MODELING AND CONTROL OF ACETYLENE
HYDROGENATION PROCESS

Attribution Non-Commercial (BY-NC)

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MODELING AND CONTROL OF ACETYLENE
HYDROGENATION PROCESS

Attribution Non-Commercial (BY-NC)

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Salam Al-Dawery1, Haider M. Dakhil2

Department of Chemical Engineering, University of Nizwa, Oman, E-mail: salam@unizwa.edu.on 2 Department of Chemical Engineering, University of Baghdad, Baghdad, Iraq, E-mail: Haider_dakhil@yahoo.com

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(Received November 2010 and Accepted May 2011) . . . , ,(PID ) , Mathematical model for an industrial acetylene hydrogenation plant was developed and then used for control purposes. The developed model covers all individual units of the plant such as reactor, cooler, steam heater etc. The key reaction of the plant was modeled by a second order transfer function plus dead time, while the heating and cooling units are modeled by first order transfer function. A conventional PID controllers were applied to control the plant units, an acceptable results were obtained.

1. INTRODUCTION

The cracking of petrochemical naphtha with vapor produces a stream composed mainly of ethylene and also of paraffins, diolefins, aromatics, and small amount of acetylene. The ethylene is mainly used in the production of polymers, especially polyethylene[1]. Small amounts of acetylene, on the order of parts per million, are harmful to the catalysts used in polymerization[2]. Therefore, the acetylene in the ethylene stream must be hydrogenated with a minimum loss of ethylene. Polyethylene has been key product for many industries since 1960's. The feed of the polymerization reactor, which comes from the olefin plant, is a mixture of hydrocarbons mainly consisting ethylene. An undesired impurity in the ethylene stream is acetylene at approximately 2% to 30% of the effluent of the olefin plant which may lead to undesirable polymer properties; the amount of acetylene in the feed of the ethylene polymerization reactor should not exceed 2-3 ppm[3]. It is harmful contaminant in polymer grade ethylene, so the removal of acetylene is a key step in the purification process. The most effective method for removing acetylene, down to typical levels of 2-3 ppm, is selective hydrogenation over palladium catalysts in multi-bed adiabatic reactor. The term selective is used

as the conditions which promote the hydrogenation of acetylene to ethane. Cider[4] studied the hydrogenation of acetylene, ethylene and propylene at transient conditions caused by cross-desorption of carbon monoxide due to a pulse of acetylene. Mathematical modeling of the transient reaction system showed that a simple model is able to explain the competition for the active sites and the difference in reactivity Schbib[2] studied the kinetics of acetylene hydrogenation in the presence of large amounts of ethylene in a laboratory flow reactor. Experiments were carried out using a Pd/-Al2O3 commercial catalyst and a simulated cracker gas mixture at varying temperature and pressure. Gobbo[5] discussed the modeling, simulation, and dynamic optimization of an industrial reaction system for acetylene hydrogenation. The process consists of three adiabatic fixed-bed reactors, in series, with interstage cooling. The model is able to satisfactorily predict the outlet temperature and concentrations of ethane, acetylene, methylacetylene, and propadiene in each reactor. The acetylene conversion and ethylene selectivity profiles were optimized for the reactors, taking into account catalyst deactivation and process constraints. Therefore, the removal of acetylene is a key in the purification process. The most effective method for

removing acetylene, down to 2-3 ppm, is selective hydrogenation over palladium catalyst in a multi-bed adiabatic reactor[6, 7]. The objective of this work is to develop a mathematical model that suitable for control purposes and to study the dynamic behaviors of the acetylene hydrogenation plant.

The acetylene hydrogenation plant consists of many units such as converter, cooler, steam heater etc, as shown in Figure 1. each of the plant units was modeled and then simulated using MatLab for which all the transient responses were obtained.

The * refers to the concentration on the catalyst surface. Mass balance Looking at small volume of the reactor V, the mass balance will follow the conservation law:

Heat balance For the solid catalyst in a small element x of the reactor, the heat balance can be expressed as in the expression below:

The material and energy dynamic models for acetylene converter as well as the reaction kinetic can be summarized as presented below. Reaction Rate and Mechanism The primary overall reactions taking place in the reactor are (several side reactions referred to green oil would be ignored[3]) C2H2 + H2 C2H4 C2H4 + H2 C2H6 reaction 1 reaction 2

The heat balance equation for the fluid (gas mixture) is presented in equation below

Several side reactions which lead to formation of C4 hydrocarbons and the heavy oligomer referred to as green oil were ignored[2]. The mechanism for reaction taking place in the acetylene hydrogenation reaction is complex as modeled by four consecutive steps.

Divided above equation by x and differentiated with limit x 0 yield the equation below

However the heat balance in the reactor for both solid and fluid has to share volume provided by the dimensions of the reactor such as the voidage . The heat balance will be as follow

Assuming that transferring between the solid and the fluid is infinitely good such that Tf = Ts = T, gives CO acts as a temporary poison by depriving C2H2 and C2H4 of surface area, thereby reducing their concentrations in the adsorbed phase. It was possible to describe the rates of the two reactions using: The model outlined above provides considerable insight into the mechanism and the dynamic of the reactor, but it was unsuitable for controller design[6,7,8]. It was highly non-linear and had many states corresponding to points on the finite difference mesh used to solve the partial differential equations. [x] denotes the concentration of the species. k1, k2, EA1 and EA2 are the appropriate pre-exponential factors and activation energies. Rc and Re are ratios between adsorption equilibrium constants as follows:

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A linear low order model was needed. Whilst the dynamic model have been subjected to some of linearization following by model order reduction, the resultant linear model would contain all the uncertainty of the full model plus the additional errors due to linearization and model order reduction. Thus, the energy linearized model for the converter can be represented by the following transfer function:

Where,

Tout

K Tin e ( D S ) ( s + 1)

2

Tin

KF ( s + 1)

2

F+

K CO ( s + 1) 2

CO

(1)

This model predicted the outlet temperature (Tout) as a function of the inlet temperature (Tin), flow rate (F) and carbon monoxide concentration (CO). There was a gain (K) associated with each input. The same second- order lag term was used for all inputs; in addition the effect of a change in the inlet temperature is delayed by dead time D. Composition dynamics are assumed to be similar to that of temperature dynamics. Therefore the Acetylene concentration model can be described by the following equation:

The dynamic responses of the converter (outlet temperature and concentration) to step changes in feed temperature, feed flow rate and carbon monoxide concentration are shown in Figures 4 to 9.

KTine( DS ) K KF Tin + F + CO 2 CO (2) 2 2 (s +1) (s +1) (s +1) The numerical values for parameters of the above two equations can be determined based on the followings: CC2H 2out =

1- assuming temperature rise across the converter bed equal to 20 oC 2- the value of the input temperature gain KTin equal to 2.3 oC/oC as calculated from Figure 2. 3- the ratio between gains (KF/KTin) was -0.14 0C/ (tone/hr), then KF=- 0.322. 4- The carbon monoxide concentration gain is constant and equal to -0.015 oC/ppm 5- The input temperature gain for acetylene concentration model KCin which represents the relationship between outlet acetylene temperature and inlet acetylene concentration at study state condition and equal to 0.001 oC/ppm 6- The time constant is fixed at 1.4 minutes. 7- Assuming the feed flow rate of gases mixture is equal to 52630 kg/hr. 8- Time delay can be found 2.5 minutes as calculated from Figure 3. By substituting all numerical values regarding parameters in equations 1 and 2, the converter material and energy balances can be modeled by the following matrix:

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Figure 8 Temperature response of acetylene converter to a step change in carbon monoxide concentration

Figure 9 Acetylene concentration response of acetylene converter to a step change in carbon monoxide concentration

The mathematical model for the shell and tube exchanger (see Figure 1) was derived based on unsteady-state energy balance and represented by the following transfer function:

(3) Figure 6 Temperature response of acetylene converter to a step change in the feed flow rate This model predicted the outlet temperature (Tout) as a function of the inlet temperature (Tin), steam flow rate (Fs) and feed flow rate (F). There was a gain (K) associated with each input. The steam heater responses to different step changes are shown in Figures 10 to 12.

The mathematical model for this shell and tube exchanger type (see Figure 1) was derived based on unsteady-state energy balance and represented by the following transfer function:

Tout ( S ) =

Figure 7 Acetylene concentration response to a step change in the feed flow rate

1.417 (0.098S+1)

(4)

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Figure 11 Temperature response of steam heater to a step change in steam feed flow rate

Figure 12 Temperature response of steam heater to a step change in feed flow rate This model predicted the outlet temperature (Tout) as a function of the inlet temperature (Tin), cooling water flow rate (Fw), cooling water temperature (Tw) and feed flow rate (F). There was a gain (K) associated with each input. The cooler responses to different step changes are shown in Figures 13 to 16.

Figure 15 Temperature response of intercooler to a step change in cooling water flow rate

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The responses of outlet temperature and acetylene concentration of the converter under PID controller are shown in Figure 18. Similarly, for the case of steam heater and intercooler, the closed loop responses of outlet temperatures under PID controller are shown in Figures 19 and 20 respectively.

4.

From the mathematical model of the converter in acetylene process, it appears that the real process was highly non-linear, and thus, a linearized model has been derived and represented by second order lag with dead time. To test the acceptability of the model, many dynamic responses (both outlet temperature and acetylene concentration) were obtained and all gave a reliable and acceptable level of accuracy. Also, the implementation of control system was shows a reliable and stable responses which agreed to that of process behavior. Also, The dynamic behaviors of steam heater and intercooler and aftercooler exchangers were both described by first order lag model. The temperature dynamic responses of both systems were at an acceptable level, and similarly for responses under control systems. From above, it can be recommended that the derived model for the Acetylene plant can be considered for applying advanced control strategies such as feedforward and or plant wide control for the overall plant control improvements.

3.

To study the dynamic behaviors of the acetylene hydrogenation plant under control, a conventional PID controller was used to control each units of the plant based on their derived models. The parameters of all controllers were determined by using the Cohen and Coon method. The construction of block diagram for temperature control of the converter is shown Figure 17, in which inlet temperature was chosen as manipulated variables and outlet temperature is the controlled variable. The best controller settings are presented in the Table below, Kc -2.5 Controller Parameters T1 TD 2.5 0.8

Figure 18 Responses of outlet temperature and acetylene of the converter under PID controller.

PID

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REFERENCES

1. Peacock, A. J., (2000) "Handbook of Polyethylene", Marcel Dekker, Inc., Basel, New York. 2. Schbib, N. S., Garcia, M. A., Gigola, C. E. and Errazu, G. A., "(1996) Kinetics of Front-End Acetylene Hydrogenation in Ethylene Production",Ind. Eng. Chem. Res. vol.35 pp. 1496-1505. 3. Mostoufi, N., Ghoorchian, A. and Sotudeh-Gharebagh, R., (2005), Hydrogenation of Acetylene: Kinetic Studies and Reactor Modeling", Int. J. Chem. React. Eng. Vol.3. 4. Cider, L., Schoon, N., (1993) "Hydrogenation of Acetylene at Transient Conditions in the Presence of Olefins and Carbon Monoxide over Palladium/Alumina", Ind. Eng. Chem. Res. vol. 30 , pp. 1437-1443. 5. Gobbo, R., Soares, R. P., Mandarin, M. A., Secchi, A. R. and Ferreira, J. M. P. , (2004) "Modeling, simulation, and optimization of afront-end system for acetylene hydrogenation reactors" ,Braz. J. Chem. Eng. vol.21 no.4 Oct./Dec. 6. Dakhil, H.M., (2007) "Integrated multi-unit controller design for chemical process plant", M.Sc. Thesis, University of Baghdad. Iraq. 7. Weiss, G. H., (1996) "Modeling and control of an acetylene converter", J. Proc. Cont. Vol. 6, No. 1, pp. 715. 8. Hobbs, J. W., (1979) "Computer control of Acetylene Hydrogenation Process", Industrial Process Control, AIChE Workshop, 7.

Figure 19 Temperature response of Steam Heater to a negative 100% step change in feed flow rate

Figure 20 Temperature response of the Intercooler to a negative 100% step change in feed flow rate

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