Journal of Natural Gas Science and Engineering 34 (2016) 499e508

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Journal of Natural Gas Science and Engineering

journal homepage: www.elsevier.com/locate/jngse

Microfluidic cold stripping of H2S from crude oil in low temperature

and natural gas consumption
Mohammad Hassan Almasvandi, Masoud Rahimi*, Yaghoub Tagheie
CFD Research Center, Chemical Engineering Department, Razi University, Kermanshah, Iran

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

Article history: This study presents the results of removing H2S from crude oil using a micro scale stripper. The main
Received 29 April 2016 issue in this work is reduction of natural gas consumption and use of low operational temperature. The
Received in revised form effects of various operational parameters (such as: crude oil flow rate, natural gas flow rate and tem-
1 June 2016
perature of crude oil) on H2S removal efficiency (efficiency) and Specific Energy Consumption (S.E.C) are
Accepted 9 July 2016
evaluated. The obtained results, even for lower amounts of the used gas (about one-third) and lower gas
Available online 11 July 2016
temperature (about 18
C), show a higher efficiency of cold stripping using microchannel compared with
other type of strippers. This superior result, with an efficiency of 77.80%, is related to efficient mixing by
Keywords:
H2S
the employed microchannel at the proposed condition. It has been demonstrated that the efficiency
Cold stripping increases with increasing the temperature of crude oil and natural gas flow rate, while temperature does
Crude oil not show a considerable effect on S.E.C. The efficiency and SEC have decreasing trend with increase in
Natural gas flow rate of crude oil at constant temperature and gas flow rate. The mathematical modeling is proposed
Microchannel for H2S removal and the relation between the parameters was determined using Response Surface
Response surface methodology Methodology (RSM) with Central Composite Design (CCD) method. The values of R2 and lack of fit (LOF),
obtained from the mathematical model for efficiency, are 0.9589 and 0.2126, respectively. In addition, the
values of R2 and LOF for S.E.C are 0.9981 and 0.0606.
© 2016 Elsevier B.V. All rights reserved.

1. Introduction
Sulfur compounds, like hydrogen sulfide as a malodorous gas,
causes many deteriorate effects on crude oil equipment (Duan et al.,
2004). It is the main source of the acid rain as oxidized to sulfur
oxide (Ko et al., 2004). H2S causes the aggravated corrosion con-
ditions when it is mixed with oil and leads to the highest equip-
ment failure in the petroleum industry (Lee and Kumar, 2013).
Purification of the petrochemical products from H2S has paramount
importance from environmental, economic and operational re-
quirements points of view (Su et al., 2010a). Stripping the crude oil
with cold or hot gas in large volume equipment is a mechanical
methods for sulfur components removal (Abdel-Aal et al., 2003;
Allen et al., 1987; Chasanis et al., 2011; Clanton and Gipson, 1969;
Mock, 2010; Stiver and Mackay, 1984), but the main disadvantage
of this method is its high cost and being timeconsuming (Vaezi
et al., 2011).
* Corresponding author. Chemical Engineering Department, Razi University,
TagheBostan, Kermanshah, Iran.
E-mail addresses: masoudrahimi@yahoo.com, m.rahimi@razi.ac.ir (M. Rahimi).
The cold stripping is a simple and desired method to flare the
overhead gas product. The rich gas in the top of the tower may be
cooled, compressed and treated in contact with a physical solvent
with famous techniques (Abdel-Aal et al., 2003).
In some studies, natural gas has been used as sweetening gas in
cold stripping process (Iijima, 1991). Several methods can be used
to remove hydrogen sulfide. Some of the methods such as: Chem-
ical oxidants (Mohammadbeigi and Tajerian, 2004), Caustic scrub-
bers (Chen et al., 2001), Adsorption (Kulkarni and Shinde, 2014),
H2S scavengers (Avila et al., 2000), Amine absorption units (Siefers
et al., 2010), Physical solvents (Siefers et al., 2010), Membrane
processes (Wiheeb et al., 2013), biological methods (Zhang et al.,
2008) and stripping (Vaezi et al., 2011) are more common in in-
dustrial processes. Choosing the proper process can depends on the
amount of gas composition, end-use of gas and the physical char-
acteristics of gas. Hydrogen sulfide removal processes can be either
physical, chemical or biological (Siefers et al., 2010). Sulfur com-
ponents can be removed completely using some chemical methods
but these methods are costly (Mohammadbeigi and Tajerian, 2004;
Siefers et al., 2010). The chemical and biological H2S removal pro-
cesses are expensive because of high energy, chemical

http://dx.doi.org/10.1016/j.jngse.2016.07.021
1875-5100/© 2016 Elsevier B.V. All rights reserved.
500 M.H. Almasvandi et al. / Journal of Natural Gas Science and Engineering 34 (2016) 499e508
requirements and recovery costs (Syed et al., 2006). In addition,
physical methods are less costly and are easy to perform (Vaezi
et al., 2011).
The stripping process is based on Henry’s law (Farasat et al.,
2013; Li and Mather, 1997; Sagebiel et al., 1992). In this law at any
temperature, the quantity of soluble gas, which is dissolved in a
liquid, is directly related to the amount of the particular gas in the
surrounding atmosphere. The employed systems for stripping
processes, like towers, require large working volume. Therefore,
designing a system for H2S removal from crude oil that is able to
overcome the problems has significant benefits for industries. In
addition, enhancing the stripping efficiency by means of alternative
solutions with low energy consumption is still an interesting sub-
ject for researchers. In the recent years, it has been widely recog-
nized that the concept of microscale devices for bringing two
phases into a more efficient contact, covers many industrial pro-
cesses such as extraction (Inoue et al., 2013; Makarshin et al., 2015;
Su et al., 2010b; Zhao et al., 2007; Zhao et al., 2010), multiphase
reactive systems (Dessimoz et al., 2008; Kuhn and Jensen, 2012),
absorption (Behroozsarand and Pour, 2014; Heo et al., 2013; Zhu
et al., 2014), etc.
Microchannels is employed to enhance mass transfer perfor-
mance of any process with some unique benefits such as easy scale-
up, improvement of the safety and chemical product quality,
reduction of the diffusion length between fluids, enhancement of
the interfacial area of fluid and reduction of the working volumes
(Aoki and Mae, 2006; Cantu-Perez et al., 2010; Kanaris and Mouza,
2011; Singh et al., 2014).
Microchannels are well known by their high surfa-
cetovolume ratio (Commenge and Falk, 2011) and can induce
the high gasliquid mass transfer rate compared with other tech-
nologies. When a fluid flows in microfluidic systems, environ-
ment surface forces are main, but gravity is the major driving force
for liquid flow in conventional separation processes (Kenig et al.,
2013; Lam et al., 2013). The main challenge in a microchannel is
mixing, where more than one fluid come together. In addition,
mixing is a basic unit operation of chemical reactions and can
extremely affect the quality of final products in various industrial
processes. Many researchers confirmed that the twophase mass
transfer may be intensified in microscale devices (Su et al., 2010a;
Mock, 2010; Constantinou et al., 2014; Cypes and Engstrom, 2004;
Sen et al., 2014).
Su et al., (2010a) characterized mass transfer of H2S absorption
from gaseous mixture in a Tjunction microchannel. They
compared the mass transfer performance in various gaseliquid
contactors with Tjunction microchannel. The results showed that
the Tjunction microchannel could provide at least one or two
orders higher gas side volumetric mass transfer coefficient
compared with the other contactors.
The extraction and stripping experiments in a Tjunction
serpentine microchannel were investigated by Sen et al. (Sen et al.,
2014). They studied the effects of residence time and flow rate ratio
on overall volumetric mass transfer coefficients. They revealed that
the overall volumetric mass transfer coefficient of stripping was
higher than extraction. In another study, Cypes and Engstrom
(Cypes and Engstrom, 2004) analyzed toluene stripping process
and compared the removal efficiency of microfabricated stripping
column with a conventional packed tower. They found that the
value of mass transfer coefficients are higher in the micro-
contactor compared with examined packed beds.
Chasanis et al. (Chasanis et al., 2011) designed a micro-
contactor for the purpose of toluene stripping. They showed that
the overall mass transfer coefficients are 1e2 times higher than
those of a conventional packed tower. Constantinou et al.
(Constantinou et al., 2014) used a microfabricated stripper for
stripping of acetone from a water solution. Their results indicated
that the separation efficiency was increased by increase in the gas/
oil flow rate ratio.
On the other hand, some methods proposed in literature for
determination of influence of various parameters in a process. In
the conventional methods, experiments were carried out by vary-
ing the studied parameters and keeping the others constant. This
should be repeated for all the major parameters, resulting in an
unreliable number of experiments. In order to optimize the effec-
tive parameters with the minimum number of experiments, the
application of experimental design methodologies can be useful.
One of the experimental design techniques that are usually used for
process analysis and modeling is RSM (Khataee et al., 2010). RSM is
a useful method for studying the effect of a number of parameters
influencing the responses by changes them together and carrying
out a limited number of experiments (Khosravi et al., 2012). In this
technique, the main objective is to optimize the response surface
that influenced by different process parameters. RSM also quan-
tifies the relationship between the input parameters and the
response surfaces (Kwak, 2005). The design procedure for RSM is as
follows (Gunaraj and Murugan, 1999):
(i) Accomplish a set of experiments for satisfactory and well
measurement of the response of interest; (ii) Expand a mathe-
matical model of the second-order response surface with the finest
fit; (iii) Distinguish the optimal set of experimental parameters; (iv)
Demonstrate the effects of process parameters on responses
through two and three-dimensional (3D) plots.
It is possible to approximate linear, interaction and quadratic
effects of the parameters and a prediction models for the responses,
using RSM. In this way, find improved or optimal process settings in
an efficient use of resources could be achieved by applying RSM.
The experimental data required are dependent on the chosen type
of designs: central composite or BoxeBehnken designs (Box and
Hunter, 1957, 1961; Khataee, 2009). These methods are different
in the number of required runs and in the combinations of the
levels that apply in the experiments. The central composite design
supply approximately as much information as a multilevel factorial,
requires much fewer runs of experiments than a full factorial and
has been shown to be sufficient to describe the process responses
(Khataee et al., 2010; Cilliers et al., 1992; Obeng et al., 2005). The
Central composite design is a helpful design that is perfect for
sequential experimentation and allows for test lack of fit whereas
not concerning an uncommonly large number of design points
(Montgomery et al., 1984). The CCD lets well estimation of the first
and second order coefficients. Because of Box-Behnken design
regularly has fewer design points; it can be less relevant to do than
central composite designs with the same number of factors. How-
ever, because of they do not have an embedded factorial design;
they are not suitable for consecutive experiments. CCD usually has
axial points out of the “cube”. These points may not be in the dis-
trict of concern, or may be impossible to carry out because they are
outside of safe operating limits. Box-Behnken design do not has
axial points; therefore, you can be sure that all design points are
inside your safe operating zone. Box-Behnken designs also verify
that all factors are not set at their high levels simultaneously
(minitab). The CCD is a capable design for fitting the second order
model (Montgomery et al., 1984) and CCD was used to model the
RSM in this design. The preceding is the generally used experi-
mental design for fitting a second-order response surface
(Montgomery et al., 1984). CCD is the most widely used and
accepted experimental design for second-order models
(Angelopoulos et al., 2009).
By referring to above mentioned study in the literature, it can be
interesting to employ microscale strippers for enhancing the
mass transfer rates of H2S removal under low operational
 M.H. Almasvandi et al. / Journal of Natural Gas Science and Engineering 34 (2016) 499e508
temperatures and less amount of sweet gas consumption. However,
as far as we know, a study concerning with the use of the micro-
channels on removal of hydrogen sulfide from crude oil can be quite
novel. In the present study, cold stripping of H2S from crude oil in a
T jointed microchannel was investigated. For this purpose, urban
natural gas was used as sweetening gas. The novelty of this work is
the reduction of the consumption of the sweetening gas and car-
rying out the process under lower operational temperature by
employing the microscale contactor. The Tjunction micromixer
was connected to a microtube and a separator in the cold strip-
ping experiments. The effects of various operational conditions
including: temperature of crude oil (T), oil flow rate (QOil) and gas
flow rate (QGas) on the efficiency and S.E.C were investigated. The
results have been compared with other equipments. The Central
Composite Design (CCD) and Response Surface Methodology (RSM)
have been applied as statistical methods to model and optimize the
removal of H2S from crude oil based on the some effective pa-
rameters. Furthermore, the influences of interactions between the
parameters on the responses have been identified.
2. Materials and methods
2.1. Materials and chemicals
In this study, all employed chemicals were provided from Merck
Company, Germany. The crude oil was supplied from “NaftShahr”
field located in the west of Iran. The properties of the crude oil are
listed in Table 1. The specifications of the employed crude oil were
measured by the Iranian West Oil and Gas Operating Companies
according to relevant test methods. The stripping gas used in this
work was urban natural gas and its properties are listed in Table 2.
2.2. Experimental setup
A flow diagram of the employed experimental apparatus in this
work is shown in Fig. 1. The main part of the experimental setup
was Tshaped microchannel built from Plexiglas and a glass
microtube with an internal diameter and length of 900 mm and
500 mm, respectively. Sour crude oil was supplied from a tank and a
dosing peristaltic pump (QIS DSP 100) adjusted its flow rate. In
order to adjust the temperature of crude oil, the inlet crude oil was
pumped from a pipe, which was immersed in a bath of water.
Natural gas was supplied from a cylinder. The flow rate of natural
gas was adjusted by needle valves. It measured by a flowmeter,
whereas a pressure gauge measured the pressure. A simple phase
separator was placed at the end of the microchannel to separate the
mixture of crude oil and natural gas. The separator was a cylinder
with an inner diameter of 63 mm and height of 400 mm. The ex-
periments were conducted in the following parameter ranges: (a)
crude oil temperature (20e40
C), (b) crude oil flow rate
(50e120 mL/min) and (c) natural gas flow rate (200e1200 mL/
min). The temperature of natural gas was kept constant at 28
C
during all the experiments.
Table 1
Specifications of the employed crude oil.
Properties Unit Result
Specific gravity at 15.56/15.56
C e 0.8134
API e 42.46
Sulfur content wt% 0.52
H2S mg/L 203
501
Table 2
Specifications of the employed natural gas.
Component Value Unit
Methane 94.41 mol %
Ethane 5.13 mol %
Propane 0.23 mol %
Butanes 0.07 mol %
Pentanes and Heavier 0.02 mol %
Nitrogen and other 0.14 mol %
Hydrogen sulfide 1 ppm
Mercaptane 13 mg/Sm3
2.3. Experimental procedure
The experiments were carried out in a continuous mode. Before
each run, the tank was filled with H2S contaminated (sour) crude
oil. Then the natural gas was allowed to enter the Tshaped junc-
tion at a prescribed flow rate. When the gas phase pressure reached
to a steady state condition, the liquid phase was pumped from the
tank to the Tshaped junction at a certain flow rate through a water
bath. The water bath is employed to adjust the temperature of the
crude oil. During the process, H2S concentration in the crude oil
was measured at the outlet of the separator. The concentration of
H2S was determined by UOP163 standard test method. The UOP
163 test method outlines a potentiometric titration with alcoholic
silver nitrate solution that allows the hydrogen sulfide and
mercaptan sulfur in hydrocarbons to be determination
(International UOP Method, 2010).
In order to evaluate the overall performance of the process, the
effect of main parameters such as: the temperature of crude oil,
flow rates of both crude oil and natural gas were investigated on the
efficiency and S.E.C. Each one of the mentioned experiments was
repeated three times to ensure the accuracy of the obtained results.
There were three different mass transfer zones in this system,
including the crossflow Tjunction, the mixing microchannel and
the outlet mass transfer zone (separator). In the Tjunction mass
transfer zone, the crude oil and natural gas flows are continuous
phases. The T junction was used to mix gasliquid phases,
vigorously. The mixing channel, as the second mass transfer zone,
was employed in order to enhance the mass transfer rate and
provide enough required residence time for mass transfer. In this
mass transfer zone, the gasliquid twophase flow regimes
intensively depend on the hydrodynamic behavior of two phases at
the Tjunction zone. The twophase mixture should be separated
in the phase separator at the outlet of the microchannel. Since the
inner diameter of the separator cylinder was larger than the
diameter of microchannel, the efficiency of separation was high and
the interfacial area of two phases in the separator could be negli-
gible in comparison with Tjunction and the mixing channel. It
was assumed that the rate of mass transfer at the outlet of micro-
channel was negligible in this study.
2.4. Definitions of relevant parameters
The H2S removal efficiency based on the liquid phase mass
transfer in the T jointed microchannel could be expressed as
follows:
CH2 S;in  CH2 S;out
Efficiencyð%Þ ¼  100 (1)
Test method CH2 S;in
ASTM D4052
ASTM D4052 where CH2 S;in and CH2 S;out are the concentration of H2S in crude oil
ASTM D2622 (mg/L) at the inlet and outlet, respectively.
UOP163
S.E.C is the power consumption caused by pressure drop per
502 M.H. Almasvandi et al. / Journal of Natural Gas Science and Engineering 34 (2016) 499e508

Fig. 1. (a) The flow diagram of the employed experimental apparatus. (b) Real photograph of experimental setup.

unit the weight of (milligram) H2S removal. where DP is the pressure drop (Pa). QOil and QGas are crude oil and
The pressure drop can be related to the S.E.C for different con- natural gas flow rates (mL/min), respectively.
ditions by Eq. (2): In this relation, the numerator is a criterion of the consumed

 energy and the denominator is the total amount of H2S removal in
J ðQ Oil þ Q Gas Þ  DP milligrams.
S:E:C ¼   (2)
mg 1000  Q Oil  CH2 S;in  CH2 S;out
 M.H. Almasvandi et al. / Journal of Natural Gas Science and Engineering 34 (2016) 499e508
3. Results and discussion
3.1. Effect of operational conditions on the removal efficiency and
specific energy consumption
The main issue micromixers are providing good mixing and
increasing interfacial surface between phase. These unique ad-
vantages may result the increased mass transfer between two-
phases, higher removal efficiency and removal rate. In this study,
the effects of some operational variables such as: temperature of
crude oil, crude oil and natural gas flow rates are investigated on
the efficiency and S.E.C. The effect of each parameter is evaluated
while the other parameters are at constant values.
3.1.1. Effect of crude oil temperature
In order to investigate the effect of the temperature of crude oil
on efficiency and S.E.C, the temperature was being change in the
range of 20e40
C. During the experiments, the flow rates of oil and
gas were kept constant at 85 and 700 mL/min, respectively. It could
be found from Fig. 2 that by increasing the temperature of crude oil,
the efficiency will increase while a slight reduction was observed
for S.E.C. By increasing the temperature from 20 to 40
C, the effi-
ciency was increased 9.5%. Increasing the temperature will enhance
the molecular diffusion coefficient of H2S in both liquid and gas
films and also may promote the surface tension of liquid phase and
the liquidegas distribution ratio of H2S. The increased temperature
may effect on desorption of H2S from crude oil because of the
enhancement of the H2S dissolution in oil. On the other hand, the
viscosity and pressure drop of the oil will be lower at the higher
temperature and according to Eq. (2); the S.E.C will be decreased
due to lower pressure drop. This behavior is illustrated in Fig. 2.
3.1.2. Effect of oil flow rate
The effect of oil flow rate on efficiency and S.E.C was investi-
gated by changing the flow rate in the range of 50e120 mL/min.
During these experiments, the crude oil temperature and natural
gas flow rate were kept constant at 25
C and 700 mL/min,
respectively. As shown in Fig. 3, by increasing the oil flow rate in the
employed range, the efficiency is slightly decreased. At the constant
flow rate of the gas, by increasing the flow rate of oil, the volumetric
Fig. 2. Effect of crude oil temperature on the efficiency and S.E.C.
503
gas to oil ratio will be decreased and it may cause phase dispersion
and consequent decrease in gaseliquid interfacial surface. This
caused a decrease in mass transfer rate and efficiency. Moreover, as
illustrated in Fig. 3, a slight reduced trend is happened for S.E.C by
increasing the flow rate of oil. This behavior is due to enhancement
of the H2S removal. On other hand, increasing the flow rate of oil
has not a significant effect on pressure drop and so the energy
consumption per each milligram of removed H2S will be decreased.
3.1.3. Effect of gas flow rate
In order to investigate the effect of flow rate of the natural gas on
efficiency and S.E.C, the flow rate of gas was changed in the range of
200e1200 mL/min. The temperature and the flow rate of the crude
oil were kept constant at 25
C and 70 mL/min, respectively. As
illustrated in Fig. 4, increase in flow rate of the gas leads to a higher
efficiency. It could be easily seen that the efficiency is higher at
lower flow rates and then it tends to an asymptote. Despite
reducing the residence time by increasing the natural gas flow rate,
the effect of increasing surface contact and mixing is more than
residence time and caused to the efficiency increasing.
It is well accepted that, at the constant temperature and flow
rate of oil, the efficiency will be increased because of an increase in
the volumetric gas to oil ratio. This increased behavior may lead to
enhancing the dispersion and mixing. Increasing the concentration
gradient causes the enhancement of the mass transfer rate. This
observation is in agreement with the previous reports (Abdel-Aal
et al., 2003).
According to Fig. 4, S.E.C is increased intensively by increasing
the flow rate of the natural gas at constant temperature and crude
oil flow rate. This behavior is due to the established higher pressure
drop and energy consumption due to more flow of fluid trough the
microchannel with increase in gas flow rate.
3.2. Comparison of the employed microchannel with the other types
of strippers
Table 3 illustrates that for H2S removal from a specified amount
of crude oil, microchannels consume less gas compared with other
Fig. 3. Effect of flow rate of crude oil on the efficiency and S.E.C.
504 M.H. Almasvandi et al. / Journal of Natural Gas Science and Engineering 34 (2016) 499e508

were coded as A, B and C, respectively (Table 4). The independent

factors were varied over five levels (a, 1, 0, þ1, þa) and the
ranges were determined based on preliminary studies.
The numbers of experiments with five levels for each factor
were totally 20, which were obtained by software package.
Quadratic model (Eq. (3)) was used as appropriate model.

X
k X
k XX
k
Y ¼ b0 þ bj Xj þ bjj X2j þ bij Xi Xj þ ei (3)
j¼1 j¼1 i ji

where b0 is a constant coefficient; bj, bjj, and bij are the interaction
coefficients of linear, quadratic and second order terms, respec-
tively; Y is the response; Xi and Xj are the variables; k is the number
of studied factors; and ei is the error. The pvalue for analysis of
variance (ANOVA) tables associated with the 95% confidence level
was used to evaluate the variables and the interactions between
them.
The operational conditions and experimental results are listed
in Table 5. Using these experiments, the values of efficiency were in
the range of 65.7%e77.8%. As shown in this table, the maximum
efficiency is 77.8% and minimum S.E.C is 0.98 J/mg.

Fig. 4. Effect of natural gas flow rate on the efficiency and S.E.C.
3.4. Regression model equation and analysis of variance (ANOVA)

equipment. In this table, the efficiency and volumetric gas to oil Tables 6 and 7, show the analysis of variance (ANOVA) of
ratio of microchannel with valve tray tower is compared. The regression parameters of the predicted response surface quadratic
calculated values of the efficiency in microchannel are higher than models for the efficiency and S.E.C, respectively. A ratio of re-
that of the valve tray tower. It should be considered that the sponses (maximum to minimum) greater than 10 usually indicates
volumetric gas to oil ratio of the tower is about 3 fold of the a transformation is required. For ratios, less than 3 the power
microchannel. Appropriate mixing and enhancement of the inter- transforms have little effect. For efficiency model: response range is
facial surface are the main reasons of priority of microchannel from 65.7 to 77.8. Ratio of maximum to minimum is 1.18. After
compared with other one. These improvements are also, led to a trying different response transforms, inverse transform shows
significant increase in mass transfer rate between two phases and it more accuracy and causes decreasing the LOF, it should be notice
provides higher efficiency with less amounts of gas consumption. that this changes results in agreeable reducing of R2 (ABOUT 0.2%
Another paramount result for the microchannels is the lower compared to non-transformation). The F-values are determined by
operational temperature of the gas phase compared with the other the ratio of the mean square of the parameter to the mean square of
conventional stripping towers. In other similar studies, the required the error term, while the P-values are obtained from the F distri-
temperature of the gas phase for an efficient stripping is higher bution (Myer and Montgomery, 2002). As the experimental design
than 46
C (Vaezi et al., 2011). However, in the studied micro- was replicated at the center points, the variability of the experi-
channel, by reducing the operational required temperature, the ments error (pure error) could be estimated from the variability of
costs of the energy is reduced, which is one of advantages of the the replicated runs. The pure error is used to examine the signifi-
proposed system. cance of the residual variance, i.e., all the remaining variability that
could not be accounted in the model and, thus, determined the
overall lack of fit of the model. As Table 6 reveals, both the model F-
3.3. Experimental design and analysis value of 65.364 and a low probability value (Prob > F < 0.0001)
indicated that the model was significant for efficiency. The
The statistical design and modeling of this study were per-
formed using Minitab 17 software (Minitab-17-Software, 2016). The
Table 4
response surface methodology (RSM) was employed to investigate
Experimental range and levels of independent process variables employed in the
the model statistically. The Central Composite Design (CCD) is one process of the H2S removal from crude oil.
of the most widely used to experimental design for fitting a second
Independent variable Code a 1 0 þ1 þa
order response surface (Montgomery et al., 1984). This method was
employed to model the experimental data. The independent factors T (⁰C) A 20 24.05 30 35.95 40
used in this experimental study were the temperature of the crude QOil (mL/min) B 50 64.19 85 105.81 120
QGas (mL/min) C 200 402.70 700 997.30 1200
oil (T), flow rates of the crude oil (QOil) and natural gas (QGas) which

Table 3
Comparison of the efficiency and volumetric gas to oil ratio of two equipments.

Equipment Crude oil specific Crude oil Sweetening gas Pressure drop H2S removal Volumetric gas to oil Reference
gravity () temperature (⁰C) temperature (⁰C) (psig) efficiency (%) ratio ()

Microchannel 0.8134 24 28 5.7 72.4 15.54 This work

Valve tray 0.8225 24.5 46.1 2 68.18 46.82 (Vaezi et al.,
tower 2011)
 M.H. Almasvandi et al. / Journal of Natural Gas Science and Engineering 34 (2016) 499e508 505

Table 5
Results of the central composite design of the experimental data of the H2S removal from crude oil.

Run Process variable Responses

A: Temperature ⁰C B: QOil mL/min C: QGas mL/min Efficiency % S.E.C J/mg

1 30.00 85.00 700.00 71.90 2.70

2 35.95 105.81 402.70 70.00 1.47
3 30.00 85.00 700.00 72.40 2.64
4 40.00 85.00 700.00 75.60 2.28
5 30.00 85.00 200.00 67.20 0.98
6 30.00 50.00 700.00 75.40 3.71
7 30.00 85.00 700.00 73.70 2.63
8 24.05 105.81 997.30 71.20 3.23
9 30.00 85.00 700.00 72.80 2.67
10 30.00 85.00 700.00 72.80 2.71
11 20.00 85.00 700.00 65.70 2.48
12 30.00 120.00 700.00 72.00 2.41
13 35.95 64.19 997.30 77.80 4.18
14 30.00 85.00 700.00 73.20 2.69
15 35.95 105.81 997.30 75.90 2.98
16 24.05 64.19 997.30 72.40 4.41
17 24.05 64.19 402.70 69.40 1.95
18 30.00 85.00 1200.00 76.40 4.43
19 35.95 64.19 402.70 72.40 1.94
20 24.05 105.81 402.70 66.00 1.48

Table 6
Analysis of variance and adequacy of the quadratic model for efficiency of H2S removal from crude oil.

Source Sum of squares Degree of freedom Mean square FValue Prob > F (P-Value)

Model 7.74E-06 5 1.55E-06 65.364 <0.0001 significant

ATemperature 3.23E-06 1 3.23E-06 136.4537 <0.0001
BOil flow rate 5.84E-07 1 5.84E-07 24.6513 0.0002
CGas flow rate 3.37E-06 1 3.37E-06 142.3954 <0.0001
A2 4.63E-07 1 4.63E-07 19.57036 0.0006
C2 1.28E-07 1 1.28E-07 5.419401 0.0354
Residual 3.32E-07 14 2.37E-08
Lack of Fit 2.62E-07 9 2.92E-08 2.110547 0.2126 not significant
Pure Error 6.91E-08 5 1.38E-08

R2 ¼ 0.9589, R2adj ¼ 0.9442, Adeq Precision ¼ 28.239.

Table 7
Analysis of variance and adequacy of the quadratic model for specific energy consumption of H2S from crude oil.

Source Sum of squares Degree of freedom Mean square FValue Prob > F (P-Value)

Model 1.626082 8 0.20326 704.2378 <0.0001 significant

ATemperature 0.004446 1 0.004446 15.40429 0.0024
BOil flow rate 0.190434 1 0.190434 659.799 <0.0001
CGas flow rate 1.367721 1 1.367721 4738.755 <0.0001
AC 0.001675 1 0.001675 5.803596 0.0347
BC 0.00841 1 0.00841 29.13715 0.0002
A2 0.015151 1 0.015151 52.49462 <0.0001
B2 0.020355 1 0.020355 70.52402 <0.0001
C2 0.013352 1 0.013352 46.2591 <0.0001
Residual 0.003175 11 0.000289
Lack of Fit 0.002677 6 0.000446 4.48096 0.0606 not significant
Pure Error 0.000498 5 9.96E-05

R2 ¼ 0.9981, R2adj ¼ 0.9966, Adeq Precision ¼ 95.8644.

“Adequate Precision” ratio of the model was 28.239 (Adequate
Precision>4), which is an adequate signal for the model (Olmez, €
2009). The lack of fit F-statistic was statistically significant as the
P-values were less than 0.05. A significant lack of fit suggests that
there may be some systematic variation unaccounted for the
model. This may happen due to the exact duplicate values of the
independent parameters in the model that provide an approximate
of pure error. The quality of the fit of the polynomial model is
expressed by the determination coefficient R2 and adjusted R2
(R2adj). In order to test the overall fit of the model, the R2 and R2adj
were evaluated. The value of R2, i.e. 0.9589 (Table 6), denotes that
the sample variation of 95.89% for efficiency is attributed to the
regression model and only about 0.5% of the total variability is not
explained by the model. The value of R2adj was 0.9442 (Table 6),
which deviates 0.0147% from the value of R2, indicates that the
model is highly significant and there is small chance for the in-
clusion of any insignificant terms in the model. As Table 6 reveals, A,
B, C, A2 and C2 are significant terms in efficiency model. Insignifi-
cant model terms, which have inconsiderable effects, such as AB,
AC, B2 and BC were excluded because they have P-values equal to
0.67,0.37, 0.15 and 0.13, respectively. The values of P-value less than
0.05 indicate that model terms are significant, while values greater
506 M.H. Almasvandi et al. / Journal of Natural Gas Science and Engineering 34 (2016) 499e508

than 0.1 indicate that the model terms are not significant (Ko € rbahti
and Tanyolaç, 2008). Based on the obtained results, the RSM con-
structed in this study for predicting efficiency was considered
reasonable.
For SEC: response ranges from 0.98 to 4.43. Ratio of maximum to
minimum is 4.51. After trying different response transforms, square
root transforms shows better results and causes reducing LOF, it
should be notice that this change results in decreasing R2 that it is
not very significant (compared to non-response transform). In this
case AB is “not significant” term and removed because P-value is
equal to 0.7724.
As Table 7 shows, both the model F-value of 704.2378 as well as
a low probability value (Prob > F < 0.0001) indicate that the model
was significant for S.E.C. The “Adequate Precision” ratio of the
model was 95.8644. The value of correlation coefficient,
R2 ¼ 0.9981, was obtained in the present study for S.E.C for H2S
removal from crude oil. As it is seen in Table 7 for S.E.C model, A, B,
C, AC, BC, A2, B2 and C2 are significant terms. Insignificant model
term (AB) removed, because it has negligible effect and its P-value
was equal to 0.7724. Based on the obtained results, the final RSM for
predicting S.E.C was considered reasonable.
In terms of actual factors, the empirical relationships of the ef-
ficiency and S.E.C based on the employed process variables are
expressed by the following second order polynomial equations.

1
¼ 0:0207  3:85E  4T þ 9:94E  6Q Oil  3:2E
Efficiency
 6Q Gas þ 5:05E  6T2 þ 1:06E  9Q 2Gas
(4)

SqrtðS:E:CÞ ¼ 0:66 þ 0:06T  0:02Q Oil þ 2:24E  3Q Gas

 8:18E  6  T  Q Gas  25:24E  6  Q Oil
 Q Gas  9:17E  4T2 þ 8:68E  5 Q 2Oil  3:44E
 7Q 2Gas
(5)
As shown in Fig. 5, the predicted values of the efficiency and
S.E.C obtained from the models are in good agreement with the
experimental data (Ko € rbahti and Tanyolaç, 2008).
The 3D surface response of the quadratic model is utilized to
evaluate the interactive relationships between independent vari-
ables and responses (H2S removal efficiency and S.E.C). Effects of
the two parameters were evaluated while one of the parameters
was at constant value. As shown in Fig. 6 (a), the results illustrate
that efficiency increases with the increase of the crude oil tem-
perature and gas flow rate in the employed range. As Fig. 6 (b)
reveals, by increasing the flow rate of oil at constant gas flow rate,
the volumetric gas to oil ratio will be decreased and it may cause
phase dispersion, and hence the efficiency is slightly decreased. The
reduction was found more at lower gas flow rates due to the
reduction of the volumetric gas to oil ratio.
Fig. 7 (a) shows the effect of crude oil temperature and gas flow
rate on S.E.C at constant gas flow rate. It can be seen from the figure
that in low range of gas flow rates, the increase of the temperature
has limit effect on S.E.C. While S.E.C decreased by the increase of the
temperature in high value of gas flow rates.
According to Fig. 7 (b), by the increase of the gas flow rate, S.E.C
is increased. On the other hand, the increase of the oil flow rate
leads to lower S.E.C. This behavior is more noticeable at high values
of gas flow rate.
The obtained results from RSM in this section are in agreement
with the results that is shown in Section 3.1.
Fig. 5. Predicted versus actual values plot for (a) efficiency and (b) S.E.C.
3.5. Determination and experimental validation of the optimal
condition
Optimization of a process has paramount significance to find the
best response in the range of the employed variables. In this study,
as is demonstrated above, increasing temperature and flow rate of
gas, increases the H2S removal efficiency. However, it has negative
effect on S.E.C. Therefore, finding the optimum conditions, with
higher efficiency along with minimum amounts of S.E.C can be
quite important.
According to the software optimization step, the desired aim for
each operational condition (temperature of crude oil, flow rates of
crude oil and natural gas) were chosen “within the range”, while
the responses (efficiency and S.E.C) were defined as “maximum”
and “minimum”, respectively. The optimum working condition
were found: the temperature of crude oil equal to 40
C, flow rate of
crude oil equal to 120 mL/min and flow rate of natural gas equal to
200 mL/min. The respective responses are listed in Table 8. An
additional experiment was performed to confirm the optimum
 M.H. Almasvandi et al. / Journal of Natural Gas Science and Engineering 34 (2016) 499e508 507

Fig. 7. Response surface for S.E.C as a function of (a) Crude oil temperature and Natural
Fig. 6. Response surface for efficiency as a function of (a) Crude oil temperature and
gas flow rate (Oil flow rate 85 mL/min) and oil and gas flow rates (Crude oil temper-
Natural gas flow rate (Oil flow rate 85 mL/min) and (b) oil and gas flow rates (Crude oil
ature 30
C).
temperature 30
C).

Table 8
result. As it is represented in Table 8, experimental values were A comparison between experimental and predicted responses at optimum
reasonably close to the predicted values. This result confirms the condition.
predictability of the model in the employed experimental
Parameter Goal Predicted responses Experimental result
condition.
Efficiency (%) Maximum 71.46 70.93
S.E.C (J/mg) Minimum 0.97 0.96
4. Conclusions

The cold stripping in a microchannel system can be employed to
effectively decrease the hydrogen sulfide content of sour crude oil.
Microchannel enhances the mass transfer by providing a good gas-
liquid multiphase flow and appropriate interface conditions. H2S
removal efficiency of 77.8% was successfully obtained in lower
amounts of used gas (about one-third) and low gas temperature
(about 18
C less) compared with other equipments. The obtained
results may cause to extend this application to other stripping
systems that still suffer low efficiency. The results showed that the
efficiency was increased with increasing the temperature of crude
oil at the constant flow rates of both crude oil and natural gas.
However, crude oil temperature have not a considerable effect on
S.E.C. Increasing the flow rate of crude oil caused a slight decrease
in the efficiency and S.E.C. Increasing the natural gas flow rate, lead
to enhancement of the efficiency and S.E.C. The H2S removal effi-
ciency was found in the range of 65.7%e77.8%, which show high
H2S removal efficiency for this stripper system. In the present
study, optimization of H2S removal by the cold stripping in
microchannel was investigated. The optimization of stripping
process has been carried out, using RSM with CCD, to find the
influence of operating variables including; temperature of crude oil,
flow rates of crude oil and gas. The optimization procedure suggests
that optimized operational conditions are; crude oil
temperature ¼ 40
C; crude oil flow rate ¼ 120 mL/min; and natural
gas flow rate ¼ 200 mL/min. Under this condition, the efficiency
value was 70.93% and S.E.C was 0.96 J/mg. This study shows the
paramount ability of the microchannel for H2S removal from crude
oil by cold stripping process, by the use of about one-third less
amount of sweetening gas and about 18
C lower gas temperature,
compared with the valve tray tower.
Acknowledgments
Authors would like to acknowledge the support from Iranian
west oil and gas operating companies for providing the crude oil for
this work.
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