Journal of Natural Gas Science and Engineering 26 (2015) 1011e1017

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Journal of Natural Gas Science and Engineering

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Sweetening liquefied petroleum gas (LPG): Parametric sensitivity

analysis using Aspen HYSYS
Hanan Jalal Qeshta a, b, Salaheddin Abuyahya a, Priyabrata Pal a, Fawzi Banat a, *
a
The Petroleum Institute, Um al Naar, Abu Dhabi, United Arab Emirates
b
Takreer Refinery, Engineering Division, Abu Dhabi, United Arab Emirates

a r t i c l e i n f o a b s t r a c t

Article history: The current investigation aims at studying LPG sweetening process using tertiary alkanolamine (meth-
Received 12 May 2015 yldiethanolamine; MDEA) by Aspen HYSYS version 8.0. Design criteria were explained for sweetening
Received in revised form LPGs including MDEA concentration, mass flow rate, circulation rate etc. The effects of operating pa-
28 June 2015
rameters such as temperature and pressure on the proposed process were also studied. A steady state
Accepted 3 August 2015
Available online 7 August 2015
model was developed for determining the sensitivity of parameters affecting the process. The most
suited feed LPG temperature was determined to be 45
C. The optimum MDEA concentration and flow
rate was found to be 35.0 wt% and 24.43 m3/h, respectively. The parameters which indirectly affect the
Keywords:
Liquefied petroleum gas
extraction process such as reboiler operating pressure, rich MDEA temperature, reflux ratio and boilup
Sweetening ratio were also determined.
Methyldiethanolamine © 2015 Published by Elsevier B.V.
Extraction
Aspen HYSYS

1. Introduction drawback of molecular sieve includes large capital and operating

costs as well as catalyzing the formation of COS when both H2S
The demand for liquid hydrocarbon sweetening facilities has and CO2 are present. The uses of alkanolamines is currently
increased with the rise in the production of liquefied petroleum becoming popular, especially in plants where alkanolamines are
gas (LPG). The most common contaminants present in LPG are being used to sweeten acid gases. It is considered one of the most
hydrogen sulfide (H2S), mercaptans (RSH), carbon dioxide (CO2), cost effective processes when significant amounts of sulfur im-
carbonyl sulfide (COS), carbon disulfide (CS2) and elemental sulfur purities are present, as it can be regenerated and recycled back to
(Holmes et al., 2006). H2S is corrosive and its presence can lead to the system. Currently, Takreer (Abu Dhabi Refinery; ADR) is using
deposition of free sulfur (Perry, 1977). Mercaptans are usually nearly 2e3 m3/h of caustic for sweetening LPG. The research work
added in small quantities for odorizing but if it is present in larger discussed in this article may replace the existing LPG sweetening
quantities it impart a bad odor and cause combustion of flue gases. unit with MDEA. Takreer has MDEA regeneration system which is
The COS can hydrolyze to H2S which become sour after settling in currently circulating at 50 T/h with design capacity of 110 T/h.
a tank. If both COS and water are present in LPG, removal of COS is Design feed information is supplied from the operating procedure
essential. The presence of CO2 can also cause problems if LPG is in order to simulate the model.
treated with caustic as CO2 cause huge caustic losses. If the The basic objective of this work was to study LPG sweetening
quantities of the contaminants are less, a caustic wash is useful using methyldiethanolamine (MDEA) by Aspen HYSYS version
(Ghanbari et al., 2003). However, for larger amount of contami- 8.0. The simulation work was carried out in two parts to simulate
nants caustic wash is quite expensive and disposal of wastes is LPG sweetening and finally conduct a sensitivity analysis of the
another major concern. For large quantities of contaminants mo- process plant. Design criteria were selected using different types
lecular sieves (Zhang et al., 2014) and alkanolamine (Fleming et al., of alkanolamine, feed LPG temperature and flow rate, MDEA
2006) treating systems can be used effectively. The major concentration, circulation rate etc. The effect of process param-
eters such as temperature, pressure and the parameters which
indirectly affect the extraction process (e.g. reboiler operating
pressure, rich MDEA temperature, reflux ratio and boilup ratio)
* Corresponding author. were also determined.
E-mail address: [email protected] (F. Banat).

http://dx.doi.org/10.1016/j.jngse.2015.08.004
1875-5100/© 2015 Published by Elsevier B.V.
1012 H.J. Qeshta et al. / Journal of Natural Gas Science and Engineering 26 (2015) 1011e1017

2. Process description 2.3. MDEA circulation rate

2.1. Selection of alkanolamine The circulation rate of lean MDEA is best determined by equi-
librium loading calculations based on acid gas content of the feed,
Alkanolamines are characterized by containing both hydroxyl concentration of MDEA used and acid gas loading. A range of
and amino groups. The hydroxyl groups serve to increase solubility 0.4e0.55 mol acid gas/mole alkanolamine was specified for the acid
in water and decrease vapor pressure; while, amino groups provide gas loading in rich MDEA (Ridnay and Parrish, 2006). In this study,
the alkalinity of solution required for reaction between acid gases simulation will be performed to estimate the required MDEA cir-
and the aqueous phase (Kohl and Nielsen, 1977). Monoethanol- culation rate for the variation of acid gas content and MDEA con-
amine (MEA) is a primary alkanolamine containing a primary centration. In this simulation an intermediate value of 0.45 is
alcohol and a primary amine while, diethanolamine (DEA) is a considered and the lean MDEA flow rate will be calculated.
secondary amine which contains two primary alcohols. Other key
tertiary alkanolamine solvents include methyldiethanolamine 2.4. Lean MDEA temperature
(MDEA) and triethanolamine (TEA) (Blauwhoff et al., 1984). Alka-
nolamines of different degrees can be used for sweetening LPG. The MDEA temperature entering the extraction column should
MEA undergoes irreversible degradation with COS/CS2/CO2 and is be 4e6
C higher than the inlet feed LPG temperature to prevent
characterized by higher solution vaporization losses due to highest condensation of hydrocarbon in the contactor. The inlet feed LPG
vapor pressure of the alkanolamines used for gas treating (GPSA, enters the extraction column at 38e48
C and the range of lean
2011). Other disadvantages include ineffective mercaptan MDEA temperature is 46e57
C. The lean MDEA temperature
removal, non-selective H2S removal and higher utility costs. Since should not exceed the limit as it could lead to poor solvent per-
selective H2S removal over CO2 is desired, a tertiary alkanolamine is formance or increase solution losses due to vaporization.
preferable (Lu et al., 2006). However, TEA was unable to remove H2S
and CO2 at low concentrations. Hence MDEA was the best choice to 3. Process simulation
remove H2S selectively, having lower vapor pressure, with lower
solution flow rates and thus requiring smaller regeneration unit. 3.1. Fluid package and components
In a counter current reversible extraction process, sour LPG
enters at the bottom of the column and flow upward in intimate The flow sheet for LPG sweetening using MDEA was developed
contact with lean MDEA. The heat of reaction between MDEA and in Aspen HYSYS (Øi et al., 2014) version 8.0 using ‘amine package’.
the acid gas is exothermic so it will raise sweet LPG temperature The composition of sour LPG and process parameters were pro-
leaving from the top of the column. The MDEA solution loaded with vided by Takreer, Abu Dhabi Refinery (ADR). The LPG sweetening
acid gas, known as rich MDEA leaves from the bottom of the col- unit had a designed capacity of 3780 barrels per stream day (BPSD)
umn. The reactions during the process are as follows: (25 m3/h). Table 1 shows the composition of sour LPG stream as per
design criteria.
R2 NCH3 þ H2 S4R2 NHCH3 HS (1)
3.2. Simulation environment
where, H2S is reacted instantaneously with MDEA to form
methyldiethanolamine-sulphide salt. However, CO2 forms carbonic Sour LPG as liquid feed at 45
C and 39.23 bars was fed to the
acid as intermediate with water given by Reactions (2) and (3). bottom of the column containing 10 stages having flow rate
24.43 m3/h. 35.0 wt% lean MDEA (stream 3) was fed at the top of the
CO2 þ H2 O/HCO
3 þH
þ
(2)
extractor at 40.21 bars and at elevated temperature of 6
C higher
than sour LPG as shown in Fig. 1. The actual operating composition
CO2 þ OH /HCOþ
3 (3) was recalculated using Aspen HYSYS when the sweetening process
was completed and the regenerated MDEA was recycled back to the
Reactions (2) and (3) are slow to produce carbonic acid which
extraction column. The circulation rate of lean MDEA was found
reacts with MDEA to form methyldiethanolamine-bicarbonate
using ADJUST logical operation in Aspen HYSYS with molar flow
(Younas and Banat, 2014).
(0.59 kmol/h) as an adjustable variable having mole fraction 0.0023
R2 NCH3 þ Hþ HCO þ  of H2S in rich MDEA (stream 4) as a target variable and selected
3 4R2 NHCH3 HCO3 (4)
sour LPG flow rate of 259.2 kmol/h to completely remove H2S from
where, R ¼ C2 H4 OH sweet LPG.
Reaction (4) predominates when both H2S and CO2 are present The simulation required 10 iterations to match the target value
and proceeds to the right at low temperature as forward reaction is with a circulation rate of 4512 kg/h (equivalent to standard liquid
exothermic. volumetric flow rate, 4.458 m3/h). At this rate, 100% of the H2S from
feed LPG was removed. Table 2 shows the simulation results of
extraction column.
2.2. MDEA concentration
3.3. Effect of H2S loading
The chosen MDEA concentration was usually made on the basis
of effective sour gas removal (Pal et al., 2014). Increasing MDEA The effect of H2S loading was studied when the sweetening
concentration reduces solution circulation rate. In fact, the prin- process was completed and the regenerated MDEA was recycled
cipal reason being that acidegas vapor pressure is higher over more back to the extraction. 35.0 wt% aqueous MDEA with H2S loading
concentrated solutions at equivalent acidegas/alkanolamine mole was simulated and the developed Aspen HYSYS flow sheet is shown
ratios. Additionally, when an attempt is made to extract the acid gas in Fig. 2. The treated LPG left the top of the contactor at an elevated
from smaller volume of solution, the heat of reaction results in a temperature of 49
C and 39 bars while the rich MDEA solution left
greater increase in temperature, with consequently increase in the bottom at 44.76
C and 41.19 bars. The rich solution flowed into
acidegas vapor pressure over the solution. a flash drum, where most dissolved hydrocarbon gas and some acid
 H.J. Qeshta et al. / Journal of Natural Gas Science and Engineering 26 (2015) 1011e1017 1013

Table 1
The composition of sour LPG stream as per design.

Component H2S H2 H2O C1 C2 C3 nC4 iC4 C5

Mole fraction 0.0023 0.0007 0.0011 0.0106 0.1320 0.2669 0.4137 0.1676 0.0048

gas flash off. The rich MDEA was then heated to a temperature of
98.89
C in lean/rich MDEA exchanger before being introduced into
the regenerator column. Rich MDEA was fed to the feed tray
number 1 of regenerator having a total number of 20 stages. In the
regenerator, stripping steam was used for the regeneration of rich
MDEA. The stripping steam was produced with the help of a
reboiler which used low pressure steam (5 bars at 158
C) for
reclaiming the latent heat of vaporization. Regeneration process is
endothermic and is favored by high temperature and low pressure.
Operating temperature and pressure range for regenerator column
were 117
C (top stage)-122
C (bottom stage) and 1.67e2.025 bars,
respectively. The rich MDEA solution flowed downward through
the stripper in countercurrent contact with vapor generated in the
reboiler which stripped the acid gas from the rich solution. Stripped
acid gas left the regenerator column at the top of the regenerator.
Entrained water vapors and hydrocarbons were separated from the
acid gas through a full reflux condenser. The regenerator top
product (acid gas and water vapor) was condensed (by water or air)
Fig. 1. HYSYS model built-up for extraction column. and collected in the reflux drum. The overhead stripper product

Table 2
Simulation results of extraction column.

Parameters MDEA (stream 3) Sour LPG Rich MDEA (stream 4) Sweet LPG

Temperature,
C 51.31 45.0 44.76 49.14

Pressure, kPa 4021.0 3923.0 4119.0 3908.0
Molar flow, kmol/h 175.7 259.2 175.9 259.1
Volumetric flow rate, m3/h 4.458 24.43 4.479 24.40

Fig. 2. Developed Aspen HYSYS process flow-sheet for LPG sweetening.

1014 H.J. Qeshta et al. / Journal of Natural Gas Science and Engineering 26 (2015) 1011e1017

from the reflux drum was the wet acid gas which could be routed
either to an acid gas flare or to sulfur recovery unit. Condensed
water from the reflux drum was pumped back to the top of the
column (reflux pump) to serve as reflux. Lean MDEA from the
reboiler was pumped to lean/rich MDEA exchanger where energy
was recovered from the lean MDEA. The lean MDEA was then
mixed with makeup MDEA to account for MDEA losses (vapor-
ization, chemical losses and mechanical losses). After that, the so-
lution was cooled down through a cooler to adjust the temperature
to the appropriate treating temperature in the extractor. The stream
was then pumped back into the top of the extractor to continue the
sweetening of the sour LPG.
The MDEA flow rate was considered as minimum when rich
MDEA leaving the extractor was in equilibrium with the entering
sour LPG. This was simultaneously done through the recycle block
iterations where the simulation got converged at a circulation rate
Fig. 3. Effect of feed LPG temperature with H2S concentration in sweet LPG and
4.458 m3/h resulting in a better product purity of LPG. reboiler duty.

4. Results and discussion

feed LPG temperature of 45
C seemed to be good for extraction
4.1. Validation of simulation results process.

First step of this study was the development of LPG sweetening 4.3. Effect of feed LPG flow rate
process using Aspen HYSYS version 8.0 and comparing the model's
results with DOW Chemical Company's result (Table 3). The sweet Fig. 4 shows the effect of sour LPG mass flow rate on the content
gas LPG specification for H2S is 10.0 ppm. Finally, parametric of H2S in the sweet LPG. The H2S concentration in sweet LPG
sensitivity analysis was carried out to validate the model. Process decreased (1.73e1.47 ppm) very less and considered almost con-
Parameters were changed accordingly associated with extraction stant as the flow rate of sour LPG was varied from 5000 kg/h to
and regeneration to perform the case studies. The optimized 20,000 kg/h. The reboiler duty increased from 377 kW to 385 kW.
simulation conditions were maintained in all the studies while The design sour LPG flow rate was 13,000 kg/h having reboiler duty
changing one parameter at a time. of 381 kW. Thus treated LPG served well below the permissible
limit of H2S concentration for larger sour LPG mass flow rate. As the
4.2. Effect of feed LPG temperature sour LPG mass flow rate increases, the mass flow rate of H2S in
sweet LPG also goes high causing decrease in H2S concentration.
A case study was made to predict the plant behavior under
different feed LPG temperatures keeping temperature difference
4.4. Effect of MDEA concentration
between feed LPG and lean MDEA constant (6.3
C). Temperature
ranges from 30
C to 60
C of feed LPG would be able to determine
MDEA concentrations have a direct effect on the extraction of
the effect of H2S content in sweet LPG and reboiler duty (Fig. 3). As
the acid gas in the extraction column. The MDEA could be operated
the feed LPG temperature increased from 30
C to 40
C the H2S
efficiently from 25 to 45 wt%. Fig. 5 illustrates the effect of varying
concentration in sweet LPG (more than 2.0 ppm) and reboiler duty
MDEA concentration on extraction of H2S and MDEA regeneration
(378.0 kW) remains almost constant. Between 40 and 45
C, the H2S
energy requirements. The design MDEA concentration was
concentration of sweet LPG decreased at the expense of more en-
considered to be 35.0 wt%. It was observed that as MDEA concen-
ergy requirement on reboiler. Beyond 45
C, the ability of MDEA to
tration increased a steady increase in reboiler duty took place while
extract acid gases was decreased which justify the exothermic re-
action behavior. At an intermediate reboiler duty of 381.8 kW, the

Table 3
Comparison of physical parameters and compositions (mole fraction) using Aspen
HYSYS and DOW Chemical Company's results for treated sweet LPG and acid gas (in
brackets) at simulated conditions.

Parameter DOWa Aspen HYSYS

Temperature,
C 47.3 (48.88) 49 (48.66)

Pressure, bar 39 (1.659) 39 (1.679)
Flow rate, kg/h 1.294  104 (23) 1.299  104 (21.2)
Water 1.21  103 (7.041  103) 3.14  103 (6.97  103)
H2S 7  106 (0.8622) 2  106 (0.906)
H2 7.3  104 (8.959  105) 7.32  104 (2.951  105)
Methane 1.06  102 (8.635  104) 1.06  102 (7.12  104)
Ethane 0.1326 (2.743  103) 0.132 (9.1  103)
Propane 0.2671 (1.91  102) 0.2670 (1.37  102)
n-butane 0.4147 (1.944  102) 0.4139 (1.0  104)
iso-butane 0.1683 (2.485  102) 0.1678 (2.75  104)
n-pentane 4.812  103 (3.435  104) 4.815  103 (1.53  105)
Fig. 4. Effect of feed LPG flow rate with H2S concentration in sweet LPG and reboiler
a
The data is published with due permission from DOW Chemical Company. duty.
 H.J. Qeshta et al. / Journal of Natural Gas Science and Engineering 26 (2015) 1011e1017 1015

Fig. 5. Effect of MDEA concentration with H2S concentration in sweet LPG and reboiler
duty.
Fig. 7. Effect of lean MDEA temperature with H2S concentration in sweet LPG and
reboiler duty.
H2S concentration in the treated LPG was lowered
(1.27 ppme0.96 ppm).
gradually increased with the increase in lean MDEA temperature.
4.5. Effect of lean MDEA circulation rate This is due to exothermic nature of extraction of H2S in MDEA in
which the H2S concentration in treated LPG was low at lower lean
The lean MDEA circulation rate is another major parameter MDEA temperature (i.e. MDEA extraction is favored at low tem-
which is directly related to the extraction of acid gas from LPG. The perature) as mentioned earlier. At higher temperature, solubility of
lean MDEA circulation rate was changed from 4000 to 5000 kg/h as H2S in aqueous MDEA is decreased, thus H2S concentration grad-
shown in Fig. 6. As the MDEA circulation rate was increased the H2S ually increases with the increase in lean MDEA temperature. As
concentration in sweet LPG also increased due to lower residence lean MDEA temperature increased, the additional heat load on
time. The minimum flow rate as per simulation was found to be reboiler decreased. There was also slight decrease in reboiler duty.
4512 kg/h. Generally, little higher flow rate is always recommended
in the plant to accommodate any abnormality in H2S concentration 4.7. Effect of rich MDEA temperature
in feed LPG. Again, increasing the circulation rate of lean MDEA
causes an increase in reboiler duty (370e395 kW) of the The rich MDEA temperature was varied from 85
C to 115
C to
regenerator. check the benefits of acid gas stripping and the reboiler duty as
shown in Fig. 8. Since stripping of acid gases is endothermic, it
4.6. Effect of lean MDEA temperature favors high temperature. Thus, increasing regenerator feed tem-
perature, eventually reduces the energy load on the reboiler
Temperature of lean MDEA could directly affect the extraction of (445e300 kW). However, acid gas breakout at high rich MDEA
acid gas. Design temperature of lean MDEA for extraction was temperatures is another concern. If a large amount of gas breakout
50e60
C. As shown in Fig. 7, the lean MDEA temperature was is present, erosion/corrosion can occur on both the exchanger as
varied to study its effect on sweet gas composition and energy well as in the process lines of the stripper. Generally, a temperature
requirements in reboiler. The H2S concentration in the treated LPG range of 99
Ce108
C is considered to avoid acid gas breakout and
erosion/corrosion problems in the equipment.

Fig. 6. Effect of lean MDEA circulation rate with H2S concentration in sweet LPG and Fig. 8. Effect of rich MDEA temperature with H2S concentration in lean MDEA and
reboiler duty. reboiler duty.
1016 H.J. Qeshta et al. / Journal of Natural Gas Science and Engineering 26 (2015) 1011e1017

4.8. Effect of regenerator stages

The effect of addition/removal of stages (10e28) in the regen-

erator from designed number of 20 stages is studied (Fig. 9). There
is a decrease of H2S concentration in the lean MDEA stream
(800 ppme550 ppm) as the total numbers of stages are increased
(from 20 to 28 stages). The reboiler duty decreases from 327 kW to
313 kW for this increment. As number of stages is removed below
designed number of stages, an increase in H2S concentration of
800 ppme1200 ppm in lean MDEA as well as in the reboiler duty of
327 kWe377 kW is observed.

4.9. Effect of reboiler pressure

To observe the effect of reboiler pressure, it is varied from 1.8 to Fig. 10. Effect of reboiler pressure with H2S concentration in lean MDEA and reboiler
3.4 bars (design reboiler pressure is 2.1 bars) and the H2S concen- duty.

tration in lean MDEA and the reboiler duty is observed as shown in

Fig. 10. Generally, stripping is conducted at low pressure and high
temperature. Pressure should maintain in such a way that reboiler
temperature does not exceed 130
C (Kohl and Nielsen, 1977) and
should control thermal degradation of alkanolamines (Stewart and
Lanning, 1994). It is evident from the simulation result that
increasing reboiler pressure increases the reboiler duty from
288 kW to 418 kW whereas H2S concentration in lean MDEA is
decreased from 996 ppm to 643 ppm.

4.10. Effect of reflux ratio

Some of the distillate fed back to the regenerator is known as

reflux. The design reflux ratio for this process is 33.5. Varying the
reflux ratio in the regenerator affects the H2S concentration in lean
MDEA as well as reboiler duty as shown in Fig. 11. Since overhead
temperature of the regenerator is an indication of the amount of
stripping steam being generated in the reboiler, the regenerator
Fig. 11. Effect of reflux ratio with H2S concentration in lean MDEA and reboiler duty.
column was made to converge by specifying different reflux ratios
and setting the overhead temperature at 48.8
C. Lowering the
reflux ratio decreases the reboiler duty from 378 kW to 289 kW but
increases H2S concentration from 1000 ppm to 1400 ppm in lean another parameter which explains the H2S content in lean MDEA.
MDEA. Fig. 12 shows the change in H2S concentration in lean MDEA and
reboiler duty with change of boilup ratio. The decrease of boilup
4.11. Effect of boilup ratio ratio below the design (0.195) results in reduction of reboiler duty
and increase in H2S concentration in lean MDEA which decreases
The reboiler is used to boil the Rich MDEA to vaporize which H2S concentration in the treated LPG. Higher boilup ratio yields
results the boilup (V) to return to the regenerator and the lean better quality sweet LPG at higher reboiler duty of 488.7 kW.
MDEA (B) is returned back to the extractor. The boilup ratio (V/B) is

Fig. 9. Effect of regenerator stages with H2S concentration in lean MDEA and reboiler
duty. Fig. 12. Effect of boilup ratio with H2S concentration in lean MDEA and reboiler duty.
 H.J. Qeshta et al. / Journal of Natural Gas Science and Engineering 26 (2015) 1011e1017 1017

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