Experimental Investigation, Analysis and Optimisation of Hybrid … · 2011. 2. 23. · Carsten...

technische

universität

dortmund

Fakultät Bio- und

Chemieingenieurwesen

Lehrstuhl für Fluidverfahrenstechnik

Carsten Buchaly | EPIC2009-Venice-Italy, 17.06.2009

Experimental Investigation, Analysis and

Optimisation

of Hybrid Separation ProcessesEFCE Excellence Award in Process Intensification 2009

Carsten Buchaly

technische

universität

dortmund

Fakultät Bio- und




Motivation

Strong interactions of both unit operations

Detailed process know-how necessary

Less experience existent

Reduced volumina of apparatuses

/ capital costs

Less energy consumption

No auxiliary components required

1

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universität

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Process Description

Propionic acid

1-Propanol

n-Propyl propionate

1-Propanol

H2O

Reactive Distillation

Integration of reaction

and separation

Increased conversion

and selectivityH2O

Membrane

separation

1-Propanol

(H2O)

Propionic acid

1-Propanol

n-Propyl propionate

1-Propanol

H2O

Membrane Separation

1-Propanol recovery

High selectivity

Independent on VLE

2

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universität

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Fakultät Bio- und



Carsten Buchaly | EPIC2009-Venice-Italy, 17.06.2009 3

Methodology

Hybrid Process

(reactive distillation + membrane separation)

Theory

Experimental design

Process analysis

Optimisation

Experiments

Pilot-scale

Start-up behaviour

Process know-how

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Methodology

Hybrid Process

(reactive distillation + membrane separation)

Theory

Experimental design

Process analysis

Optimisation

Experiments

Pilot-scale

Start-up behaviour

Process know-how

Experiments

Pilot-scale

Operational parameters

Model validation

Unit operation 1

(reactive distillation)

Unit operation 2

(membrane separation)

Theory

Experimental design

Process analysis

Experiments

Lab-scale

Separation characteristics

Model parameters

Experiments

Pilot-scale

Scale-up

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Reactive distillation: pilot-scale plant

Katapak SP 11

Distillation column (DN 50)

5.5 m packing height

Investigated operating parameters

Pressure: atmospheric

Distillate-to-feed ratio: 0.33 - 0.45

Molar feed ratio (c): 2.1 - 2.5

Reflux ratio (RR): 2.0 - 4.0

Database of 15 successfully

realised RD experiments4

12m

ProAc

POH

Sulzer BX

2.3 m

Katapak SP 11

2.7 m

Sulzer BX

0.5 m

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Vapour permeation: pilot-scale plant

Steady state vapour permeation experiments

Connection with reactive distillation column to hybrid separation process

Sulzer Pervap 2201(D) with AMemb = 0.5m²

Plate-and-frame module

Buchaly, Kreis, Górak (2007): Chemical Engineering and Processing, 46, p. 790-799

5

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Vapour permeation: pilot-scale plant

Steady state vapour permeation experiments

Connection with reactive distillation column to hybrid separation process

Sulzer Pervap 2201(D) with AMemb = 0.5m²

Buchaly, Kreis, Górak (2007): Chemical Engineering and Processing, 46, p. 790-799

5

Binary system 1-propanol/water

Water concentration: 13 - 30 wt.-%

Feed temperature: 92.0 - 98.7 °C

Feed pressure: atmospheric

Permeate pressure: 30 - 70 mbar

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Hybrid separation process: experimental investigations

RD and VP separated sequential configuration „closed recycle“

6

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Successful experiment with coupled

unit operations

Buchaly, Kreis, Górak (2008): Chemie Ingenieur Technik, 80, p. 145-156

7

-0,5

0,0

0,5

1,0

1,5

2,0

2,5

3,0

3,5

4,0

4,5

5,0

5,5

0,0 0,1 0,2 0,3 0,4 0,5 0,6 0,7 0,8 0,9 1,0

molar fraction in the liquid phase / mol mol-1

packin

g h

eig

ht

/ m

POH (exp)

ProPro (exp)

ProAc (exp)

Water (exp)

POH-Feed

reactive section

evaporator

ProAc-Feed

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7


unit operations

Increase of ester concentration in

the bottom

Change of distillate composition

-0,5

0,0

0,5

1,0

1,5

2,0

2,5

3,0

3,5

4,0

4,5

5,0

5,5

0,0 0,1 0,2 0,3 0,4 0,5 0,6 0,7 0,8 0,9 1,0


packin

g h

eig

ht

/ m

POH (exp)

ProPro (exp)

ProAc (exp)

Water (exp)

POH-Feed

reactive section

evaporator

ProAc-Feed

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Strong interactions between both

unit operations

7


unit operations

Increase of ester concentration in

the bottom

Change of distillate composition

-0,5

0,0

0,5

1,0

1,5

2,0

2,5

3,0

3,5

4,0

4,5

5,0

5,5

0,0 0,1 0,2 0,3 0,4 0,5 0,6 0,7 0,8 0,9 1,0


packin

g h

eig

ht

/ m

POH (exp)

ProPro (exp)

ProAc (exp)

Water (exp)

POH-Feed

reactive section

evaporator

ProAc-Feed

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Modelling approach

Reactive distillation based on non-equilibrium stage model

Multicomponent mass transfer (Stefan-Maxwell)

Packing specific correlations (hold-up, Dp, kga, kla)

Steady state and dynamic process simulation

Vapour permeation based on

„Solution-Diffusion-Model“

Polarisation effects (c,T)

Hydrodynamics (co-, counter-current; Dp)

Membrane materials

Implemented in Aspen Custom ModelerTM (ACM)8

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Reactive distillation: model validation

-0,5

0,0

0,5

1,0

1,5

2,0

2,5

3,0

3,5

4,0

4,5

5,0

5,5

0,0 0,1 0,2 0,3 0,4 0,5 0,6 0,7 0,8 0,9 1,0

molar fraction in liquid phase [mol/mol]

packin

g h

eig

ht

[m]

POH (exp)

ProPro (exp)

ProAc (exp)

Water (exp)

POH-Feed

reactive section

reboiler

ProAc-Feed

2,0 kg/h

2,068

2,49

0,85 kg/h

Feed:

cPOH/ProAc:

RR:

Distillate:

9

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-0,5

0,0

0,5

1,0

1,5

2,0

2,5

3,0

3,5

4,0

4,5

5,0

5,5

0,0 0,1 0,2 0,3 0,4 0,5 0,6 0,7 0,8 0,9 1,0

molar fraction in liquid phase [mol/mol]

packin

g h

eig

ht

[m]

POH (exp)

ProPro (exp)

ProAc (exp)

Water (exp)

POH-Feed

reactive section

reboiler

ProAc-Feed

2,0 kg/h

2,068

2,49

0,85 kg/h

Feed:

cPOH/ProAc:

RR:

Distillate:

Correlations for column internals:

Sulzer BX -> Bravo et al.*; Rocha et al.**

Katapak-SP -> Brunazzi***

9

* Bravo et al. (1985): Hydr. Proc., 1, p. 91–95

** Rocha et al. (1993): Ind. Eng. Chem. Res., 32, p. 641–651

*** Brunazzi, Viva (2006): Distillation & Absorption 2006

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2,0 kg/h

2,068

2,49

0,85 kg/h

Feed:

cPOH/ProAc:

RR:

Distillate:

0,0

0,2

0,4

0,6

0,8

1,0

0,0 0,2 0,4 0,6 0,8 1,0

liquid phase mole fractionsimulated / mol mol-1

liq

uid

ph

as

e m

ole

fra

cti

on

ex

pe

rim

en

tal /

mo

l m

ol-

1

-15%

+15%

-5%

+5%

9







technische

universität

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2,0 kg/h

2,068

2,49

0,85 kg/h

Feed:

cPOH/ProAc:

RR:

Distillate:

0,0

0,2

0,4

0,6

0,8

1,0

0,0 0,2 0,4 0,6 0,8 1,0

liquid phase mole fractionsimulated / mol mol-1

liq

uid

ph

as

e m

ole

fra

cti

on

ex

pe

rim

en

tal /

mo

l m

ol-

1

-15%

+15%

-5%

+5%

9







Model validation successful

technische

universität

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Fakultät Bio- und




Hybrid separation process: model validation

10

-0,5

0,0

0,5

1,0

1,5

2,0

2,5

3,0

3,5

4,0

4,5

5,0

5,5

0,0 0,1 0,2 0,3 0,4 0,5 0,6 0,7 0,8 0,9 1,0


packin

g h

eig

ht

/ m

POH (exp)

ProPro (exp)

ProAc (exp)

Water (exp)

POH-Feed

reactive section

evaporator

ProAc-Feed

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XProAc,exp

XPOH,exp

= 74.4 %

= 29.8 %

XProAc,sim

XPOH,sim

= 73.6 %

= 29.4 %

Sequential configuration


10

-0,5

0,0

0,5

1,0

1,5

2,0

2,5

3,0

3,5

4,0

4,5

5,0

5,5

0,0 0,1 0,2 0,3 0,4 0,5 0,6 0,7 0,8 0,9 1,0


packin

g h

eig

ht

/ m

POH (exp)

ProPro (exp)

ProAc (exp)

Water (exp)

POH-Feed

reactive section

evaporator

ProAc-Feed

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XProAc,exp

XPOH,exp

= 74.4 %

= 29.8 %

= 73.3 %

= 31.8 %

XProAc,sim

XPOH,sim

= 73.6 %

= 29.4 %

XProAc,exp

XPOH,exp

XProAc,sim

XPOH,sim

= 73.5 %

= 31.9 %

Closed recycle

Excellent agreement between experiments and simulation


10

Sequential configuration

-0,5

0,0

0,5

1,0

1,5

2,0

2,5

3,0

3,5

4,0

4,5

5,0

5,5

0,0 0,1 0,2 0,3 0,4 0,5 0,6 0,7 0,8 0,9 1,0


packin

g h

eig

ht

/ m

POH (exp)

ProPro (exp)

ProAc (exp)

Water (exp)

POH-Feed

reactive section

evaporator

ProAc-Feed

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RR = const

D = const

wH2O varied

Amemb = ?

QH = ?

Hybrid separation process: process analysis

11

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Strong influence on AMemb

High degree of dewatering

requires large AMemb


12

0,0

0,2

0,4

0,6

0,8

1,0

0,0% 2,5% 5,0% 7,5% 10,0% 12,5% 15,0%

mass fraction of water in the recycle

me

mb

ran

e a

rea

/ m

2

1200

1300

1400

1500

1600

1700

reb

oil

er

he

at

du

ty /

W

Amemb

Column:

D/F mass = 0.375

RR = 2.5

Membrane:

p perm = 30 mbar

D T sup = 4.0 °C

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Lower QH at higher recycle

purity required





12

0,0

0,2

0,4

0,6

0,8

1,0

0,0% 2,5% 5,0% 7,5% 10,0% 12,5% 15,0%


me

mb

ran

e a

rea

/ m

2

1200

1300

1400

1500

1600

1700

reb

oil

er

he

at

du

ty /

W

Amemb

Column:

D/F mass = 0.375

RR = 2.5

Membrane:

p perm = 30 mbar

D T sup = 4.0 °C

QH

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purity required

Optimisation problem





12

0,0

0,2

0,4

0,6

0,8

1,0

0,0% 2,5% 5,0% 7,5% 10,0% 12,5% 15,0%


me

mb

ran

e a

rea

/ m

2

1200

1300

1400

1500

1600

1700

reb

oil

er

he

at

du

ty /

W

Amemb

Column:

D/F mass = 0.375

RR = 2.5

Membrane:

p perm = 30 mbar

D T sup = 4.0 °C

QH

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purity required

Optimisation problem





Modified stochastic optimisation

algorithm based on a differential

evolution* approach (MDE)

* Babu, Angira (2008): Comp. Chem. Eng., 30, p. 989–1002

Angira, Babu (2006): Chem. Eng. Sci., 61, p. 4707–4721

Frerick et al. (2008): Chem. Ing. Tech., 1, p.1-10

12

0,0

0,2

0,4

0,6

0,8

1,0

0,0% 2,5% 5,0% 7,5% 10,0% 12,5% 15,0%


me

mb

ran

e a

rea

/ m

2

1200

1300

1400

1500

1600

1700

reb

oil

er

he

at

du

ty /

W

Amemb

Column:

D/F mass = 0.375

RR = 2.5

Membrane:

p perm = 30 mbar

D T sup = 4.0 °C

QH

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Objective function: min QH = f (RR, D/Fmass, wH2O,recycle)

Solution space: 0.8 RR 5; 0.25 D/Fmass 0.55; 0.02 wH2O,recycle 0.15

Constrain: xProPro,bottom 0.75

no LLE

Hybrid separation process: rigorous optimisation using MDE

wH2O= ?

QH= ?

RR = ?

D/Fmass = ?

Amemb= ?

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65 generations with 8 parents

CPU-time ~ 12 hour

QH,min = 1059 W

RR = 0.98; D/Fmass = 0.52; wH2O,recycle = 0.022

Amemb = 3.04 m²

feasibility and applicability of the now

available optimisation package based

on detailed process models proven

Objective function: min QH = f (RR, D/Fmass, wH2O,recycle)

Solution space: 0.8 RR 5; 0.25 D/Fmass 0.55; 0.02 wH2O,recycle 0.15

Constrain: xProPro,bottom 0.75

no LLE

wH2O= ?

QH= ?

RR = ?

D/Fmass = ?

Amemb= ?

0

20000

40000

60000

80000

100000

120000

0 5 10 15 20 25 30 35

generation

ob

jective f

un

ctio

n

parent 1

parent 2

parent 3

parent 4

parent 5

parent 6

parent 7

parent 8

13

Hybrid separation process: rigorous

optimisation using MDE

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Conclusion

14

Reliable experimental database for both unit operations

and hybrid process

Choice of an appropriate chemical test system

Development of a generic methodology for the design of hybrid processes

Provision of reliable experimental data for the applied unit operations

Experimental investigation of the fully coupled unit operations

Model validation for the stand-alone unit operations and the hybrid process

Analysis of the influence of decisive operational parameters on the

performance of the hybrid separation process

Optimisation of the hybrid process using an evolutionary algorithm

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Special thanks to:

EU-Project INSERT

“Integrating Separation and Reaction Technologies“

(Contract No. NMP2-CT-2003-505862)

Marie Curie Training Site „Reactive Separations“

(Contract Nr. HPMT-CT-2001-00408)

Fonds der Chemischen Industrie

Stefan Kluckhenn; Ildefonso Campos-Velarde; Christian Schroeder; Marcel

Kotora; Martin Cruz-Dias; Carlos Duarte; Katrin Kissing; Siggi Weiss; Piotr

Mitkowski; Paulo Perez; Gencay Cengiz; Rocio Castillo-Tornay; Dominik

Plaßmann; Markus Hengsbach; Bharat Karanth; Mayur Dalwani; Mayuratheepan

Puthirasigamany & the Laboratory of Fluid Separations

http://cordis.europa.eu/improving/networks/home.htm

technische

universität

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Fakultät Bio- und




Experimental Investigation, Analysis and

Optimisation

of Hybrid Separation ProcessesEFCE Excellence Award in Process Intensification 2009

Carsten Buchaly

Experimental Investigation, Analysis and Optimisation of Hybrid … · 2011. 2. 23. · Carsten...

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