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Energy Sources, Part A: Recovery,

Utilization, and Environmental Effects
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Soapnut Extract as a Natural Surfactant

for Enhanced Oil Recovery
a a a a
A. B. Chhetri , K. C. Watts , M. S. Rahman & M. R. Islam
a
Faculty of Engineering , Dalhousie University , Halifax, Canada
Published online: 20 Aug 2009.

To cite this article: A. B. Chhetri , K. C. Watts , M. S. Rahman & M. R. Islam (2009) Soapnut Extract
as a Natural Surfactant for Enhanced Oil Recovery, Energy Sources, Part A: Recovery, Utilization, and
Environmental Effects, 31:20, 1893-1903, DOI: 10.1080/15567030802462622

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 Energy Sources, Part A, 31:1893–1903, 2009
Copyright © Taylor & Francis Group, LLC
ISSN: 1556-7036 print/1556-7230 online
DOI: 10.1080/15567030802462622

Soapnut Extract as a Natural Surfactant for

Enhanced Oil Recovery

A. B. CHHETRI,1 K. C. WATTS,1 M. S. RAHMAN,1 and

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M. R. ISLAM1
1
Faculty of Engineering, Dalhousie University, Halifax, Canada

Abstract Primary and secondary recovery of oil from oil reservoirs contributes
approximately 30% of the total oil in place in most oil reservoirs. Since the current
economic development is heavily dependent on fossil fuel, increasing the amount of
oil recovery is given considerable attention. One of the most widely used methods for
enhanced oil recovery is the application of various types of surfactants in order to
reduce the oil-water interfacial tension. However, the surfactants being used today
are usually synthetic chemicals and polymers, which are expensive, linked to fossil
fuels, and detrimental to the environment. In thisarticle, a natural surfactant prepared
from the pericarp shell of fruit (Sapindus mukurossi) collected from a naturally
available tree was used to reduce oil-water interfacial tension. The effect of surfactant
concentration with 1%, 2%, 4%, 8%, and 12% was investigated. The effect of heat
on interfacial tension was also studied. The experimental results showed that extract
has a great potential to be used as a surfactant for enhanced oil recovery schemes.

Keywords enhanced oil recovery, interfacial tension, natural and synthetic surfactant

1. Introduction
Fossil fuels are considered to be the major driver of the economic growth of modern
society. With the increase in population and living standard of people, the demand of
fossil fuels is constantly increasing. However, only approximately 30% of the total oil
in place can be recovered naturally leaving approximately 70% oil in the reservoir itself
(Curbelo et al., 2007). The remaining oil is trapped in reservoir pores due to various
surface and interfacial forces. This trapped oil can be recovered by reducing capillary
forces, surface and interfacial tension (IFT), and altering the wettability that prevents oil
from flowing within the pores of reservoir rocks and to the wellbore. Conventional oil
production is characterized by stagnant oil production and unimpressive recovery. Hence,
considerable attention has been paid to enhanced oil recovery (EOR) techniques in order
to recover more oil from existing oil fields. EOR is any process that involves injection of
fluids into the depleting reservoir to supplement the natural energy present and to create
favorable condition for maximum oil recovery (Ayirala, 2002).
Various EOR techniques are being employed currently in the oil industry. The thermal
recovery includes steam injection, combustion, hot water injection, and electromagnetic
heating. The chemical method involves the application of chemical compounds, such as

Address correspondence to M. Rafiqul Islam, Department of Civil and Resources Engineering,

Dalhousie University, Sexton Campus, Rm D510, 1360 Barrington St., Halifax, NS B3J-1Z1,
Canada. E-mail: rafiqul.islam@dal.ca

1893
 1894 A. B. Chhetri et al.

polymers, alkaline flooding, and surfactant enhanced recovery. The gas injection EOR
method uses miscible or immiscible injection of various gases, such as CO2 , hydrocarbon
gases, nitrogen, and others. There are also other techniques, such as microbial injection,
vibration technique, etc., that have not received widespread applications despite some
successful pilot projects.
This article investigates the possibility of using alternative natural surfactants from
plant sources for the enhanced oil recovery. The use of ground fruit pericarp shell has been
investigated as a natural surfactant in order to reduce the oil water IFT and increase the oil
mobility. Fruit pericarps have naturally available saponins, which have been traditionally
used for various applications including bathing and fabric washing (Oommachan, 1977).
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2. Use of Surfactants in EOR

The alkaline solution is one of the major surfactants that are used in the enhanced oil
recovery in the petroleum industry. Crude oils naturally contain a certain amount of
organic acid (Liu et al., 2007). When acidic oil comes in contact with alkaline solution,
surface active agents are produced in situ in the oil-water interface resulting in the
reduction in IFT (Islam and Farouq Ali, 1989). This phenomenon helps to increase the
oil mobility. The IFT between acidic crude oil and alkaline solution is affected by its
pH, type of organic acids in the crude oil, and the concentration of surfactants among
others (Elkamel et al., 2002).
Even though the world is facing an energy crisis and thereby looking for innovative
methods for enhanced oil recovery to produce more oil to meet the current and future
energy needs, the EOR schemes have declined recently in the U.S. and the rest of the
world. The major challenge the EOR schemes are facing today are to produce oil under
attractive economic and environmental conditions (Islam, 1999; Khan and Islam, 2007).
Figure 1 shows the total EOR production in the U.S. between 1982 and 2006. The EOR
production increased from 1982 but started to decrease significantly from 1998. Figure 2
shows the decline of U.S. EOR production attributed to chemical flooding at the same
period. Despite chemical flooding being one of the widely used EOR techniques, its
decline started sharply in the U.S. and in other countries after 1988.
Major reasons for the decline of EOR by chemical flooding are the rising price of sur-
factants and their environmental impacts in the long-term. The alkalis mostly used during
alkaline flooding are sodium hydroxide (NaOH), sodium orthosilicate .Na4 SiO4 /, sodium
metasilicate .Na2 SiO3 /, sodium carbonate .Na2 CO3 /, ammonium hydroxide (NH4 OH),
and ammonium carbonate .NH4 /2 CO3 (Burk, 1987; Taylor et al., 1996; Almalik et al.,
1997). It has been found that the costs of these chemicals have significantly increased
recently. Figure 3 shows their cost increment from 1998 to 2006.
The use of synthetic surfactants usually increase toxic load to the ecosystem
(Mandava, 1994). Moreover, unlike natural surfactants, synthetic surfactants including
polymers may not always be easily biodegradable. Haynes et al. (1976) reported that a
dose of 1.95 grams of sodium hydroxide can cause death in humans. According to the
EPA (1992), various types of alkali compounds have also significant adverse effects on
human health and are one of the major direct or indirect causes of air pollution. Inhalation
of dust, mist, or aerosol of sodium hydroxide and other alkalis may cause irritation of the
mucous membranes of the nose, throat, and respiratory tract (MSDS, 2006). Exposure
to the alkalis in solid or solution can cause skin and eye irritation, direct contact with
the solid or with concentrated solutions causes thermal and chemical burns leading to
deep-tissue injuries and also permanent damage to any tissue (ATSDR, 2006). The use of
 Natural Surfactant for Enhanced Oil Recovery 1895
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Figure 1. Total EOR production in the USA between 1982–2006 (Worldwide EOR Survey, 2007).

Figure 2. Total EOR production in the USA through Chemical Flooding (Moritis, 2004).
 1896 A. B. Chhetri et al.
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Figure 3. Price of common alkali chemicals (Mayer et al., 1983; Chemistry Store, 2005; ClearTech,
2006).

such compounds in underground reservoirs could have impacts on microbial diversity and
other long-term environmental consequences. Hence, there has been a growing interest
in developing surfactants from biological sources that are environment friendly and less
expensive compared to synthetic surfactants.
Saponins are naturally occurring chemical compounds that produce foam or lather in
water similar to soap. Saponins are the glycosides with their aglycones, which are related
to sterols. These sterols consists of tigogenin, gitogenin, digitogenin, and sarsasapogenin
and triterpines, which themselves consist of hedaragenin and oleanolic acid (Mandava,
1994). The saponification value was found to be 138.2 (Shetty, 1972). Huang et al. (2006)
isolated the Tirucallane-type saponins assay from Sapindus mukorossi in Taiwan from
NMR study (Figure 4). The sapogenin, which is obtained from Hedera helix as well as
from Sapindus saponnria L. and Sapindus mukorossi utilis, was hederagenin, C31 H50 O40 .
However, Mandava (1994) reported that the saponins isolated from Sapindus mukorossi
fruits were reported to be C52 H84 O21
2H2 O (2007).
Table 1 is the measure of the pH of a solution in water at different concentrations.
The pH was more or less similar with the concentration of the solution both for hot and
cold water extraction. This indicates that solution in water has weak acidic properties.
UNESCO (1981) reported that solution has a non-ionic or weak acidic property in water.
The characterization of soapnut including SEM micro-structure analysis is described in
detail by Chhetri et al. (2007).

3. Material and Methods

3.1. Preparation of Surfactant Solution

Soapnut fruit pericarp shell samples were collected from Nepal. The samples were
collected randomly from the stock. The fruit pericarps were dried in an oven at 50ıC
for 36 h. The dried pericarp shells were crushed to a fine powder, which was added to
deionized water. The mixture was continuously stirred, left for 24 h and the undissolved
 Natural Surfactant for Enhanced Oil Recovery 1897
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Figure 4. Tirucallane-type saponins assay (Huang et al., 2006).

matter was filtered out. The final filtrate was used for the experiments. The concentration
was measured in weight per unit volume basis (grams of powder per 100 ml of deionized
water). For preliminary tests, solutions of 0.5%, 1%, 2%, 4%, 8%, and 12% concentrations
were used (Figure 5). Similarly, hot water extracts of the same concentrations were also
prepared heating the deionized water at 50ıC for 15 min. It is found that the saponin
concentration of solution is not much different in cold extract and hot extract within the
range of 25ı C of room temperature and heated solution up to 50ı C. For all experimental
work, solutions were prepared with a mixing time of 24 h at room temperature (24ıC)
for cold extract and at 50ı C for hot extract. The strong acidic pH of solution could be
due to the hydrolysis of the constituent glycosides of saponins.

3.2. Oil Water IFT Measurement Using Du Nouy Ring Method

The value of IFT can be determined by different methods (Nouy, 1919). In this study,
IFT values were measured using the Du Nouy ring method. The ring method is based
on the fact that before any enlargement of a phase boundary area between liquid/air or
liquid/liquid can take place only after overcoming some resistance. This resistance is
proportional to existing surface and interfacial tension and the result can be directly read
in dynes/cm with an accuracy of 0.05 dynes/cm. The instrument was first checked using

Table 1
pH at different concentrations of solution

Concentration 0.5% 1% 2% 4% 8% 12%

pH (cold extract) 4.94 4.90 4.83 4.81 4.81 4.81

pH (hot extract) 4.66 4.61 4.58 4.56 4.54 4.58
 1898 A. B. Chhetri et al.
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Figure 5. Mixture samples.

distilled water at 18ı C and found that it shows the standard value of 72.9 dynes/cm.
The properties of crude oil are summarized in Table 2. In this experiment, the IFT was
measured at different concentrations of solutions. IFT was measured for 0.5%, 1%, 2%,
4%, 8%, and 12% concentrations of solution.

4. Results and Discussion

As has been in use as natural soap extracted from the saponin of its pericarp shells, it
is expected that can be effectively used as a natural surfactant for EOR application. The
use of ground pericarp shell as a surfactant in EOR was investigated by measuring the
interfacial tension between crude oil and water. Hot water and cold water extraction was
employed to extract the saponin. The average of three readings was recorded and plotted.
In Figure 6, it is observed that the IFT between crude oil and water reduces sig-
nificantly after the application of cold water extract. The IFT readings against different
concentrations were recorded at different times. It is found that the IFT reduced from 19
dynes/cm to 2.5 dynes/cm after the application of surfactant. The consecutive readings at

Table 2
Physical properties of the crude oil

Physical properties Value

Specific gravity 0.7 to 0.95

Vapor pressure >0.36 Kpa at 20ı C
Vapor density 3 to 5 (approx)
Freezing point 60ıC to 20ıC
Viscosity <15 centistokes at 20ıC
Solubility Insoluble
Co-efficient of water/oil distribution <1
Source: Rahman, 2007.
 Natural Surfactant for Enhanced Oil Recovery 1899
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Figure 6. IFT measurement for various concentrations of cold water extract.

increased concentration show that there is only small reduction in IFT compared to the
first reading. It was also observed that the IFT slightly increased after several hours and
remained at steady state value. Hot water extract was also used but showed very similar
results as that of cold water extract. Error bars were plotted and it was found that the
maximum standard deviation was 5.8%.
Figure 7 shows the variation of interfacial tension with time for different surfactant
concentrations. Before the application of surfactant, the initial IFT between oil and water
was 19 dynes/cm. When the surfactant was first applied, IFT reduced significantly. IFT
was measured at 1 h, 2 h, and 4 h intervals. It was observed that IFT first reduced and then
slightly increased (Figure 7). After an hour, the IFT seems to remain almost constant.
Even if there were slight changes, the non-digital equipment used in the experiment
might not have detected it due to lack of precision. Liu et al. (2007) reported that there

Figure 7. Variation of IFT at different concentration with time.

 1900 A. B. Chhetri et al.
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Figure 8. IFT measurement at different concentration for a heated solution.

was a significant reduction in IFT due to the use of Na2 CO3 and NaOH in the presence
of alkyl ether sulfate at surfactant concentration of 0.30% by weight. The IFT reduction
trend reported by Liu et al. (2007) is comparable with the IFT reduction by 2–3% of the
surfactant concentration (Figures 6 and 7).
The effect of heat on the IFT due to the surfactant was also investigated. The oil-
water and surfactant solution was heated to 50ıC and the IFT was measured. It was
found that the IFT reduction in heated solution was higher than in the solution without
heating. The IFT slightly increased after the first reading and remained almost constant
afterwards in both hot and cold water extracts (Figure 8).
From Figures 6–8, it is observed that the effect of surfactant concentration on
IFT reduction from 1 to 12% does not vary much. Hence, to optimize the surfactant
concentration, lower concentrations were investigated for IFT reduction. It was found
that lowest average IFT of 3.25 dyne/cm was recorded at the concentration of 1.5% of
surfactant solution, which is considered to be the optimum concentration (Figure 9). The
error bars are plotted and maximum standard deviation was found to be 7.6%. Even
though the same crude oil was used for this experiment, the initial value of IFT was
found to be different because the second experiment was carried out after two months

Figure 9. Optimum concentration for IFT reduction.

 Natural Surfactant for Enhanced Oil Recovery 1901

and the organic acid of the crude oil might have changed the properties due to natural
degradation.
Borwankar and Wasan (1986) studied the dynamic interfacial tensions in acidic crude
oil using alkaline flooding for EOR and reported that interfacial tension reduction using
surfactant is a dynamic phenomenon. This study reported that the interfacial tension
rises after it reached to minimum to the final value corresponding to the equilibrium
interfacial tension between oil and aqueous phase containing caustic solutions. They
used sodium hydroxide as surfactant and reported that the IFT was significantly reduced
at the beginning and then increased later on. Chatterjee and Wasan (1998) reported that
dynamic IFT minimum observed in some systems have been attributed to the maxima in
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interfacial specific adsorption caused by the desorption of the surfactant into the initially
surfactant-free phase. Similar results were reported by Taylor et al. (1990) in surfactant
enhanced alkaline flooding. They reported that the IFT reduction at the shortest time
possible is very useful as the frontal movement during oil recovery takes place right after
the application of surfactant in the injection hole. This means that IFT reduction may not
be useful if it takes a long time to influence the oil properties. Ayirala and Rao (2004)
experimentally investigated the effects of nonionic surfactants, such as ethoxy alcohol,
and anionic surfactants, such as ethoxy sulfate, to reduce the interfacial tension in the
crude oil. The results showed that an optimum concentration of 3,500 ppm was most
effective for the maximum oil recovery.
Liu et al. (2006) studied the emulsification and entrainment of crude oil into dis-
placing water as one of the mechanisms of alkaline flooding for conventional oil and the
possibility of using this phenomenon in heavy oil recovery. A very dilute surfactant (alkyl
ether sulfates) and alkali .Na2 CO3 / together were used for IFT reduction. It was found
that emulsification of heavy oil in brine was possible at ultra low IFT, which occurred
due to the application of a surfactant along with alkali. The IFT reduces significantly at
the beginning and increases slightly after 60 min. The result of this study is very similar
to what was found in the present study with surfactant.

5. Conclusions
In this article, pericarp shell of grounded soapnut (Sapindus mukorossi) was used as
a natural surfactant to reduce the oil-water interfacial tension. The effect of surfactant
concentration with 1%, 2%, 4%, 8%, and 12% was investigated. The experimental results
showed that surfactant can effectively reduce oil-water IFT. The effect of heat on IFT was
also studied. It was found that higher IFT reduction was achieved after heating the system
to 50ı C. The experimental results showed that extract has a great potential to be used as
a surfactant for the enhanced oil recovery schemes. It is also discussed that compared to
synthetic surfactants, a surfactant is an economical and environmental friendly option to
use in EOR schemes.

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