Journal of Cleaner Production 220 (2019) 1005e1013

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Journal of Cleaner Production

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

Sustainability of water in diesel emulsion fuel: An assessment of its

corrosion behaviour towards copper
Davannendran Chandran a, *, Mohammad Khalid a, Revathi Raviadaran b,
Harrison Lik Nang Lau c, Chee Liang Yung c, Dinesh Kanesan d, Mohammed Salim e
a
Graphene & Advanced 2D Materials Research Group (GAMRG), Sunway University, No. 5, Jalan Universiti, Bandar Sunway, 47500, Subang Jaya, Selangor,
Malaysia
b
Department of Chemical and Environmental Engineering, University of Nottingham Malaysia Campus, Jalan Broga, 43500, Semenyih, Selangor, Malaysia
c
Malaysian Palm Oil Board, No.6, Persiaran Institusi, Bandar Baru Bangi, 43000, Kajang, Selangor, Malaysia
d
Petroleum Engineering Department, University Teknologi PETRONAS, 32610, Seri Iskandar, Perak, Malaysia
e
School of Mechanical Engineering, Linton University College, 71700, Mantin, Negeri Sembilan, Malaysia

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

Article history: Despite studies have demonstrated the possibilities of using water in diesel emulsion fuel to reduce the
Received 7 June 2018 harmful exhaust emission, limited studies are available at present on the effect of emulsified diesel to-
Received in revised form wards metal corrosion. This study therefore aims to investigate the corrosion behaviour of copper
21 November 2018
exposed to emulsified diesel. Copper immersion tests in diesel, biodiesel and emulsified diesel were
Accepted 19 February 2019
Available online 20 February 2019
carried out for 1200 h at 25
C. Similar immersion test in emulsified diesel was also carried out for 240 h,
480 h, 720 h, 960 h and 1200 h at 25
C. Two emulsifiers such as Span 80 and Tween 80 were used to
prepare emulsion consisting of 5 vol% of water in diesel. Among the performed analysis were mass loss,
Keywords:
Emulsified diesel fuel
surface morphology, elemental composition, surface topography, surface roughness, microscopy, Fourier
Exhaust emission transform infrared spectroscopy, emulsion characterization, density, viscosity, water content and total
Copper corrosion acid number. 11.7 times and 4.7 times higher corrosion rate occurred to the copper coupon exposed to
Emulsifier emulsified diesel as compared to diesel and biodiesel, respectively. 68% reduction in corrosion rate
Acidity occurred for the copper exposed to emulsified diesel between 240 h and 1200 h of immersion duration.
Up to 3.6 mm and 1.7 mm in pit depth and width, respectively, formed on the copper surface exposed to
emulsified diesel for 1200 h at 25
C. The increased acidity of emulsified diesel by 4.5 times as compared
to diesel due to the addition of emulsifiers to form stable water in diesel emulsion is suggested to have
caused the increased corrosion rate. Neutralization and/or use of less acidic emulsifier are recommended
to reduce the corrosive effect of emulsified diesel. More works on this area are required to establish the
compatibility present between emulsified diesel and fuel delivery metals.
© 2019 Elsevier Ltd. All rights reserved.

1. Introduction 2017). Therefore, it is more viable to adopt renewable and cleaner

Despite electric powered vehicle have gathered attention due to
its zero emission, the zero emission is debateable for countries
which mainly relies on burning of fossil fuel to generate electricity.
The requirements of huge battery space of 150 gallons which
weighs 2000 pounds for electric vehicle to travel the same distance
of a fuel powered vehicle equipped with a 13-gallon tank weighing
82 pounds poses another critical challenge for electric powered
vehicles to displace conventional engines (Todd Davidson et al.,
* Corresponding author.
E-mail address: dchandran@sunway.edu.my (D. Chandran).
energy to displace fossil fuel at present. Aligned to this, a number of
countries adopted biodiesel fuel since it is capable to reduce
harmful exhaust emission of unburned hydrocarbon (UHC), carbon
monoxide (CO) and nitrogen oxide (NOx) by 52.4%, 47.6%
and 10%, respectively, as compared to diesel fuel (Hofman, 2003).
In 2017, biodiesel has been adopted in blended form with diesel in
European Union, Malaysia, Brazil and Indonesia at a blending
mandate of 5.75 vol%, 7 vol%, 8 vol%, and 20 vol% of biodiesels,
respectively (Lane, 2016).
Besides the adoption of biodiesel, there has also been research
works which exhibited the potential of emulsified diesel (water in
diesel) fuel to reduce harmful exhaust emission of diesel engine.

https://doi.org/10.1016/j.jclepro.2019.02.210
0959-6526/© 2019 Elsevier Ltd. All rights reserved.
1006 D. Chandran et al. / Journal of Cleaner Production 220 (2019) 1005e1013

Perumal and Ilangkumaran (2018) investigated the emission char- total acid number, viscosity and density.
acteristics of water emulsified hybrid Pongamia biodiesel-diesel
fuel blend using a direct injection engine. The authors utilized
2. Material and methods
Kirloskar AV1 single cylinder four stroke naturally aspirated DI
diesel engine attached with eddy current dynamometer for the
Copper coupons of 0.02 m in diameter and 0.002 m in thickness
investigation. The authors reported a reduction of NOx, smoke, CO
were utilized in this study. The coupon was hanged using a silk
and UHC by 32%, 7.4%, 2.3% and 1%, respectively, as compared to B20
string through a hole of 0.002 m in diameter drilled near the edge.
biodiesel-diesel fuel blend. Ithnin et al. (2018) investigated the
Not additized diesel supplied by the Malaysian Palm Oil Board,
exhaust emission of emulsifier free emulsified diesel consisting of
distilled water prepared from TKA Smart2Pure and the combina-
5 vol% of water using a single cylinder, four stroke, air-cooled, direct
tion of two types of emulsifiers (Span 80 and Tween 80) were used
injection diesel engine of 0.4l capacity. The authors reported
to prepare the emulsified fuel. The emulsion consisting of 5 vol% of
reduction in NOx and particulate matter (PM) by 31.67% and 16.33%,
water, 3 vol% of emulsifiers and 92 vol% of diesel was prepared
respectively, as compared to neat diesel. In another study by Ithnin
using Silverstone LM-5 high shear mixer. The emulsion preparation
et al. (2015), the authors reported reduced NOx and PM by 41% and
consisted of 4 stages. Firstly, 1.5 vol% of Span 80 was mixed with
35%, respectively, for emulsified diesel with 20 vol% water in low
92 vol% of diesel for 5 min. This was then followed with the addi-
grade diesel as compared to low grade diesel using the similar
tion of 1.5 vol% of Tween 80 and mixed for another 5 min. Finally,
engine setup as described above.
5 vol% of water was added and mixed for 10 min. Rotational speed
Hasannuddin et al. (2018) investigated the emission of a single
of 3500 revolutions/min was used throughout the mixing.
cylinder, air cooled, vertical MC-D6500E diesel engine using 10 vol%
For comparisons, two other types of fuels such as not additized
of water and 20 vol% of water in diesel, independently. The authors
diesel and palm biodiesel with 11 h of oxidation stability supplied
reported decreased PM and NOx with increased water content in
by the Malaysian Palm Oil Board were included in the copper im-
the emulsion fuel. Khalife et al. (2017) reported reduced carbon
mersion study. The fatty acid compositions of the palm biodiesel
dioxide (CO2), HC, and NOx emissions by over 8.5%, 28%, and 24%,
consisted of 0.20 ± 0.01%, 1.09 ± 0.01%, 41.80 ± 0.34%, 4.84 ± 0.10%,
respectively, with 4 vol% of water in B5 biodiesel-diesel fuel blend
41.20 ± 0.12%, 10.32 ± 0.20% and 0.55 ± 0.02% of C12:0, C14:0, C16:0,
as compared to neat diesel. The authors performed the experiment
C18:0, C18:1, C18:2 and C18:3, respectively, determined using Per-
using a single cylinder, four-stroke and direct injection diesel en-
kin Elmer Autosystem XL Gas Chromatography according to EN
gine (YANMAR L48N) coupled with an eddy current dynamometer
14103 (EN 14103, 2011).
(10 kW). Ogunkoya et al. (2015) in a study investigated the emis-
The metal corrosion investigation was carried out according to
sions in a diesel engine operated with fuel-in-water emulsions
ASTM G1 (ASTM G1-(03)17, 2017a) and ASTM G31 (ASTM G31-12a,
based on lignin. The authors conducted the investigation using a
2012) standard methods. 38 ml of fuel quantity was utilized for
single-cylinder air-cooled compression-ignition engine (Model CS-
each copper immersion study according to SAE J1747 (SAE J1714-13,
186 from Carroll Stream Motor Company, Inc) with 0.46 kW of
2013). The samples were sealed and placed in a closed and dark
power. The authors reported reduced NOx by up to 44% for emul-
environment at 25
C. For emulsified diesel, the samples were
sified diesel consisting of 30 vol% of water in diesel as compared to
stored for 240 h, 480 h, 720 h, 960 h and 1200 h. For diesel and
diesel. Besides the above studies, several other studies have also
biodiesel, the samples were stored for 1200 h. An additional spec-
demonstrated the reduction of exhaust emission with the utiliza-
imen was analysed as duplicate for each condition. The copper
tion of emulsified diesel (Fahd et al., 2013; Mazlan et al., 2018; Xu
coupons were polished with silicon carbide abrasive papers from
et al., 2016; Yang et al., 2013).
grade 400 to 1200, washed, degreased with acetone and dried prior
Considering the benefits of reduced harmful exhaust emission
to measuring its initial mass. After the immersion, coupons were
that can be achieved from emulsified diesel as highlighted above, it
cleaned in stream of water and dried prior to measuring its final
is absolutely necessary to investigate the feasibility of adopting
mass. The average of the mass loss measured from the duplicate
emulsified diesel for use in diesel engine. Among the critical aspect
specimens were used for calculating corrosion rate using the
that needs to be fulfilled prior to adopting an alternative/modified
equation from ASTM G31 (ASTM G31-12a, 2012) as presented in Eq.
fuel is the materials compatibility. This is chiefly because the
(1).
components in a diesel engine fuel system has been designed to be
compatible with diesel. The use of incompatible fuel could signifi- KxW
cantly reduce the components lifespan culminating in stalling the Corrosion rate ðmm=yrÞ ¼ (1)
AxTxD
engine due to fuel leakage (Chandran et al., 2016a).
Despite the research on emulsified diesel towards emission
reduction has been continuously reported since 1970s’, limited
information is available to date concerning the compatibility of Constant, K;
emulsified diesel with diesel engine fuel delivery materials. This Time of exposure, T (h);
study aims to investigate the compatibility of emulsified diesel with Area, A (cm2);
fuel delivery metals by performing immersion study. Copper cou- Mass loss, W (g);
pons were exposed to emulsified diesel, biodiesel and diesel at 25 Density, D (g/cm3)

C for 1200 h according to ASTM G1 (ASTM G1-(03)17, 2017a) and

ASTM G31 (ASTM G31-12a, 2012) standard methods. Similar im-
mersion test was also performed with copper coupons in emulsi-
fied diesel at various immersion duration such as 240 h, 480 h,
720 h and 960 h. The prepared emulsified diesel consisted of 5 vol%
of water, 1.5 vol% of Span 80, 1.5 vol% of Tween 80 and 92 vol% of not
additized diesel. Among the performed analysis were mass loss
determination, surface morphology, elemental composition, sur-
face topography, roughness profile, microscopy, Fourier transform
infrared spectroscopy, emulsion characterization, water content,
The surface morphology, surface topography and roughness
profile were analysed using LEXT 3D Measuring Laser Microscope
OLS5000. The elemental composition was determined using Oxford
Instruments Inca Energy-dispersive X-ray spectroscopy. The images
of the fuels before and after the immersion investigation were
captured using Panasonic Lumix DMC-TZ20. The optical images of
the emulsified fuel were captured using Nikon DS-Fi1 light mi-
croscope. Fourier transform infrared (FTIR) spectroscopy analysis
was performed using Perkin Elmer Frontier model FTIR
 D. Chandran et al. / Journal of Cleaner Production 220 (2019) 1005e1013
spectrometer. The stability of the emulsified diesel was measured
in terms of the change in droplet size and dispersity index. Existing
studies have extensively employed droplet size and dispersity in-
dex to exhibit the stability of the formed emulsion (Tang et al.,
2013; Ushikubo and Cunha, 2014; Steuber et al., 2016; Raviadaran
et al., 2018a, 2018b, 2018c). The droplet size and dispersity index
were measured using Malvern Instruments Zetasizer Nano ZS 90.
Among the determined fuel properties before and after the
immersion investigations were water content, total acid number,
viscosity and density. Metrohm 809 Titrando, Metrohm 831 KF
Coulometer, Herzog HVM 472 and Mettler Toledo DE40 were uti-
lized to determine the total acid number, water content, viscosity
and density, respectively. For total acid number analysis, fuel
samples of 20.0 g and standard titrant 0.01 M alcoholic potassium
hydroxide (KOH) were used according to ASTM D664 (ASTM D664-
17a, 2017b). For water content, 2.0 g of fuel samples was utilized
according to ISO 12937 (ISO 12937-00, 2000). For viscosity, 40 ml of
fuel sample was used according to ISO 3104 (ISO 3104-94, 1994). For
density, 5 ml of fuel sample was used according to ISO 12185 (ISO
12185-96, 1996). Error bars based on standard errors are pre-
sented in the graphs.
3. Results and discussion
As shown in Table 1, the corrosion rate of copper in emulsified
diesel was determined to be the highest at 0.000494 mm/yr fol-
lowed by in biodiesel at 0.000105 mm/yr and finally in diesel at
0.000043 mm/yr after 1200 h of immersion at 25
C. 11.5 times
higher corrosion rate of copper occurred in emulsified diesel as
compared to diesel. Whilst, 4.7 times higher corrosion rate of
copper was observed in emulsified diesel when compared to in
biodiesel. This shows that emulsified diesel causes higher corrosion
compared to fossil-based diesel and palm oil-based biodiesel.
Comparisons of copper corrosion rate in emulsified diesel with
existing studies was not made possible due to the scarcity of
research work in this area till present. The higher corrosion rate of
copper in biodiesel as compared to in diesel by 2.4 times corrob-
orates with several existing studies. Haseeb et al. (2010) conducted
corrosion test of copper in biodiesel and diesel at room (25e30
C)
temperature for 2640 h. The authors reported 1.6 times higher
corrosion rate of copper in biodiesel as compared to diesel. Fazal
et al. (2012) reported 2.9 times higher corrosion rate of copper in
biodiesel as compared to in diesel when performed immersion test
at room (25e27
C) temperature for 2880 h. Hu et al. (2012) re-
ported 6.6 times higher corrosion rate of copper exposed to bio-
diesel as compared to diesel after 60 days of immersion at 43
C.
Other studies have also reported higher corrosion rate of metal due
to biodiesel exposure as compared to diesel exposure (Samuel et al.,
2016; Samuel and Gulum, 2018).
As shown in Fig. 1, the copper corrosion rate was observed to
reduce with increasing immersion duration in emulsified diesel.
The corrosion rate reduced by 68% after 1200 h of immersion
duration as compared to 240 h of immersion duration. Compari-
sons on the trend of corrosion rate of emulsified diesel corre-
sponding to immersion duration was not possible due to scarcity in
this area. However, the observed trend of reduced corrosion rate
with increasing immersion duration corroborates with the study
Table 1
Corrosion rate of copper exposed to diesel, biodiesel and emulsified diesel for 1200 h at 25
C.
Diesel
Mean SD
Corrosion rate, mm/yr 4.29E-05 8.76E-08
1007
0.0009
Corrosion rate (mm/yr)
0.0008
0.0007
0.0006
0.0005
0.0004
0 240 480 720 960 1200
Duration (hours)
Fig. 1. Corrosion rate of copper exposed to emulsified diesel at 25
C corresponding to
immersion duration.
reported by Chandran et al. (2016b) for copper exposed to biodiesel.
The authors in the study reported reduced corrosion rate by 2.8%
after 540 h of immersion duration as compared to 108 h of im-
mersion duration. Similarly, Fazal et al. (2013) in a study reported
reduced corrosion rate of copper by 19.5% due to biodiesel exposure
between 1200 h and 2880 h of immersion duration. Contrastingly,
Fazal et al. (2018) in a different study reported increased corrosion
rate of copper by 50% after 1200 h of immersion duration as
compared to 600 h of immersion duration in biodiesel. In the same
study, the authors also reported that the corrosion rate of copper
was similar between 600 h of immersion duration and 1200 h of
immersion duration exposed to diesel. Similarly, Fazal et al. (2010)
in another study also reported increased corrosion rate of copper
with increasing immersion duration due to biodiesel exposure
while the corrosion rate remained similar due to diesel exposure.
From the surface morphology as shown in Fig. 2, it is evident
that the copper surface exposed to emulsified diesel had the
highest corrosion attack followed by the copper exposed to bio-
diesel and finally to diesel. Formation of pits are visible for the
copper coupon exposed to emulsified diesel at 2000 times
magnification. Pits of about 3.1e3.6 mm in width were measured on
the copper surface exposed to emulsified diesel.
From the elemental compositions analysis as shown in Fig. 3, the
copper coupon exposed to emulsified diesel has the highest in-
crease in oxygen composition by 21.2 times, followed by the coupon
exposed to biodiesel by 10 times and the coupon exposed to diesel
by 7.6 times, as compared to the as-received copper coupon. This
increase in the oxygen composition on the copper coupon surface
exhibits the level of corrosion activity as the oxygen participated
during the corrosion process and displaced the copper present on
the coupon surface.
The intensity of corrosion attack towards the copper coupons
due to the exposure to diesel, biodiesel and emulsified diesel was
more apparent by performing surface topography analysis as
exhibited in Fig. 4. Referring to the 2-dimensional surface topog-
raphy, the colours such as red, yellow, green, light blue and dark
blue were used to project the condition of the copper surface. Based
on it, the copper coupons exposed to diesel and biodiesel, inde-
pendently, did not show noticeable difference as compared to the
Biodiesel Emulsified diesel
Mean SD Mean SD
1.05E-04 1.07E-07 4.94E-04 1.24E-07
1008 D. Chandran et al. / Journal of Cleaner Production 220 (2019) 1005e1013

Fig. 2. Surface morphology of copper exposed to diesel, biodiesel and emulsified diesel
at 25
C for 1200 h.

as-received copper surface. On the other hand, the copper surface

exposed to emulsified diesel deteriorated significantly as a number
of dark blue spots are present denoting the formation of pits.
Fig. 5 shows the surface roughness of copper coupons before
and after exposure to diesel, biodiesel and emulsified diesel,
independently. Based on the roughness profile, the copper coupon
exposed to diesel and biodiesel, independently, remained close to
the mean line. The copper coupon exposed to emulsified diesel
however exhibited a number of valley formations (below the mean
line). The roughness average (Ra) of the copper coupon after
exposure to diesel, biodiesel and emulsified diesel is higher by 1.3
times, 1.7 times and 4.8 times, respectively, as compared to the as-
received copper coupon. The copper coupon exposed to emulsified
diesel has a Ra value of 3.7 times higher than the copper exposed to
diesel. The 1.3 times higher Ra value for the copper coupon exposed
to biodiesel as compared to diesel agrees with the study reported
by Fazal et al. (2011). The authors reported 1.3 times higher Ra value
for the mild steel exposed to biodiesel as compared to diesel at 80 Fig. 3. Elemental compositions of copper exposed to diesel, biodiesel and emulsified

C for 1200 h. The maximum profile valley depth (Rv) of the copper diesel at 25
C for 1200 h.

coupon exposed to emulsified diesel is 4.3 times and 2.9 times

higher as compared to the copper coupon exposed to diesel and
biodiesel, respectively. The high Rv value for the copper coupon
exposed to emulsified diesel of 1.706 mm denotes the highest depth
of formed pit. The copper coupon exposed to emulsified diesel has a
higher maximum height of the profile (Rt) of 321% as compared to
copper coupon exposed to diesel. The significantly higher Ra, Rv
and Rt values for the copper coupon exposed to emulsified diesel as
compared to biodiesel and diesel, independently, demonstrates the
severity of corrosion attack.
Fig. 6 shows the fuels colour before and after exposure to copper.
It is observed that the prepared emulsified diesel is creamy brown,
while the as-received diesel and biodiesel are orange and light
yellow, respectively. After exposure to copper, the colour of the
emulsified diesel changed to creamy green, diesel changed to dark
orange and biodiesel changed to yellow. The changes in diesel and
biodiesel exposed to copper has also been reported in existing
studies. Fazal et al. (2010) reported biodiesel changed from col-
ourless to green while diesel changed from light yellow to dark
orange due to exposure to copper at 80
C for 1200 h. In a different
study, Fazal et al. (2013) reported the biodiesel changed from light
yellow to dark greenish yellow due to copper exposure for 1200 h at
room temperature. Hu et al. (2012) reported the biodiesel changed
from yellow to green due to copper exposure for 60 days at 43
C.
These changes in the fuel colour indicates changes in fuel proper-
ties. Critically, no separation of water and diesel was detected for
the emulsified diesel after exposure to copper.
Fig. 7 shows the FTIR spectrum of diesel, emulsified diesel and
biodiesel before and after exposure to copper for 1200 h.
Comparing the as-received diesel and prepared emulsified diesel
FTIR spectra, no additional functional group was detected for to
 D. Chandran et al. / Journal of Cleaner Production 220 (2019) 1005e1013
Fig. 4. 2-Dimensional surface topography of copper exposed to diesel, biodiesel and
emulsified diesel at 25
C for 1200 h.
Fig. 5. Surface roughness of copper exposed to diesel, biodiesel and emulsified diesel
at 25
C for 1200 h.
prepared emulsified diesel. Comparing the prepared emulsified
diesel and emulsified diesel after exposed to copper FTIR spectra,
1009
Fig. 6. Colour of emulsified diesel (W5D2), diesel (D2) and biodiesel (B100) before and
after exposure to copper at 25
C for 1200 h.
Fig. 7. FTIR spectrum of diesel, emulsified diesel and biodiesel.
no peak was detected at about 3400 cm1 which corresponds to
hydrogen-bonded water molecules (Chaplin, 2000). This shows
that the water remained in emulsion form and did not form free
water throughout the study. Comparing the FTIR spectra of the as-
received biodiesel and biodiesel after exposed to copper, additional
functional group located at 3460 cm1 was detected for the bio-
diesel exposed to copper. This peak which corresponds to oxygen
bearing compound (CeOH) (Gomez et al., 2011) reveals that the
biodiesel has oxidized due to copper exposure for 1200 h at 25
C.
This finding corroborates to the study reported by Chandran et al.
(2016b).
Fig. 8 shows the optical micrographs of diesel, emulsified diesel,
emulsified diesel after 1200 h, as well as emulsified diesel after
exposure to copper for 1200 h at 40 times magnification. From it, no
droplets were present in diesel while droplets with a mean droplet
diameter of 200.5 ± 6.1 nm and dispersity index of 0.220 ± 0.024
were present in emulsified diesel. After 1200 h of storage, the mean
droplet diameter of the emulsified diesel increased to
388.8 ± 16.0 nm with a dispersity index of 0.582 ± 0.035. Consid-
ering that no separation was observed coupled with no detection of
free water from FTIR analysis, the emulsified diesel was considered
stable after 1200 h of storage at 25
C (Chen and Zhang, 2017). As a
result of copper exposure to the emulsified diesel for 1200 h at 25

C, the mean droplet diameter increased by 6.3 times and 3.2 times
as compared to as-prepared emulsified diesel and emulsified diesel
after 1200 h of storage, respectively. The emulsified diesel exposed
to copper has a dispersity index of 0.790 ± 0.25. The corrosion of
copper led to leaching of copper ions in the emulsion culminating
in sedimentation. The copper ion (Cu2þ) could have prevented the
electrostatic/steric repulsion between the water droplets, bringing
1010 D. Chandran et al. / Journal of Cleaner Production 220 (2019) 1005e1013

Fig. 8. Optical micrographs of diesel, emulsified diesel, emulsified diesel after 1200 h
and emulsified diesel exposed to copper for 1200 h at 25
C.

them together. This caused thinning of the emulsifier film coating

the droplets hence favoured coalescence and led to sedimentation
(Tadros et al., 2004).
Fig. 9 (a) shows the density of the fuels before and after expo-
sure to copper. From it, the prepared emulsified diesel has 2%
higher density than diesel. Increase in density by 1.9% and 3.5% for
the emulsified diesel with 5 vol% of water as compared to diesel
was also reported by Ismael et al. (2018) and Elsanusi et al. (2017),
respectively. This increase in the density of the prepared emulsified
diesel could have resulted due to emulsification of water in diesel.
Generally, the density of water of ~1000 kg/m3 is higher than the
density of diesel of between 820 kg/m3 and 860 kg/m3. Changes in
density before and after exposure to copper of less than 1% for all
three fuels shows that the density property was not affected due to
copper exposure. Similar outcome of less than 1% change for den-
sity was reported by Fazal et al. (2018) for both diesel and biodiesel
exposed to copper for 1200 h at room temperature.
As shown in Fig. 9 (b), the viscosity of the emulsified diesel is
18% higher than diesel. Ismael et al. (2018) and Elsanusi et al. (2017)
reported increase in viscosity for the emulsified diesel with 5 vol%
of water by 57% and 40%, respectively, as compared to diesel. This
increase in the viscosity value of the prepared emulsified diesel
could have resulted due to the presence of water in emulsion form
in diesel. Changes in viscosity before and after exposure to copper
are 3% and 29% for biodiesel and emulsified diesel, respectively.
Whilst, the viscosity remained close to the as received for the diesel
exposed to copper. The increase in the viscosity of the emulsified
diesel after exposure to copper could be due to the increase in the
size of water droplets. The increase in viscosity for biodiesel
meanwhile agrees to the study by Fazal et al. (2012) which the
authors reported 25% increase in viscosity due to biodiesel expo-
sure to copper for 2880 h at room temperature. Shahabuddin
Ahmmad et al. (2018) also reported 21% increase in biodiesel’s
viscosity due to copper exposure for 1600 h at 80
C. Fig. 9. Changes in (a) density, (b) viscosity, (c) water content and (d) total acid number
From Fig. 9 (c), the prepared emulsified diesel has 868 times and of diesel, biodiesel and emulsified diesel exposed to copper for 1200 h at 25
C.
180 times higher water content to those of diesel and biodiesel,
respectively. The 5 vol% water content in emulsified diesel reflects
the concentration of water in the prepared emulsion. This shows water content increased by 12 times for the biodiesel due to
that Karl-Fischer titrator detects the water content in the fuel exposure to copper while it remained for diesel and emulsified
sample regardless of whether it is in free or emulsion form. The diesel. The hygroscopic nature of biodiesel to capture moisture
 D. Chandran et al. / Journal of Cleaner Production 220 (2019) 1005e1013 1011

could have influenced this as suggested in literature (Chandran

et al., 2016b). The increase in the water content for the biodiesel
exposed to copper corroborates with several existing studies
(Chandran et al., 2016b; Fazal et al., 2010, 2014, 2017; Haseeb et al.,
2010).
As shown Fig. 9 (d), total acid number of the prepared emulsified
diesel is 4.5 times and 3.3 times higher than diesel and biodiesel,
respectively. The addition of emulsifier/surfactant to form stable
water in diesel emulsion contributed to the increase in total acid
number as compared to diesel. The total acid number of Span 80
and Tween 80 are 13.90 mgKOH/g and 2.65 mgKOH/g, respectively.
Changes in total acid number before and after exposure to copper
are 96%, 595% and 15% for diesel, biodiesel and emulsified diesel,
respectively. The significant increase in total acid number for the
copper exposed biodiesel shows that the fuel has degraded during
the immersion investigation (Chandran et al., 2016b). Biodiesel’s
higher susceptibility to degradation due to its lower oxidation
stability as compared to diesel could have influenced this. This in-
crease in total acid number for diesel and biodiesel exposed copper
corroborates with the findings from the existing studies (Fazal
et al., 2010, 2012, 2013). The reduction in total acid number for
the emulsified diesel suggest that the acidity of the fuel reduced
during the exposure to copper. This reduction in total acid number
could have been influenced by the participation of the acidic sub-
stance present in the emulsified diesel in the corrosion process
which culminated in severe corrosion attack towards the copper
coupon.
Since the density and water content of the emulsified diesel did
not change after 1200 h of exposure to copper at 25
C, the change
in viscosity and total acid number of emulsified diesel exposed to Fig. 10. Changes in (a) viscosity and (b) total acid number of emulsified diesel exposed
to copper at 25
C corresponding to immersion duration.
copper for 240 h, 480 h, 720 h, 960 h and 1200 h are presented in
Fig. 10 (a) and (b), respectively. Based on it, the viscosity of the
emulsified diesel is observed to increase with increasing copper of injection pressure. The water reduction was suggested due to
exposure duration. Meanwhile, the total acid number of the water separation or evaporation out of the emulsion. The lost water
emulsified diesel is observed to decrease with increasing copper from the emulsion reported from the study above would never-
exposure duration. theless form free water in the fuel system. Free water in the fuel
Considering no formation of free water in the emulsified diesel system of a diesel engine is detrimental since water promotes
since water diesel separation did not occur throughout the im- corrosion resulting in an accelerated mass loss leading to fuel
mersion duration, the influence of water present in emulsion form leakage. Fuel leakage could cause fuel pump seizing abruptly
in diesel is unlikely to have caused the significant increase in the stalling the engine (Chandran et al., 2016a).
corrosion rate as compared to diesel. Instead, the addition of sur- In order to establish the compatibility present between emul-
factants to form stable water in diesel emulsion preventing sepa- sified diesel and fuel delivery materials, it essential to determine
ration is suggested to have contributed to the increased corrosion the deterioration of emulsified diesel under real-life diesel engine
rate. Existing study have shown the adverse effect of diesel fuel operation (Chandran, 2017; Chandran et al., 2017; Wadumesthrige
acidity towards metal corrosion. Tsuchiya et al. (2006) reported et al., 2010). This is important considering the high fuel pressure of
increased metal corrosion with increased acidity (total acid num- up to 2000 bar and temperature of up to 100
C under physical
ber) of the tested diesels. Neutralization of the emulsified diesel’s common rail type diesel engine operation could alter the physico-
acidity and/or utilization of less acidic emulsifier are recommended chemical properties of emulsified diesel which subsequently could
to reduce the corrosive effect of the emulsified diesel. Preparation adversely affect the degradation of fuel delivery materials. Through
of surfactant free emulsified diesel might mitigate the acidity effect this, the fuel properties which should be emphasized could be
of surfactants towards metal corrosion. Nevertheless, the formation identified. Besides, modifications might be required to the existing
of free water due to water diesel separation as a result of poor immersion test in order to mimic the deterioration of emulsified
emulsion stability would adversely affect the metal corrosion diesel under laboratory condition to produce materials degradation
instead. which resembles the actual condition in the fuel delivery system of
With regard to the above, Ismael et al. (2018) recently reported an engine (Chandran et al., 2016b, 2018).
the effects of fuel injection equipment towards the dispersed
phased of water-in-diesel emulsions. No addition of surfactant was
reported for the emulsion preparation. The prepared emulsion was 4. Conclusions
reported stable for the initial 2 h and exhibited some de-
mulsification after 7 h. Instead of a real-life diesel engine, the au- The corrosion behaviour of emulsified diesel was evaluated in
thors utilized an experimental setup which consisted of a common this study. The exposure of copper to emulsified diesel resulted in
rail electronically controlled injected system to generate and significantly higher corrosion rate by 11.7 times and 4.7 times as
induce high pressure sprays into the samples collector. The authors compared to diesel and biodiesel, respectively. The severe corrosion
reported 2.5 vol% of water reduction in the emulsion which origi- attack on the copper exposed to emulsified diesel as compared to
nally constituted of 15 vol% of water in diesel as a result of 1500 bar diesel and biodiesel, was evident from the surface morphology,
1012 D. Chandran et al. / Journal of Cleaner Production 220 (2019) 1005e1013
elemental composition, surface topography and roughness profile
analysis. 2.8 times higher oxygen composition and 3.7 times higher
roughness average value for the copper coupon exposed to emul-
sified diesel as compared to diesel exhibited the intensity of
corrosion attack towards the copper surface. The corrosion rate of
copper exposed to emulsified diesel reduced by 68% with increased
immersion duration of between 240 h and 1200 h. Pits of a width
and depth of up to 3.6 mm and 1.7 mm, respectively, formed on the
copper surface exposed to emulsified diesel for 1200 h at 25
C.
Formation of free water as a result of water diesel separation did
not occur hence prevented water’s influence towards the corrosion
rate. Instead, the addition of emulsifiers to form stable water in
diesel emulsion preventing the formation of free water adversely
affected the rate of copper corrosion due to the increased acidity of
emulsified diesel by 4.5 times than diesel. Neutralization of the
emulsified diesel’s acidity and/or utilization of less acidic emulsifier
for the preparation of emulsified diesel are recommended to reduce
the corrosiveness of emulsified diesel in order to benefit the po-
tential reduction of exhaust emission which can be achieved by
adopting it. Despite surfactant free emulsified diesel might prevent
the adverse surfactant’s acidity effect towards metal corrosion, the
formation of free water due to water diesel separation would pro-
mote corrosion instead. More works on this area especially the
deterioration of emulsified diesel under real-life diesel engine
operation, as well as identification of the required modifications for
the immersion test to produce materials degradation which re-
sembles the condition in a physical engine are necessary to estab-
lish the compatibility present between fuel delivery metals and
emulsified diesel.
Declarations of interest
None.
Acknowledgements
The authors acknowledge the support provided by Sunway
University through the provided research grant (INT-2018-SST-
RCNMET-05) and the Malaysian Palm Oil Board in facilitating this
study.
Abbreviations
ASTM American Society for Testing and Materials
CO2 carbon dioxide
CO carbon monoxide
FTIR Fourier transform infrared
ISO International Organization for Standardization
mm/yr millimetre per year
NOx nitrogen oxide
PM particulate matter
Ra roughness average
Rt maximum height of the profile
Rv maximum profile valley depth
SAE Society of Automotive Engineers
UHC unburned hydrocarbon
vol volume
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