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KELOMPOK 2

UNIVERSITAS INDONESIA

DEPOK 2019

Example 10.2

Suppose that a fixed bed reactor is to be designed for oxidation of SO2 using platinum/Al2O3

catalyst. The intrinsic rate equation (g mole / (h)(g catalyst) from experimental rate data is:

1

PSO P1/O 2−(

)P

2

K SO

2 3

r= 2

[0.176+12.9 PSO ] 3

Intra particle transport effects are negligible, but external concentration and temperature

differences may be important. We will assume isothermal conditions at 480 °C in order to

simplify the calculations. The superficial mass velocity of gas through the bed will be 147 lb/

(h)(ft)2. To demonstrate the procedure for accounting for external mass transport limitation,

calculate the global rate at a location in the reactor where the bulk partial pressures are those

given in table below.

Solution:

Density of air:

28.9 273

(

359 480+ 273 )( 790

760 )

=0.0304 lb/ft 3

Schmidt group:

μ 0.09

= =1.21

ρD 0.0304 (2.44)

Equation 10-20:

μ 23

Cb −C s=

rp

ρD ( )

=

0.0956

2

( 1.21 )3

=1.40 x 10−5 lb mol/ ft 3

G 5.12 147

at

ρ

jD ( ) 0.31 (

0.0304 )

So,

( pb− p s )SO =R g T ( C b−C s ) =0.73 [ 1.8 ( 480+273 ) ] ( 1.40 x 10−5 ) =0.0139 atm

2

ps=0.0603−0.0139=0.0464 atm

Calculation for O2

Equation 10-20:

2

μ 3 0.0956

Cb −C s=

ρD

rp

=

( )

2 ( 0.81 )

2

3

=5.4 x 10−6 lb mol /ft 3

G 5.12 147

at

ρ

jD ( ) 0.31

0.0304 ( )

So,

2

ps=0.201−0.005=0.196 atm

Equation 10-20:

μ 23

Cb −C s=

rp

ρD ( )

G

at

ρ D

j ( )

So,

3

ps=0.0067+0.0150=0.0217 atm

(0.0217)

0.176+ 12.9¿

¿

¿2

¿

1

r=

2

1

1/ 2

PSO PO −(

K2

=

3

1/ 2

)PSO 0.0464 (0.196) −

73

0.0217( )

[0.176+12.9 PSO ]2 ¿

3

Since this result is close to the assumed value, it is the desired global rate for a location in

the reactor where the conversion is 10%.

Problem 10.3

Predict the global rate of raction for the oxidatation of SO 2 at bulk gas condition of 20%

conversion at 480 oC. Other condition are as given in Prob 10-2. The rate at the catalyst

surface is to be calculated from Eqs. (G) and (H) of Example 9-2. Assume isothermal

condition. The constants in Eqs. (G) and (H) at 480 oC are :

K = Kp = 73 (atm) -1/2

Also calculated the ratio ƴ of the global rate and the rate evaluated at bulk condition.

Solution :

From table problems 10.2 we can get the rp, g mol SO2/ (h) (g catalyst) in term of

Temperature :

rp, g mol SO2/ (h) 0,02397 0,0344 0,0514 0,0674 0,0898 0,122

(g catalyst)

To develop an expression for the rate of reaction we must postulate the method of obtaining

adsorbed atomic oxygen. If it is supposed that molecular oxygen is first adsorbed on a pair of

vacant centers and that is product then dissociates into two adsorbed atoms, the process may

be written :

O-O

O2 + 2X → | | → 2O . X

X–X

Since the surface reaction is controlling, the adsorpstion of oxygen must be at equilibrium.

Then the concentration of adsorbed atomic oxygen is given by the equilibrium equation.

2 2

r AO=ko . P o 2 . Ć v −k −o Ć O

1 2

(

r AO=ko . Po 2 . Ć 2v −

Ko O

Ć )

1 2

Where r AO=0 (

0=ko . Po 2 . Ć2v − Ć

Ko O )

1 2

Ć O =ko Po 2 . Ć 2v

Ko

So,

2

Ć O

Ko= 2

Po2 Ć v

(1)

the consentration of vacant centers. Solving this expression for Ć o yields :

1/ 2 1 /2

Ć o = K o P o 2 Ć v

The surface-raction step is represented by :

SO2 . X + O . X → SO3 . X + X

r s =k s . C s

1

(

r s =k s Ć so2 Ć0 − Ć Ć

K s so 3 v )

(2)

The concentrations of SO3 and SO2 adsorbed on the catalyst are given by the conventional

equilibrium expressions

SO3 + X → SO3 . X

r AD 2=k SO 3 . P So3 . ĆV −K−So 3 ĆSO 3

1

(

r AD 2=k SO 3 Ć SO 3 ĆV −

K SO 3

Ć so3 )

Where r AD 2=0

1

0=k SO 3 . P So 3 . ĆV − Ć

K SO 3 SO 3

1

Ć SO 3=k SO 3 . PSo 3 . Ć V

K SO 3

Ć SO 3=K SO 3 . P So 3 . Ć V (3)

SO2 + X → SO2 . X

r AD 3=k SO 2 . P So2 . ĆV −K−So 2 Ć SO 2

1

(

r AD 3=k SO 2 Ć SO 2 Ć V −

K SO 2

Ć SO 2 )

Where r AD 3=0

1

0=k SO 2 . P So 2 . ĆV − Ć

K SO 2 SO 2

1

Ć SO 2=k SO 2 . PSo 2 . Ć V

K SO 2

Ć SO 2=K SO 2 . P So 2 . ĆV (4)

1

(

r s =k s K SO 2 . P So2 . ĆV . Ko 1/ 2 . P1/o 22 . Ć V − K SO 3 . PSo 3 . Ć V . ĆV

Ks )

K SO 3

(

r s =k s Ko1/ 2 . K SO 2 . P So2 . P 1/o 22−

Ks )

. PSo 3 ĆV 2 (5)

Ćm =ĆV + Ć SO 2 + Ć SO 3 + ĆO + Ć N 2

1/ 2 1 /2

Ćm =ĆV +¿ K SO 2 . P So 2 . ĆV + K SO 3 . P So3 . Ć V + K o . Po 2 . Ć v +

K N 2 . PN 2 . Ć V

The last term is include to take into account the possibility that N 2 may be adsorbed on the

catalyst. Eliminating ĆV from Eq. (2) by introducing Eq (6) :

Ć m

ĆV = 1/ 2 1 /2

1+ K SO 2 . P So2 + K SO3 . PSo 3 + K o Po 2 + K N 2 . P N 2

(6)

2

K Ć m

(

r s =k s Ko . K SO 2 . P So2 . P − SO 3 . PSo 3

1/ 2 1/ 2

o2

Ks )( 1 /2 1/ 2

1+ K SO2 . PSo 2+ K SO 3 . P So3 + K o Po 2 + K N 2 . PN 2 )

1/ 2

K SO 3

Noting that Ko . K SO 2 , = K, may we write :

Ks

1 1

r=

(

k s Ćm2 Ko 2 . K SO 2 P So2 . P o22−

1

.P

K So 3 )

2

(1+ K SO 2 . PSo 2 + K SO 3 . P So 3 .+ K 1o/2 P1/o 22+ K N 2 . PN 2)

(7)

Because the partial pressures of sulfur of sulfur dioxide and sulfur trioxide are both small, the

value of PN 2 will not vary significantly with conversion. Hence K N 2 . PN 2 may be

regarded as a constant in Eq (7). Since conversion was only variable causing the composition

to change PO 2 PSo 2 , and PSo 3 are not independent, but are related to the initial,

constant composition and the conversion. Hence Po 2 in the denominator of Eq. (7) can be

expressed in terms of conversion or, more conveniently, in terms of PSo 3 . Eq (7) may be

simplified to :

[ ]

1 1

r=

k s Ć m2 Ko 2 . K SO 2 P So 2 . Po22− ( K1 ) P So 3

2

( A' +B ' PSo 3 )

(8)

R= A+ Bp so3 (G)

1/ 2

[ ]

1

1

R=

P So2 . P − P 2

o2

K So 3 ( )

r

(H)

Since conversion was the sole variable, individual adsorption equilibrium constants

K o , K SO 2 , K SO 3 , K N 2 cannot be determined. Table 9-1 for Partial pressure from r, g mol

SO2/ (h) (g catalyst).

gmoll/(h)(g

catalyst) SO3 SO2 O2

0,02 0,0428 0,0255 0,186

0,04 0,0331 0,0352 0,19

0,06 0,0272 0,0409 0,193

0,08 0,0236 0,0443 0,195

0,10 0,0214 0,0464 0,196

0,12 0,0201 0,0476 0,197

We must interpolate data to partial pressure in r = 0,0898 , interpolated from excel we get :

gmoll/(h)(g catalyst) SO3 SO2 O2

0,0898 0,0225 0,0453 0,1955

Where :

K = Kp = 73 (atm) -1/2

With these values the rate equation from Eq (G) and (H) is :

[ ]

1 1

r=

2 2

k s Ć m Ko . K SO 2 P So 2 . P − 2

o2 ( K1 ) P So 3

2

( A' +B ' PSo 3 )

1

r=

2

PSo 2 . P −

o2 ( K1 ) P So 3

2

( A ' + B' P So 3 )

r=

0,0453(0,1955)1 /2− ( 731 ) 0,0225

2

[−0,127+15,3(0,0225)]

0,019721

r=

0,047197

Air density 273 K P

x x

Molal volume∈STP T ( C ) +273 K Patm

x x = 0,0304 lb/ft3

359 ft 3 /lbmol 480 C+273 K 760 atm

µ 0,09

=

ρ D (0,0304)(2,44)

= 1,21

rp, gmol

0,004 0,0078 0,0144 0,0239

SO2/(h)(g 0,0344 0,0514 0,0674 0,0898 0,122

9 8 3 7

catalyst)

At 480◦C, the viscosity of air is about 0,09 lb/(h)(ft) and superficial mass velocity is 350 lb/(h)

(ft2) The particle diameter to employ is the diameter of the sphere with the same area as that of

the cylindrical pellets. Hence πdp2 will equal the sum of the areas of the lateral and end

surfaces of the cylinder :

dp = 0,0128 ft

0,09 lb /(h)(ft)

dp G ¿

µ = (0,0128 ft )(350

lb

) = 49,7

( h ) ( ft 2 )

¿

Then we can substitute the void fraction of the bed which is 0,43 and Reynold number to

Equation 10-10,

−0,407

(0,458) d p G

JD = ( )

εB µ

−0,407

(0,458)

JD = (49,7)

(0,43)

JD = 0,2173

µ 2/ 3

Cb - C s =

rp

ρD( )

G

at

ρ D( )

J

0,0898 lbmol 2 /3

( ) (1,21 )

( h ) ( lb )

( )

lb

Cb - C s =

(5,12

ft 2

)

( 350

( h )( ft 2 ) )

(0,2173)

= 7,9605 x 10-6 lbmol/ft3

lb lb

0,0304

ft 3

Because that we evaluated the rate of reaction in bulk, so we can assume that C s~0, so Cb is

7,9605 x 10-6. At first, the rate equation of transport reactant to the catalyst surface is in

Equation 10-1,

rp = kmam(Cb - Cs)

But, because we assume that reactant haven’t reacted at the catalyst surface and the reaction-

rate constant k is very much greater than kmam, so Cs~0, in Equation 10-3 which is,

rp = kmamCb

To find the value of rp we have to solve the kmam value by Equation 10-9,

km ρ am 2/ 3

JD = ( )( )( )

G at

µ

ρD

J DG at

2/3

kmam = µ

ρ( )

ρD

lb ft 2

kmam =

(

(0,2173) 350

( h )( ft 2 ) )

(5,12

lb

)

lb 2 /3

(0,0304 ) ( 1,21 )

ft 3

We can substitute the value of kmam and Cb to Equation 10-3, to solve the value of rate-reaction

in bulk condition.

rp = kmamCb

But, the value of the bulk reaction is less than the surface reaction and it’s impossible.

Because the value of bulk rate reaction should be greater than value of surface rate reaction.

Because the limiting reaction is surface rate reaction which is the slowest reaction. And the

bulk rate reaction should be faster than surface reaction. So we can try another way with

interpolation.

Table 10-2

conversion of (h)(g catalyst) SO2 SO3 O2

SO2

0.1 0.0956 0.0603 0.0067 0.201

0.6 0.0189 0.0273 0.0409 0.187

gmol/(h)(g catalyst) SO3 SO2 O2

0.0898 0.0135 0.0537 0.1982

r b=

PbSo 2 . Pbo22 − ( K1 ) Pb So 3

2

( A ' + B' Pb So 3)

r b=

0,0537 (0,1982)1 /2− ( 731 ) 0,0135

2

[ −0,127+15,3( 0,0135) ]

The value of bulk rate reaction in this calculating is 3,7486 gmol/(h)(gr catalyst) which is

greater than the value of surface rate reaction which is 0,4179 g mol /(h) (gr catalyst).

Ratio γ

Ratio γ =

Bulk Rate Reaction

gmol

(0,4179 )

h gr catalyst

Ratio γ =

gmol

(3,7451 )

h gr catalyst

1

Ratio γ = 0,126 ~

9

We assumed that the γ ratio in this problem is the comparation of the surface rate reaction with

the bulk rate reaction. And we solve that the value of γ is 0,126 and the value of bulk rate

reaction is 9 times faster than the value of surface rate reaction. That makes sense, because the

theory that the bulk rate reaction will be much faster than the surface rate reaction.

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