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I

A.1 FENSKE METHOD.........................................................................................................I

A.2 SHORTCUT METHOD USING UNISIM........................................................................III

A.3 DIMENSIONS OF COLUMN......................................................................................III

APPENDIX B: CALCULATION OF Tcarnot.........................................................................V

APPENDIX D: SIZING OF THE METHANOL REACTOR...............................................VII

APPENDIX E: SIZING OF SEPARATORS........................................................................VIII

APPENDIX F: SIZING OF HEAT EXCHAGERS, CONDENSERS AND REBOILERS

....................................................................................................................................................X

APPENDIX G: Heat Exchanger Network Design.................................................................XII

G.1 HEAT EXCHANGERS HE-1, HE-2 AND HE-3.......................................................XII

G.2 HEAT EXCHANGERS HE-4 AND HE-5.................................................................XIII

G.3 HEAT EXCHANGERS HE-6 AND HE-7.................................................................XIII

APPENDIX A: . .SIZING OF DISTILLATION COLUMNS

A.1 FENSKE METHOD

The minimum number of stages was found using the Fenske equation (Sinnot, 2009):

min

log

log

LK HK

HK LK

d b

LK

x x

x x

N

1 1

1 1

] ]

where:

is the relative volatility of the more volatile component i to the less volatile component j,

y

i

is the vapor-liquid equilibrium concentration of component i in the vapor phase,

x

i

is the vapor-liquid equilibrium concentration of component i in the liquid phase,

y

j

is the vapor-liquid equilibrium concentration of component j in the vapor phase and

x

j

is the vapor-liquid equilibrium concentration of component j in the liquid phase

The vapor-liquid equilibrium was found from The Perry's Chemical Engineers' Handbook:

At 91,2 C:

y

i

= 0,304

x

i

= 0,06

y

j

=0,696

x

j

=0,94

I

Thus the relative volatility was calculated to be 6,84

For the distillate:

X

LK

=0,999

X

HK

=0,001

For the bottoms:

X

LK

= 0,001

X

HK

=0,999

From the Fenske equation the minimum number of stages was calculate to be 7,2. A factor of

three was assumed to get the real number of stages. Thus the number of stages became 22.

II

A.2 SHORTCUT METHOD USING UNISIM

Using the shortcut module in UniSim and the specifications given in table A.1 the number of

stages was calculated for COL-2. Assuming a stage efficiency of 60% the real number of

stages was calculated. The result of the calculation is given in table A.2. The number of stages

in COL-1 was calculated by using the distillation column module in UniSim. The flow molar

flow rate from the reboiler was specified to be 0,997 of the total amount of methanol + water

in the feed. The temperature in the condenser was set to 18 C. The number of stages and feed

stage was found using trial and error until the CO

2

mole fraction was near zero in the bottom

stream and until the recycle ratio was reasonable.

Table A.1 - Specifications used in the short cut column

COL-2

Water in

distillate [mole

fraction]

0,001

Methanol in

Bottoms[mole

fraction]

0,001

Condenser

pressure[kPa]

100

Reboiler

pressure [kPa]

200

External reflux

ratio

0,68*

*Set to 1,2 times the minimum reflux ratio (IA1)

Table A.2 Result of calculation

COL-1 COL-2

Number of stages reboiler 27 6

Number of stages with 60 %

Efficiency

45 10

Feed stage (from the top) 11 Reboiler

A.3 DIMENSIONS OF COLUMN

The columns was sized using a procedure described by Sinnot.

Procedure from Sinnot:

The plate spacing was set to 0,5 m.

The column diameter was calculated according to the following equations:

0,5

^

2

( 0,17 0, 27 0, 047)

L v

v

t t

v

u l l

1

+

1

]

III

Where

^

v u

is the maximum allowable vapor velocity, based on the gross (total) column cross

sectional area, m/s, and l

t

is the plate spacing in meters.

w

c

v v

V

D

u

Where D

c

is the column diameter in meters,

w

V is the maximum vapor rate in kg/s.

IV

APPENDIX B: CALCULATION OF T

carnot

The temperature where the reaction changes

from being non-spontaneous to spontaneous is

called T

Carnot

. T

Carnot

was calculated using the relation:

RX RX RX

G H T S +

At equilibrium the equation above is equal to zero, and the T

carnot

could be calculated:

RX

carnot

RX

H

T

S

Thermodynamic data for different pressures and temperatures was obtained from UniSIM and

SI-chemical data. The data are listed in table B.1.

The thermodynamic data in from table B.1 was used to calculate H

RX

and S

RX

for reaction

B.1. The results are shown in table B.2.

4 2 2

( ) ( ) ( ) 3 CH g H O g CO g H + +

(B.1)

Table B.1. Thermodynamic data collected at different temperatures and pressures.

298 K and 1 bar 200 C and 40 bar 800C and 40 bar

Components

H

[kJ/kgmol)

S

[kJ/kgmolC]

H

[kJ/kgmol)

S

[kJ/kgmolC]

H

[kJ/kgmol)

S

[kJ/kgmolC]

CH4(g) -74920,00 183,60 -68193,94 170,74 -31150,49 219,65

CO(g) -110600,00 159,20 -105531,10 141,82 -86367,16 167,79

H2(g) -0,11 123,10 5038,69 105,62 22920,71 129,93

H2O(g) -245550,00 189,00 -272048,48 90,71 -213118,89 189,76

Table B.2. T

carnot

for different temperatures and pressures

298 K and 1 bar 200 C and 40 bar 800C and 40 bar

H

RX

[kJ/kgmol] 209870 249827 226664

S

RX

[kJ/kgmolC] 156 197 148

T

carnot

[C] 1073 994 1257

It would seem that the temperature have to above 1257 Celsius to make the reaction

spontaneous. The T

carnot

seemed to vary quite a lot, which is a bit distubing, since one could

expect that the T

carnot

should be

relative constant because there are no phase transitions present.

UniSIM are probably not be best tool to use, when collection thermodynamic data, but was

used because of the simplicity. In the literature (S. Lee, 1997) thermodynamic calculations

were done for the same reaction. The result was a T

carnot

temperature of 950K. The temperature

in the steam was chosen to be 1000 C to be sure that the reaction actually is above T

carnot,

and

to ensure that reaction would give good conversion. The latter is especially important for the

process described in this report, because of the lack of a secondary reformer.

V

APPENDIC C: AMOUNT OF NATURAL GAS FEED

This appendix shows the calculation of the amount of natural gas feed needed for the process

to produce 2500 tonne pr day methanol assuming 100% conversion,

By combining the equations C.1 and C.2, equation can be formed:

4 2 2

( ) ( ) ( ) 3 ( ) CH g H O g CO g H g + +

(C.1)

2 3

( ) 2 ( ) ( ) CO g H g CH OH g +

(C.2)

4 2 3 2

( ) ( ) ( ) ( ) CH g H O g CH OH g H g + +

(C.3)

From this equation it is easy to see that 1 mole of methanol is equivalent to 1 mole of

methane. Using a molar mass of 32,0418 kg/kgmole methanol, the amount of methane

required to make 2500 tonne/day methanol was found to be 3251kgmole/h. This value was

used as an approximation of the amount of natural gas needed in the methanol production.

VI

APPENDIX D: SIZING OF THE METHANOL

REACTOR

The reaction of syngas to methanol is highly exothermic. Heat released from the reaction

needs to be removed to keep the reactor isothermal. To be able to cool the reactor sufficient,

the catalytic mass has to be divided into small enough pieces that heat efficiently can be

removed. Tjeldbergodden has similar reactor and reaction, which is carried out at a similar

temperature. The tube dimensions used at Tjeldbergodden were used as an estimate for the

catalytic tubes size estimation. The reactor length was also assumed to be the same as used at

Tjeldbergodden.

In the industry, a 4:1 recycle ratio is commonly used (Aasberg-Petersen, 2001). The number

of tubes needed in the reactor are based this recycle ratio, a single tube diameter of 4 cm (O7)

and a maximum flow velocity of 5m/s (O4).

A flow rate of 13199 kgmole/h incoming feed from the reformer section would result in a

allowed recycle of 65995 kgmole/h. Which is equivalent to a volume flow rate of 16,88 m

3

/s

when using a molar density of 1,09 kgmol/m

3

. A maximum allowable flow rate in the reactor

lead to a cross section area of 6,75 m

2

,when assuming a catalyst void fraction of 0,5. This

will lead to a total number of 5373 tubes inside the reactor shell.

The outer diameter of the shell was calculated by assuming a triangular pitch of 1,25 times the

outer tube diameter (Smith, 2005) and a wall thickness of 0,5 cm. A single tube in a triangular

pitch arrangement was reported by the literature (Smith, 2005) to be contained in an area of

0,866 times the pitch squared. From this, the area and the diameter were calculated. The total

diameter was found to be 4,8 m.

VII

APPENDIX E: SIZING OF SEPARATORS

The size of the separators was calculated using the procedure described by Sinnot et. al

(Sinnot, 2009). Sizing data from UniSIM was compared with the data from the procedure

above. It was assumed that demister pads were used for both separators.

The procedure from Sinnot et al goes as the following:

Equation E.1 can be used to calculated the settling velocity (u

t

) :

1

2

( )

0, 07

L v

t

v

u

1

]

(E.1)

where

L

v

Minimum vessel diameter:

4

v

v

s

V

D

u

(E.2)

Where V

v

is the volumetric flow rate in m

3

/s, u

s

=u

t

since demister pads were used.

Required liquid level was calculated by assuming a 10 min hold up time.

The height were calculated according to figure 10,67 page 638 in Sinnot et. al (Sinnot, 2009).

Key data are given in table E.1

VIII

Table E.1 Key data

Variable SEP-1 SEP-2

u

t

[m/s]

0,67

0,39

L

[kg/m

3

] 1004,6 821,4

v

[kg/m

3

] 10,9

25,0

V

v

[m/s] 3,10 9,33

D

v

2,43 5,49

Liquid height [m]

2,32 1,22

Liquid level to inlet (min(d/2,0.6m))

[m] 1,21 1,22

Inlet to demister pad (min(d,1m)) [m] 2,43 5,49

Demister pad to vapor outlet

(min0.4m) [m] 0,40 0,40

Total height [m] 6,36 9,85

IX

APPENDIX F: SIZING OF HEAT EXCHAGERS,

CONDENSERS AND REBOILERS

This appendix describes the sizing of the heat exchangers, condensers and reboilers. Heat

transfer coefficients for the fluids used in the model are given in table F.1.

Table F.1 Heat transfer coefficients (Skogestad, 2003)

Fluids

Heat transfer coefficients

[W/m

2

K]

High pressure process stream- water 570

High pressure process stream vaporizing

water (assumed)

500

High pressure process stream high pressure

vapor

450

High pressure process stream- High pressure

process stream

450

Low pressure process stream Water 140

Boiling liquid- condensing vapor 800

Boiling liquid- Cooling of super heated

steam (assumed)

800

The exchanger area was calculated by using the duty given from UniSIM. The log mean

temperature difference was calculated for each heat exchanger. If one or both of the fluids

experienced phase transitions, the exchanger was split into appropriate pieces such that

correct heat transfer coefficients could be used. All heat exchangers are assumed to be

counter-current heat exchangers.

Example:

Duty: Q (given from UniSIM)

LMTD (log mean temperature difference) =

1 2

1

2

T T

T

ln

T

_

,

Where

1

T

is the temperature difference between the hot inlet stream and cold outlet is is

stream and

2

T

is the difference between the hot outlet stream and the cold inlet stream.

Using the relation:

X

*

Q

A

U LMTD

The heat exchanger area could then be calculated. The results are shown in table F.2.

Table F.2 Key heat exchanger data

Duty [kW] Surface area [m

2

] Type

Heat exchanger (HE-1)

28673 -

Included in heat recovery unit on

the steam reformer

Heat exchanger (HE-2)

20360 -

Included in heat recovery unit on

the steam reformer

Heat exchanger (HE-3)

121776 -

Included in heat recovery unit on

the steam reformer

Heat exchanger (HE-4) 61583 1321 U-tube

Heat exchanger (HE-5) 137072 13087 Flat plate

Heat exchanger (HE-6) 74205 2934 U-tube

Heat exchanger (E-105) 133129 894 Falling film evaporator

Reboiler (REB-1) 9434 99 Kettle

Reboiler (REB-2) 59945 473 Kettle

Condenser (CON-1) 262 163 Shell and tube

Condenser (CON-2) 60620 7508 Shell and tube

XI

APPENDIX G: Heat Exchanger Network Design

The synthesis gas (H1) from the steam reformer is to be cooled from 1000C to 30C.

The product out from the methanol reactor (H2) is to be cooled from 260C to 30C.

Flue gas from the steam reformer (H3) should be cooled from 1000C to below 150C

The natural gas feed (C1) is to be heated from -0,26C to 455C.

The methane rich gas from the prereformer (C2) is to be heated from 448,25C to

650C

The methanol reactor feed (C3) is to be heated from 46,03C to 260C.

Table G.1 summarizes the flow rate, heat capacity and temperature intervals for the six

streams.

Table G.1 Properties for the hot and cold streams

Stream Flow rate, m Cp (average) T Q = mCpT

# (kg/s) (kJ/kgC) C MW

C1 Natural Gas 15,21 3,047 455,26 21,10

C2 Methane from PR 51,74 2,744 201,75 28,64

C3 Reactor feed 286,49 2,648 213,97 162,32

H1 Exhaust gas 157,24 1,255 850 177,53

H2 Syngas 51,74 3,440 970,00 172,66

H3 Methanol 273,70 2,677 230,00 168,53

G.1 HEAT EXCHANGERS HE-1, HE-2 AND HE-3

To ease the start-up of the plant, the flue gas (H3) is only heat integrated with the process

streams before the steam reformer (C1 and C2). It should also be ckecked if there is enough

heat in the flue gas to generate the amount of MP Steam needed in process. The dew point for

water at 30 bar (pressure for MP steam) is 234,6C. The heat of vaporization is 1822,70 kJ/kg.

Generating MP steam with a flowrate of 36,351 kg/s and target temperature of 455C requires

a duty of

1 1 2 2

( )

36,351 kg/s x (4,789 kJ/kg C x 224,37 C + 1822,70 kJ/kg + 2,249 kJ/kg C x 220,4 C)

123,94 MW

MP p vap p

Q m c T H c T + +

&

The total required duty is then

Q = Q

C1

+ Q

C2

+ Q

MP

= 21,10 MW + 28,64 MW + 123,94 MW = 173,68 MW.

Assuming an outlet temperature of 150C for the flue gas, the c

p

is found to be 1,153 kJ/kgC.

At 1000C the c

p

is 1,370 kJ/kgC, and the average c

p

is then 1,262 kJ/kgC. The outlet

temperature of the flue gas becomes

173680kW

1000C 125, 8C

157, 24kg/s 1, 262kJ/kgC

s

p

Q

T T

mc

&

XII

At 125,8C the c

p

is 1,147 kJ/kgC, and the average c

p

is then 1,259 kJ/kgC. The exit

temperature then becomes 122,7C which is an acceptable exit temperature. Further in the

calculations, if nothing else is stated, c

p

is assumed to not change cignificantly for smaller

temperature intervals.

The outlet temperature of H3 out of HE-1 becomes

21100kW

1000C 893, 67C

157, 24kg/s 1, 262kJ/kgC

s

p

Q

T T

mc

&

The outlet temperature of H3 out of HE-2 becomes

28640 W

893, 67C 749, 34C

157, 24kg/s 1, 262kJ/kgC

s

p

Q k

T T

mc

&

G.2 HEAT EXCHANGERS HE-4 AND HE-5

The synthesis gas from the steam reformer could possibly be used to generate HP steam. The

dew point for water at 40 bar (HP steam) is 251,3C. The heat of vaporization is

1741,17 kJ/kg. Generating HP steam with a flowrate of 38,671 kg/s and target temperature of

510C requires a duty of

1 1 2 2

( )

38,671 kg/s x (5,517 kJ/kg C x (251,3-10) C + 1741,17 kJ/kg + 2,397 kJ/kg C x (510-251,3) C)

142,79 MW

HP p vap p

Q m c T H c T + +

&

The excess heat for the syngas is (172,66-142,79) MW = 29,87 MW. The outlet temperature

of the syngas becomes

142790kW

1000C 197, 4C

51, 74kg/s 3, 440kJ/kgC

s

p

Q

T T

mc

&

To reach the target temperature of 30C cooling water (duty = 29,87 MW) could be used

(HE-5). Because there will be a phase transition, the heat exchanger will have a larger duty.

G.3 HEAT EXCHANGERS HE-6 AND HE-7

The feed to the methanol reactor (C3) could be heat integrated with the methanol stream out

of the methanol reactor (H3). The methanol stream has a dew point of 110,8C. To ease the

calculations, no phase transition is assumed during the heat exchange with the methanol

reactor feed. Assuming a T

min

equal to 20C, i.e. the outlet temperature of C3 to be 240C,

the duty for HE-6 becomes

286, 49 kg/s 2,648 kJ/kg C (240 - 46,03) C 147,15 MW Q

XIII

The duty of the cooler (HE-7) becomes (168,53-147,15) MW = 21,38 MW and the outlet

temperature H3 becomes

147150kW

260C 59,16C

273, 70kg/s 2, 677kJ/kgC

s

p

Q

T T

mc

&

Because there will be a phase transition, the heat exchanger (HE-7) will have a larger duty.

The duty of the heater becomes (assuming c

p

will not change significantly because of the

small temperature difference)

286, 49 kg/s 2,648 kJ/kg C (260 - 240) C 15,17 MW Q

In reality, since phase transition will occure, the outlet temperature of C3 will be lower and

the duty of the heater will be higher, and the outlet temperature of H3 will be higher and

therefore will also the duty of the cooler be higher.

In figure G.2 below the proposed heat exchanger network is shown. Heat exchanger I

represents, HE-1, II represents HE-2 and so on. HE-5 and HE-7 is replaced by the symbol C

for cooling.

Figure G.2 Heat Exchanger Network Design

XIV

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