pool boiling ref
heating surface is su
is not flowing at any
motion of the bubbl
of pool boiling are p
fluid temperature is
collapse of the bubb
pool boiling, with bu
resulting in net vapo
The general shape
FIG. 5-10 Dukler plot showing average condensing-film coefficient as a func- to " tb, the tempera
tion of physical properties of the condensate film and the terminal Reynolds temperature and the
number. (Dotted line indicates Nusselt theory for Reynolds number < 2100.)
[Reproduced by permission from Chem. Eng. Prog., 55, 64 (1959).] metric relations tha
boiling curve was ori
[ J. Soc. Mech. Eng.
Transport
hl / kl !l1/2 = 0.065(N 1/2 Phenomena
1/2 10/31/08
Pr)l Fvc (5-99a) one of the great dile
2 faced with at least s
 Heat Exchanger
41

1st bed 580 490 K

35 MW power to take out
Boiling water to produce low pressure steam
16 kg/s steam produced
Shell tube heat exchanger: 2 (5cm) tubes
hout=220W/m2K
U 200 W/m2K

Low pressure steam 1-2 atm 120C

Tln= 140K
Exchange Area 1300 m3 (about 2000 tubes)
40 banks of 50 tubes (4-5 m in size)
Transport Phenomena 10/31/08
 Further Reading
42

Part I
Bird, Steward, Lightfoot
Transport Phenomena
Asano Welty
Mass Transport Fundamentals of M,H&M Transfer
Part II
Handout
Web: Document DB # 15375
Perrys Chemical Engineering Handbook

Transport Phenomena 10/31/08

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