Energy 70 (2014) 43e48

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Energy
journal homepage: www.elsevier.com/locate/energy

Mackerel biodiesel production from the wastewater containing fish oil

Y.P. Wu a, *, H.M. Huang b, Y.F. Lin a, W.D. Huang a, Y.J. Huang a
a
Department of Chemical and Materials Engineering, National Ilan University, I-lan 26047, Taiwan, ROC
b
Department of Aquaculture, National Suao Marine & Fisheries Vocational High School, I-lan 27048, Taiwan, ROC

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

Article history: Marine fish such as mackerel are important for coastal fisheries in Taiwan. Nearly 60,000 tons of
Received 8 September 2013 mackerel are produced in Suao, I-lan, Taiwan every year. In this study, oil from the discarded parts of
Received in revised form mackerel fish contained in wastewater stream were used as the raw material to produce biodiesel
14 February 2014
through transesterification reaction. The major fuel properties of MB (mackerel biodiesel), including the
Accepted 20 March 2014
Available online 1 May 2014
iodine value, dynamic viscosity, flash point, and heat value, were determined and compared with sun-
flower seed oil methyl ester (SFM), JCB (Jatropha curcas biodiesel), and premium diesel (D). MB had a
higher iodine value, dynamic viscosity, density, and flash point, but a lower heat value, than did D. MB
Keywords:
Mackerel biodiesel
was also used as fuel in a regular diesel engine to verify its emission characteristics. The MB fuel used for
Biodiesel emissions exhaust emission test included pure MB (MB100) and a 20% MB blend with premium diesel (MB20). The
Fish oil wastewater exhaust emission of MB was also compared with the exhaust emissions of D and JCB. The results showed
Jatropha curcas biodiesel that MB20 provided a significant reduction in NO, NOx, and SO2 emissions under varied engine loads, and
required no engine modification.
Ó 2014 Elsevier Ltd. All rights reserved.

1. Introduction
Biodiesel is an alternative diesel fuel derived from a variety of
fatty-acid-methyl-ester-producing processed vegetable oils, animal
fats, or waste frying oils [1e4]. It is described as an alternative fuel
which improves environmental conditions and contributes to
gaining energy sustainability [5]. The use of blends with 2e30%
fossil diesel fuel does not require any modification of the car engine.
In some cases minor modifications are required for the use of 100%
pure biodiesel [6].
Lapuerta et al. [7] collected and analyzed the body of work
written mainly in scientific journals about diesel engine emissions
when using biodiesel fuels as opposed to conventional diesel fuels.
They point out that biodiesel fuels have an interesting potential to
reduce chemical emissions. However, the effect of biodiesel is
specific for each of the different pollutant species, and depends on
the type of engine, on the engine speed and load conditions, on the
ambient conditions, and on the origin and quality of the biodiesel.
In our previous work, a comparison of exhaust emissions produced
by different kinds of FAME (fatty acid methyl esters) derived from
used cooking oils and animal fats [8], the differences in the
observed species between each run suggested that the sources of
* Corresponding author. Tel.: þ886 3 9327495.
E-mail address: ypwu@niu.edu.tw (Y.P. Wu).
the collected waste oil affected the formation path of the trace
compounds during engine operations.
Hall and Howe [9] pointed out that energy management and
waste saving methods must become more widely researched and
discussed if the environmental, social and economic aspects of
sustainability are to be balanced. The production from seed oils by
transesterification into methyl esters is well established. The
feasibility of using waste as a source of energy will become more
important as fossil fuels shortage become a greater concern. Fish
oils also for consideration as a raw material for biodiesel
production.
Mrad et al. [10] produced biofuel from fish oil industrial residue
and ran this biofuel and its blend in a single cylinder, air-cooled,
direct injection diesel engine. The biofuel from fish oil industrial
residue was produced by catalytic cracking. Their results showed
that the brake thermal efficiency of the fish oil biofuel was slightly
higher than that of diesel. The biofuel and its blend emitted less HC,
CO, and particulate matter, but slightly more NOx than diesel. Mrad
et al. concluded that the fish oil industrial residue biofuel produced
by catalytic cracking is a viable substitute for diesel fuel.
Bhaskar et al. [11] studied the performance and emission char-
acteristics of fish oil methyl ester. Fish oil was extracted from
wastes of processed marine fish and refined through trans-
esterification. This biofuel and its blends were run on a 4.4 kW,
direct-injection, single-cylinder, naturally aspirated, air-cooled,
constant-speed diesel engine. Bhaskar et al. ran an engine on

http://dx.doi.org/10.1016/j.energy.2014.03.081
0360-5442/Ó 2014 Elsevier Ltd. All rights reserved.
44
pure fish oil methyl ester, diesel blends of 20%, 40%, 60%, and 80%
fish oil methyl ester, and diesel. Their results showed that the 20%
fish oil methyl ester blend yielded almost the same brake thermal
efficiency as diesel fuel, with lower unburned hydrocarbons, CO,
and soot emissions than diesel, but with higher NOx emissions.
They also pointed out that the fish oil methyl ester and its blends
can be used without any major modification in diesel engines.
Marine fish such as mackerel are important for coastal fisheries
in Taiwan. The annual production quantity of marine fisheries in
Taiwan amounted to 1167 thousand metric tons of catches in 2010
[12]. The amount of discarded parts of marine fish in the
manufacturing processes of various fish products is about 25% of
the fishery production [13]. Nearly 60,000 tons of mackerel is
produced in Suao, I-lan, Taiwan every year. In this study, mackerel
fish oil was collected from the wastewater of mackerel processing
plants, converted into mackerel biodiesel, and compared with
biodiesel made from plant oil. The converted mackerel biodiesel
was then used during an emissions test on a diesel engine running
on pure mackerel biodiesel, premium diesel, and a mixture of the
two. The formation of CO, CO2, NO, NOx, SO2, and particulate matter
was investigated.
2. Materials and methods
A total of 50 L of wastewater containing mackerel fish oil was
collected from the wastewater stream. The oil containing liquid
phase was collected from the upper level of the wastewater which
was allowed to settle overnight. The mackerel fish oil was then
obtained by boiling the liquid phase at 130  C for 30 min to remove
the water content. The mackerel biodiesel used in this study was
produced from the transesterification of recycled mackerel fish oil
with methanol (CH3OH, Malliuckrodt Baker Inc., USA) catalyzed by
sodium hydroxide (NaOH, Shimakyu, Osaka, Japan).
The reaction scheme of the transesterification of triacylglycerols
is shown in Fig. 1, and, for further reference, can also be found
elsewhere [8,14e16]. Transesterification is the process of reacting a
triglyceride with an excess of alcohol in the presence of NaOH as a
catalyst to produce fatty acid esters and glycerol. Triglycerides are
first reduced to diglycerides, then diglycerides are reduced to
monoglycerides, and finally the monoglycerides produce fatty acid
esters. For transesterification, 200 mL CH3OH plus the required
amount of NaOH was added for every liter of recycled mackerel fish
oil, and the reactions were carried out at 65  C. A titration was
performed to determine the amount of NaOH needed to neutralize
the free fatty acids in the recycled mackerel fish oil. The amount of
NaOH needed as catalyst for every liter of recycled mackerel fish oil
was determined as 5.2 g in this study. A total of 20L of recycled
mackerel fish oil was used to produce biodiesel. The water wash
process was performed by using a sprinkler which slowly sprinkled
water into the biodiesel container until there was an equal amount
of water and biodiesel in the container. The water/biodiesel
mixture was then agitated gently for 10 min, allowing the water to
settle out of the biodiesel. After the mixture had settled, the water
was drained out.
O
H2C O C R
O O
NaOH
HC O C R + 3 CH3OH 3 R C O CH3 +
O
H2C O C R
Triglyceride Methanol Fatty esters (Biodiesels)
Fig. 1. Transesterification of triglyceride with methanol in the presence of NaOH.
Y.P. Wu et al. / Energy 70 (2014) 43e48
A series of tests were performed to characterize the properties
of the produced biodiesel. Density at 15  C was determined by
using a glass hydrometer cylinder according to ASTM D 1298. Acid
value was analyzed by titration with 0.1 N KOH according to ASTM
D 664. The kinematic viscosity at 40  C was measured by a Ostwald
type BS/U-tube capillary viscometer according to ASTM D 445.
Flash point was measured by a manual PenskyeMartens closed cup
apparatus according to ASTM D 93. Gross heating value was
determined by a isoperibol oxygen bomb calorimeter (model 6200,
Parr Instrument Company, USA) according to ASTM D 240. The
iodine value was analyzed, based on the methods of the ASTM
D5554, by titration with 0.1 N sodium thiosulfate for the mixture of
tested fuel and chemical reagents. The chemical components in the
biodiesels were analyzed using a gas chromatograph-mass spec-
trometer (ThermoQuest Trace MS, GC/MS) with a 1.0 mm, 0.25 mm,
30 m DB-1 column (J & W Scientific). For comparison purpose, the
biodiesels used in the fuel testing in this study were fuels produced
from plant seed oils. The biodiesels used for comparison were:
sunflower seed oil methyl ester (SFM) and Jatropha curcas seed oil
methyl ester (JCB). In addition, pure diesel fuel (D) was also tested.
The experiments were carried out in a three-cylinder, four-
stroke-cycle 1331 c.c. marine diesel engine (YARMAR 3TN82). The
engine characteristics are cited in Table 1. The emission tests were
performed at an engine speed of 1800 rpm with engine loads of 0, 1,
2, 4, and 8 kW, respectively. Exhaust gas emissions of CO, CO2, and
NOx were simultaneously measured by an exhaust gas analyzer
(IMR 2088P). Exhaust gas emissions of SO2 were collected in a
sampling bag and analyzed by a fluorescent SO2 analyzer (API
100A). Particulate matter (PM) was withdrawn isokinetically from
the exhaust pipe and collected on a glass fiber filter according to the
procedure described in Method 1A, 40 CFR Part 60, U. S. EPA
(Environmental Protection Agency). The experimental value for
each gas or particle was the average taken from three
measurements.
3. Results and discussion
A total of 20 L of mackerel fish oil was used and converted into
biodiesel. After the transesterification process, the separation pro-
cess produced a nearly 90% volume ratio of methyl ester phase to a
10% volume ratio of glycerol phase, a result similar to that of our
previous study of recycled cooking oil biodiesel [8]. The chemical
compositions of biodiesels analyzed by the GC/MS are listed in
Table 2. The results show that the C18s (C18:0, C18:1, and C18:2) are
the major components contained in the plant seed produced bio-
diesels, SFM and JCB (Jatropha curcas biodiesel), in this study, while
MB (mackerel biodiesel) not only mainly contains C16:0 and C18s,
but contains higher carbon numbers and more unsaturated bonds,
C20:5 (11.6%) and C22:6 (16%). MB contains molecules with higher
carbon numbers, yielding a lower ratio of H/C at 1.79, while the
ratios of H/C of SFM and JCB were 1.84 and 1.85, respectively.
Table 3 compares the major properties of the three biodiesels
and a commercialized diesel fuel, premium diesel from China Pe-
troleum Corp. The acid values of the tested biodiesels were all
higher than D. Among these biodiesels, JCB has highest acid value
H2C OH Table 1
Engine specifications.
HC OH Type 4-cycle, water-cooled diesel
Combustion Direct injection
Aspiration Natural
H2C OH
Cylinders 3, in-line, vertical
Bore  stroke 82  84 mm
Glycerol
Piston displacement 1331 cc
Compression ratio 18.1 1
 Y.P. Wu et al. / Energy 70 (2014) 43e48 45

Table 2
Chemical components of biodiesels used in this study.

Component Name Formula MB SFM JCB

C13:0 Tridecanoic acid methyl ester C14H28O2 0.12 e e

C14:0 Tetradecanoic acid methyl ester C15H30O2 3.32 e e
C15:0 Pentadecanoic acid methyl ester C16H32O2 1.27 e 0.04
C16:0 Hexadecanoic acid methyl ester C17H34O2 14.9 6.92 10.6
C16:1 (Z)-9-hexadecenoic acid methyl ester C17H32O2 6.87 0.11 e
C17:0 Heptadecanoic acid methyl ester C18H36O2 e e 0.24
C17:1 (Z)-10-heptadecenoic acid methyl ester C18H34O2 e e 0.11
C17:2 (9Z,12Z)-9,12-octadecadienoic acid C18H32O2 1.96 e e
C18:0 Octadecanoic acid methyl ester C19H38O2 7.52 4.14 8.54
C18:1 (Z)-9-octadecenoic acid methyl ester C19H36O2 27.1 26.32 21.75
C18:2 (9Z,12Z)-octadeca-9,12-dienoic acid methyl ester C19H34O2 1.92 58.18 55.75
C19:1 10-Nonadecenoic acid methyl ester C20H38O2 0.29 e e
C20:0 Icosanoic acid methyl ester C21H42O2 e e 0.45
C20:1 (Z)-11-icosenoic acid methyl ester C21H40O2 5.06 0.94 0.152
C20:5 (5Z,8Z,11Z,14Z,17Z)-icosa-5,8,11,14,17-pentaenoic acid methyl ester C21H32O2 11.6 e e
C22:0 Docosanoic acid methyl ester C23H46O2 0.92 0.69 0.06
C22:6 (4E,7E,10E,13E,16E,19E)-docosa-4,7,10,13,16,19-hexaenoic acid methyl ester C23H34O2 16.0 e e

due to the fact that Jatropha curcas seed oil contains more free fatty CCO ¼ concentration of CO
acids. The acid value of MB was between the values of JCB and SFM.
The iodine value is an indicator of the number of unsaturated bonds The calculated combustion efficiencies of fuels tested in this
in oil. As shown in Table 3, MB has the highest iodine value, because study are shown in Fig. 2(c). As Fig. 2(c) shows, the fuels
it contains more unsaturated fatty acid methyl esters (Table 2
shows MB’s higher content of unsaturated fatty acid methyl es-
ters). As shown in Table 3, the biodiesels used in this study showed
higher densities and flash points, but lower gross heating values
than D. The biodiesels tested in this study also showed higher ki-
nematic viscosity values than the value of D.
The fuels used in the engine test were pure mackerel fish oil
methyl ester (MB100), a mixture of 20% (volume ratio) of MB and
80% of D (MB20), and pure premium diesel (D). The emission tests
were performed at an engine speed of 1800 rpm with engine loads
of 0, 1, 2, 4, and 8 kW, respectively. The emissions of CO, CO2, and
combustion efficiency for MB100, MB20, and D against engine load
are shown in Fig. 2. As shown in Fig. 2(a), CO formation increased
with increasing engine loads at lower engine loads for fuels con-
taining biodiesels. The CO emission decreased at higher engine
loads for engine runs on fuels containing biodiesels (MB100 and
MB20). For engine runs on D, the CO emission increased with
increasing engine load, however, at the highest load (8 kW), CO
emission was not detected. Fig. 2(b) shows that CO2 concentration
increased with increasing engine loads for all fuels. In order to
combine the results of CO and CO2 formation, the combustion ef-
ficiency was computed as followed:

CCO2
Combustion efficiency ¼ h ¼  100% (1)
CCO2 þ CCO

where CCO2 ¼ concentration of CO2

Table 3
Major properties of premium diesel and biodiesel used in this study.

MB SFM JCB D

Acid value 0.359 0.145 3.380 0.034 ASTM D 664

(mg KOH/g)
Iodine value 139.93 137.81 93.29 12.74 ASTM D5554
(g I2/100 g)
Kinematic viscosity 4.700 5.251 3.686 3.110 ASTM D 445
at 40  C (mm2/s)
Density (g/cm3) 0.893 0.897 0.863 0.842 ASTM D 1298
at 15  C
Gross heating value 9388 9464 9473 10592 ASTM D 240
(cal/g)
 Fig. 2. Comparison of (a) CO, (b) CO2, and (c) combustion efficiency from MB100,
Flash point ( C) 173 172 152 70 ASTM D 93
MB20, and D fuels at 1800 rpm under varied loads.
46 Y.P. Wu et al. / Energy 70 (2014) 43e48

500 4000
0kw
0kw 1kw
(a)
400 1kw 2kw
2kw 3000
4kw
4kw 8kw

PM(mg/m )
3
NO(ppm)

300 8kw
2000
200

1000
100

0 0
B100 B20 D B100 B20 D
700
Fig. 5. Comparison of PM emissions from MB100, MB20, and D fuels at 1800 rpm
0kw
600 (b) under varied loads.
1kw
2kw
500
4kw
NOx (ppm)

400
8kw the other fuels for the tested engine loads, and PM concentration
increased with increase engine loads for all tested fuels.
300 As mentioned in the discussion of the results shown in Table 2,
MB has a much higher amount of high carbon-number products
200
compared with the biodiesel which converted from vegetable oil,
100 for example, JCB in this study. This study also compares the

0
B100 B20 D 100
(a) MB100
Fig. 3. Comparison of (a) NO and (b) NOx emissions from MB100, MB20, and D fuels at JCB
80
1800 rpm under varied loads. D
CO(ppm)

60
containing diesel (D and MB20) exhibit better combustion
efficiency. 40
The emissions of NO and NOx against engine load from various
fuels are compared in Fig. 3. Fig. 3(a) shows that NO increased with 20
increased engine loads for all tested fuels, while MB100 and MB20
produced less NO at lower engine loads (0 kWw4 kW). Fig. 3(b) 0
shows that NOx concentration also increased with increasing en- 0kw 1kw 2kw 4kw 8kw

gine loads. Fig. 3(b) also shows that fuel containing more biodiesel, Engine load
6
emitted more NOx. (b)
As shown in Fig. 4, MB100 produced the lowest concentration of 5
SO2 for all engine loads, while D produced the highest concentra-
tion. For all tested fuels, SO2 formation increased with increased 4
CO2(%)

engine load. However, SO2 emission profiles from MB100, MB20, MB100
3 JCB
and D are similar to each other for each engine load. As the engine D
used in this study was a used one, there may have been a residue of 2
sulfur species left in the engine from when the engine was used in
the past, which then formed SO2 during the biodiesel runs. 1
The PM concentrations from MB100, MB20, and D fuels are
0
compared in Fig. 5. MB100 yielded higher PM concentrations than
0kw 1kw 2kw 4kw 8kw

Engine load
100.0
800 (c) MB100
0kw
JCB
1kw
D
2kw 99.5
600
CO2/(CO+CO2)

4kw
8kw
SO2(ppb)

99.0
400

98.5
200

98.0
0kw 1kw 2kw 4kw 8kw
0
B100 B20 D Engine load

Fig. 4. Comparison of SO2 emissions from MB100, MB20, and D fuels at 1800 rpm Fig. 6. Comparison of (a) CO, (b) CO2, and (c) combustion efficiency from engine runs
under varied loads. on MB100, JCB, and D at 1800 rpm under varied loads.
 Y.P. Wu et al. / Energy 70 (2014) 43e48 47

500 efficiency for these three fuels under varied engine loads. As shown
(a)
in Fig. 6(b), engine runs on JCB produced lower CO2 emissions but
400 showed the poorest combustion efficiency among the three test
fuels.
Fig. 7 presents the NO and NOx emissions from engine runs on
NO(ppm)

300
MB100, JCB, and D under varied engine loads. As shown in Fig. 7(a)
MB100 and (b), the emitted concentrations of NO and NOx for the three
200
JCB fuels increased with increased engine load loads. Engine runs on
D JCB produced higher NO and NOx than engine runs on MB100. Fig. 8
100
compares the PM emission for engine runs on MB100, JCB, and D
under varied engine loads. As shown in this figure, when the engine
0 ran on JCB, it produced the highest level of PM while engine was
0kw 1kw 2kw 4kw 8kw
free-load (0 kW), and other loads yielded a steady but lower
Engine load amount of PM emission. As engine loads, engine runs on MB100
800 produced higher PM concentrations.
(b)

600
4. Conclusions
NOx(ppm)

MB100 As compared on the fuel properties, MB has a higher iodine

400 JCB
D
200
0
0kw 1kw 2kw 4kw
Engine load
Fig. 7. Comparison of (a) NO and (b) NOx emissions from engine runs on MB100, JCB,
and D at 1800 rpm under varied loads.
emissions from engine runs on pure MB (MB100), JCB, and D at an
engine speed of 1800 rpm under varied engine loads. Fig. 6 com-
pares the CO emission, CO2 emission, and combustion efficiency for
engine runs on MB100, JCB, and D at 0, 1, 2, 4, and 8 kW power
loads. As shown in Fig. 6(a), when run on biodiesels (MB100 and
JCB), the engine emitted more CO than when it was run on D under
all engine loads. Also, the engine runs on MB100 produced lower
CO emissions than the engine runs on JCB. Fig. 6(b) shows that
engine runs on JCB yielded lower CO2 emissions than engine runs
on MB100 and D for most of the engine loads. Using the same
analysis method as Fig. 2(c), Fig. 6(c) also compares the combustion
value, dynamic viscosity, density, and flash point than D, but a
lower heat value than D. The analysis results show MB contains
higher amounts of unsaturated fatty acid, such as C20:5 (11.6 wt%)
and C22:6 (16.0wt%) polyunsaturated fatty acids, so it has a higher
iodine value than other biodiesels. During the engine emission test,
CO formation increased with increasing engine loads at lower en-
8kw
gine loads when run on fuels containing biodiesels. CO emission
decreased at higher engine loads for engine runs on fuels con-
taining biodiesels. CO2 concentration increased with increasing
engine loads for all fuels and the fuels containing diesel (D and
MB20) exhibited better combustion efficiency. The concentration of
NO and NOx increased with increasing engine loads for all tested
fuels. MB100 and MB20 produced less NO at lower engine loads
(0 kWe4 kW) but it was also observed that the more biodiesel a
fuel contains, the more NOx it emits. For all tested fuels, SO2 for-
mation increased with increased engine loads and MB100 pro-
duced the lowest concentration of SO2 for all engine loads. PM
concentration increased with increased engine loads for all tested
fuels, and MB100 yielded higher PM concentrations than the other
fuels. Engine runs on MB100 yielded a higher combustion efficiency
and lower NOx emission, but a higher PM concentration than en-
gine runs on JCB.
Acknowledgments

4000 The authors wish to express their appreciation for the funding
MB100 (NSC 100-2221-E-197-027) from the National Science Council of
JCB Taiwan, R.O.C.
D
3000
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PM(mg/m )
3

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