design and evaluation of a system to obtain polymer …

BRAZILIAN JOURNAL OF PETROLEUM AND GAS | v. 13 n. 4 | p. 323-332 | 2019 | ISSN 1982-0593

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DESIGN AND EVALUATION OF A SYSTEM TO OBTAIN POLYMER GRADE PROPYLENE BY MEANS OF VAPOR RECOMPRESSION DISTILLATION

a, b Fontana, M. 1; b Fernandes, L. M.; c Souza, T. A.

a University of Campinas (UNICAMP), School of Chemical Engineering, Campinas, SP, Brazil

b Federal Technological University of Paraná, UTFPR, Department of Chemical Engineering, Francisco Beltrão, PR, Brazil

c Federal University of Rio de Janeiro, Graduate Program in Technology of Chemical and Biochemical Processes, School of

Chemistry, Rio de Janeiro, RJ, Brazil

Received: 15.08.2019 / Revised: 03.11.2019 / Accepted: 03.11.2019 / Published on line: 20.12.2019

ABSTRACT Propylene in a purity degree above 99.5% (polymer purity grade- PPG) is a first-generation basic petrochemical that represents a vital link in refining-petrochemical integration. The strict specification of the product and the need to maximize the energy efficiency of the propylene/propane distillation process poses several challenges to the optimization of both the design and operation of the plant. Using a Petro-SIM (KBC) technology, a polymer grade general model from a propylene distillation unit was developed by means of vapor recompression. The sensitivity for feeding with different propylene fractions was analyzed, reaching a value of 0.94, which is considered the minimum propylene fraction in the feed required to the tower to generate a product with polymer purity grade. Based on the data obtained in the simulation, the tower was designed and evaluated by means of vapor recompression, showing a potential alternative way to obtain propylene at polymer grade which could be cost saving in industrial processes.

KEYWORDS propylene; distillation; steam recovery; simulation, design

1 To whom all correspondence should be addressed.

Address: School of Chemical Engineering, University of Campinas (UNICAMP), Av. Albert Einstein, 500 - Cidade Universitária, CEP, Campinas, SP, Brazil. ZIP Code: 13083-852 | e-mail: [email protected] doi:10.5419/bjpg2019-0027


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1. INTRODUCTION

The separation of propane/propylene mixtures is very important commercially for the chemical and petrochemical industry (Rege & Yang, 2002; He et al., 2018). Propylene is used in the production of polypropylene, acrylonitrile, acrylic acid, isopropanol, cumene, phenol, gasoline blend, trimmers, tetramers for detergents, propylene oxide, and oxo-alcohols (Gomes et al., 2009; Umo & Bassey, 2017; Roeentan et al., 2017; Ravanchi et al., 2010).

The most common way of obtaining propylene is via fluidized catalytic cracking or steam cracking; the latter accounting for 56% of the global propylene production (He et al., 2018; Kuah et al., 2018). An important source of propylene is through three-carbon hydrocarbons, which are obtained in several processes of refinement and cracking to which oil is subjected. The propylene produced in the refineries can be found in three specifications: (1) the refinery-grade, which has 50 to 70% of purity; (2) the chemical grade, containing between 90 and 95% of molar purity; and (3) the polymer grade, which exceeds 99.5% of molar purity (Umo & Bassey, 2017).

The polypropylene industry accepts only propylene at polymer purity grade (PPG) (Lopes, 2011). Polypropylene is a thermoplastic polymer, that is, it can be molded using heating. It is one of the most used olefin polymers because it does not include any polar group in its chain (Kawasumi et al., 1997). To produce polypropylene, propylene is polymerized through high catalytic activity, under controlled heat and pressure. Industrially, propylene is reacted with an organometallic, transition metal catalyst, to provide a site for the reaction to occur. Propylene molecules are added sequentially through a reaction between the metallic functional group on the growing polymer chain and the unsaturated bond of the propylene monomer (Maier & Calafut, 1998). Thus, high-purity propylene is necessary, since even low amounts of impurities deactivate the catalysis in the production of polypropylene (Mauhar et al., 2004).

Propylene is a highly flammable colorless gas. Its molecular formula is C3H6, and its boiling point is 225.45 K at ambient pressure. The propane molecular formula is C3H8 and its boiling point is

231.05 K at ambient pressure (He et al., 2018; GETIS, 2018). This similarity of propane and propylene boiling points makes it difficult to separate their mixtures, requiring the use of large-sized towers, increasing expenses due to the high-reflux stream (Briggs & Segers, 1971).

The propylene and propane mixture separation is conventionally carried out via distillation (Umo & Bassey, 2017). These processes involving distillation are the main consumers of industrial energy, accounting for 40 to 70% of capital and operating costs in a typical chemical plant (Bruinsma et al., 2012).

The propylene splitter is the last distillation column from the fractionation system of liquefied petroleum gas (LPG). Its purpose is to separate propane and propylene streams from other impurities (Lopes, 2011). The propylene feeding splitter varies in composition and this is the main process disturbance. The feed that arrives at the propylene splitter comes from the de-ethanizer, in which all the lighters of the stream (methane, ethanes, ethenes, CO, CO2, and H2S) are separated.

Aiming at producing propylene to supply the commercial demand, the industry is gradually adopting technologies such as propane dehydrogenation, olefin metathesis, and methanol to propylene. However, regardless of the technique used to obtain this product, the propane and propylene mixture is always generated, and it must be separated with one more process step (Umo & Bassey, 2017).

Nowadays, the propylene and propane are separated by distillation. Such process demands a great amount of energy because of the resemblance in their relative volatilities (Bruinsma et al., 2012; Ghosh et al., 1993). Due to the low thermodynamic process efficiency (Kazemi et al., 2017a) and the increasing of environmental requirements for quality petroleum products (Speigh & Heinemann, 2006), it becomes necessary to expand the knowledge about these systems. The low energy efficiency of the process lies in a large amount of energy required in the reboiler and in the thermal demand at a lower temperature in the condenser (Bruinsma et al., 2012; Ponce et al., 2015; Zygula & Kolmetz, 2011).

Due to the increase of oil prices and the growing market demand for propylene, the interest in


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developing new processes for propylene production has increased in recent years (Kazemi et al., 2017b). Therefore, processes such as vapor recompression, heat pump distillation (Kazemi et al., 2017c), thermally coupled distillation columns and internally heat-integrated distillation columns have been proposed to reuse the heat from the currents of their own system (Kazemi et al., 2017a). By means of process simulators, a plant can be operated in several conditions, determining which condition provides the optimum operating performance (Rocha, 2009).

The thermodynamic operation principle of a distillation system by vapor recompression uses work to produce temperature differences to allow for heat transfer (Luyben, 2018). The heat from the overhead vapor is upgraded by means of a compressor to such a level that its saturation temperature exceeds the reboiler temperature (Bruinsma et al., 2012). Therefore, the condensation heat can be used to drive the distillation column reboiler (Bruinsma et al., 2012). Because of this, no water stream is required in the reboiler (Coker, 2010), making the process economically attractive. Cost savings even greater than 42% can be achieved using the vapor recompression system (Harwardt & Marquardt, 2012).

The use of an appropriate process simulator makes it possible to quickly evaluate various industrial scenarios, and it is also useful to help in the decision-making process (Jorge et al., 2017). The Petro-SIM (KBC) simulator makes it possible to evaluate them. The use of these innovative technologies improves the management of the challenges facing the industry significantly. This platform integrates business data into a database system offering operational support for plant designs and for performance monitoring (KBC, 2017).

This work aims at evaluating the distillation process of vapor recompression to achieve propylene at a polymer purity grade using the simulator Petro-SIM (KBC). Moreover, a distillation tower was designed to find an efficient internal tower, aiming at reducing the cooler load to obtain an efficient and environmentally friendly process.

2. SIMULATION AND TOWER DESIGN

The propylene and propane distillation tower projects were carried out by the Petro-SIMTM software (KBC). The simulation was based on operational parameters such as temperature, pressure, flow rate, molar composition, and product composition obtained from the literature.

The plant design was assembled according to the vapor recompression distillation system discussed by Kazemi et al. (2018). The distillation tower was simulated with 190 theoretical stages with the main feeding into stage 121. Two recycles, one from the bottom stream fed into tray 190 and another from the top stream fed into stage 1 were considered. The thermodynamic package used was Peng Robinson, as accurately predicted by Kazemi et al. (2018) to describe a propane/propylene distillation system. Other data for the base case are shown in Table 1.

The purity degree obtained with the proposed conditions was evaluated, and a sensitivity analysis was performed, changing the propylene fraction at the tower feed. Since the tower distillation internals were designed based on a series of sizing calculations where tower internals were sized according to the methodology presented by Caldas et al. (2007).

Table 1. Base case data.

Stream Vapor (phase

fraction) Stage

Pressure [kPa]

Temperature [K]

Flow rate

[kmol/h]

Composition (molar fraction)

Energy [kW]

Propylene Propane

Feed 1.0 121 2240 348.75 376.4 0.9622 0.0378 -

Bottom_recycle 1.0 190 2240 333.19 4729.5 0,1971 0,8029 - Top_recycle 0.03 0.97 2200 325.83 4829.9 0.9958 0,0041 - Condenser - - - - - - - -4350

Compressor - - - - - - - 3054


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3. RESULTS AND DISCUSSION

Propane and propylene have similar molecular sizes and physical properties, which makes the process of separation problematic. The separation is generally performed in towers with a stage number between 150 and 200, with high reflux and high pressure (1600 to 2640 kPa), requiring high energy (Umo & Bassey, 2017; Gadalla et al., 2005). This justifies the use of 190 stages at the tower and high pressure (2200 kPa). According to Roeentan et al. (2017), distillation columns up to 100 m height that include about 200 trays with very large reflux ratio are usually required. Besides that, the number of trays is related directly to the column capital cost. A higher tray number means higher capital invested in the tower and a reduction on the capital invested in the heat exchanger, also reducing energy costs (Hussain & Lee, 2018). Likewise, high pressure values lead to a decrease in the column diameter, as the vapor density increases (Hussain & Lee, 2018).

The steam recompression system does not have a condenser and a reboiler coupled to the

distillation column. These two pieces of equipment were eliminated from the system to give rise to another type of current integration to supply the energy required. Even though they were not considered in the simulation, both condenser and reboiler still appear interconnected to the distillation column in the illustration. The justification for their presence is because the design of the tower in the simulator is fixed and does not change with their removal from the flowsheet. Based on the study of Kazemi et al. (2018), the process arrangement used in the simulation was organized. Figure 1 shows the configuration applied in the study, as well as the currents that interconnect the system.

The top stream that passed through the compressor was compressed from 2200 kPa to 5226.2 kPa. Its temperature was increased from 325.83 to 388.55 K and to the dew point. Then, the top stream was used to supply the energy to the bottom stream using a shell and a tube heat exchanger. Afterwards, the top product passed through the shell and its temperature decreased from 388.55 K to 351.85 K. The bottom stream

Figure 1. Propylene distillation by means of vapor recompression.


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passed through the tube. With this step, the bottom stream became vapor. Following, the bottom product returned to the bottom in a vapor recycle stream at 333.19 K. In the end, the top product underwent a pressure drop from 5226.2 kPa to 2200 kPa, as well as a cooling step to decrease its temperature from 325.83 K to 324,07 K, entering the tower as a liquid recycle stream, going to the top of the distillation tower (Kazemi et al., 2017c).

As shown in Table 2, at the top product, PGP was obtained in a molar fraction of 0.9959 and propane was obtained at 0.0041. This stream leaves the tower at a flow rate of 5189.4 kmol/h and only a part of it (355.8 kmol/h) is removed from the system, the remaining 4833.6 kmol/h return to the tower through the recycle stream from the top. These data corroborate the results obtained by Kazemi et al. (2018) in the Aspen Hysys simulator and in an operational plant. Both studies generated a flow of 359.9 kmol/h at the top in a propene molar fraction of 0.9960.

In the bottom stream, the composition of

0.8027 of propane and 0.1973of propylene was obtained at a molar fraction, leaving the tower at a molar flow of 4746.4 kmol/h. This stream passes through the heat exchanger, where it becomes purely vapor and its flow is divided between the recycle that returns to the tower (4725.84 kmol/h) and the product stream that leaves the system (20.56 kmol/h).

The simulation was also studied by varying the propylene molar fraction in the main feed stream. In this study, the main feed composition stream was considered to contain propylene and propane. This analysis was carried out to obtain, for the same processing conditions, the feed containing lower propylene molar fraction that still provided PGP as the product from the top stream. The more propylene at the feed also contributes to more propylene at the top (Fig. 2) and bottom (Fig. 3) stream.

The lowest molar fraction of propylene in the tower feed that made it possible to obtain the polymer grade propylene at the top was 0.94 of propylene, with the remaining 0.06 of propane

Table 2. Base case output process data.

Stream Molar fraction

Flow rate [kmol/h] Density [kg/m3]

Propylene Propane

Top product 0.9958 0.0042 5189.4 48.71

Bottom product 0.1973 0.8027 4746.4 407.2

Propane 0.1973 0.8027 20.56 51.85

Propylene 0.9958 0.0042 355.8 344.84

Figure 2. Sensitivity analysis of propylene at the top stream.


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molar fraction. With this feed composition, it was possible to generate PPG with molar composition of 0.9953 of propylene and 0.0047 of propane at a molar flow rate of 352.4 kmol/h. In addition, under these conditions, a bottom stream with propylene molar composition of 0.1134 and 0.8866 of

propane was generated, leaving the system in a flow rate of 23.96 kmol/h.

The presence of impurities, such as n-butane, even in low fractions in the feed composition can be listed as a negative factor in yield. Table 3 shows

Figure 3. Sensitivity analysis of propylene at the bottom stream.

Table 3. Analysis with the presence of n-butane in feed composition.

Chemical species Molar fraction

Feed Top product Bottom product

Propylene 0.9600 0.9958 0.1982 Propane 0.0350 0.0042 0.8023 n-butane 0.005 0 0.0003











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the composition obtained in the top and bottom products with the presence of n-butane in the feed at different molar fractions.

For the less favorable feed conditions (rich in C4 and low in propylene), the model has difficulty at converging, a condition that is only reached when there is strict specification control of the maximum fraction of C4 (<0.0055 molar fraction) in the upstream process (depropanizer).

The top distillation product almost reaches the temperature to be used as a thermal source, but it is usually incapable of direct utilization, being treated as waste heat in conventional processes

(Galvão, 2016). The vapor recompression technology is used to upgrade the heat by compressing the vapor distillate, emerging as a cost saving opportunity (Kiss et al., 2012). In a context in which automation technologies guide the necessary process evolution industry to the technological level idealized for Industry 4.0, the development of in silico chemical processing model assumes fundamental importance for the development of advanced manufacturing tools and technologies (Joly et al., 2018).

According to Kazemi et al. (2018), the vapor recompression results in a 73.6% reduction in cold utility process requirements when compared to the

Table 4. Tower project.

Parameter Value Unit

dp (Droplet diameter) 25 mm g (Acceleration of gravity) 9.81 m/s

2

Cd (Drag coefficient) 0.7 - Ffluid (Fluid factor) 0.9 -

Fsystem (System Factor) 0.9 - CFSgas (Volumetric flow rate of gas in tray conditions) 0.115 m

3/s

Fflood (Flood factor for the system) 0.8 - GPM (Liquid flow) 407.2 m

3/h

X (Souders and Brown factor) 0.307 - Vn (Gas velocity) 0.0605 m/s

CSB (Souders and Brown constant) 0.0216 m/s Vaf (Maximum gas velocity in a tower running on the air-water system) 0.0605 m/s

Vf (Maximum steam speed) 0.049 m/s Af (Free area) 2.93 m

2

VDSG (Maximum downcomer speed) 0.234 m/s Adm (Minimum downcomer area) 4.502 m

2

Atower (Tower area) 7.435 m2

Dt (Tower diameter) 3.076 m hw (Output spout height) 60 mm

Dynamic seal 75 mm Ada (Area under the downcomer) 0.225 m

2

Lw (Length of downcomer) 3.032 m H (Downcomer height) 1.795 m

hud (Clearance on the downcomer for the entry of liquid into the tray) 74.339 mm Number of main indents 1 -

αfd (Area of all trays drain holes) 0.002 m2

td (Drainage time) 6 min Trapdoor size 0.45 x 0.6 m

“Dead area” (Area on the tray holder without valves or holes) 0.063 m NPASSE (Tray number passes) 2 -

FPL (Length of liquid path) 13.84 m Δ (Hydraulic gradient) 0.848 m

ΔPd (Pressure drop on downcomer output) 0.024 m

ΔPiw (Pressure drop on inlet spillways) 0.0004 m

hd (Downcomer pressure drop) 0.024 m Valve Specification 14 gage

Tray thickness 1.88 mm Tray hole diameter 38 mm

Perforated area 0.351 m2

Center to center valves distance 75 mm Valves number per tray 378 -


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conventional distillation column that requires the highest net energy for its operation and application. This system shows significant improvement in the process regarding energy-saving. Therefore, it is a great process intensification system (Niu & Rangaiah, 2016), showing operating cost savings for the production of propylene at the polymer purity grade.

Although the simulation provides a lot of information about products, tower configuration characteristics needed to be further developed with another methodology. To verify whether the process data and the plant configurations are applicable to the industry, a methodology of project calculations was applied. Considering the parameters used in the design calculations, as well as the parameters obtained in response, all factors used in the project were checked. Table 4 shows the main parameters obtained in the literature to the project and the calculated ones by the equations presented by Caldas et al. (2007).

The diameter calculated for the tower was 3.07 meters. This is also supported by the work of Umo and Bassey (2017) in a propylene distillation tower, where they used three meters of diameter tower to system with 290.7 kmol/h at the feed. Towers with two passages must be at least two meters in diameter (Caldas et al., 2007). Because the tower diameter is of approximately three meters, it was chosen for the two-passage plate.

The perforated area should be 8 to 15% of the active area, where optimum value is 12% (Caldas et al., 2007). The value obtained for this parameter was 0.351 m2. In addition, the number of valves per plate obtained was equal to 378. These values corroborate what was used by Mauhar et al. (2004). Their work presents a system to distillate propylene with a valve tray type with two passages and with 388 holes per tray. This result shows that the tower size for a vapor recompression system can be kept the same for processes that are already operating by conventional distillation. This allows the use of the same tower to make the alteration in the steam recompression system generating energy and cost savings, without the need to build a new column for the vapor recompression process.

4. CONCLUSIONS

The distillation with vapor recompression was effective for the PPG separation at feeds with molar propylene fractions over 0.94. The model was robust but significantly sensitive to different feed qualities. This vapor system recompression can show cost savings in the process, being a great choice to separate propylene from propane.

It was possible to note that the propylene fraction was reduced in the feed, and so was the top thermal load. Therefore, the investments required for the condenser also decreased. In addition, it was possible to see that the efficient feed control composition is a critical variable for the process energy optimization, since it affects the performance and the convergence of the simulation directly.

The tower was designed considering valve trays. The sizing resulted in a diameter pursuant to that found in the literature for other processing systems with the same load, which shows that it is suitable for applications in processes already used in industrial operation.

ACKNOWLEDGMENTS

The authors would like to recognize the Federal Technological University of Paraná for the support provided.

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