Energy 38 (2012) 151e156

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

Improving biodiesel yields from waste cooking oil by using sodium methoxide
and a microwave heating system
Kang-Shin Chen, Yuan-Chung Lin*, Kuo-Hsiang Hsu, Hsin-Kai Wang
Institute of Environmental Engineering, National Sun Yat-sen University, Kaohsiung 804, Taiwan

a r t i c l e i n f o

a b s t r a c t

Article history:
Received 6 May 2011
Received in revised form
3 October 2011
Accepted 18 December 2011
Available online 10 January 2012

The major obstacle to biodiesel commercialization is the high cost of biodiesel. Biodiesel made from
waste cooking oil is an economical source that can effectively reduce raw material cost. Although using
a microwave heating system to improve the yields of waste-cooking-oil biodiesel has received little
attention in the literature, experimental results indicate that it outperforms conventional heating, with
the best performances found with 0.75 wt% sodium hydroxide (NaOH) and 0.75 wt% sodium methoxide
(CH3ONa) catalysts, respectively. The biodiesel yields produced with CH3ONa catalyst are higher than
those produced with NaOH catalyst. An increase in the reaction time from 1 to 3 min signicantly
increases the yield, which decreases with a further increase to 6 min. A methanol-to-oil molar ratio of 6
is suitable for the synthesis of biodiesel. The biodiesel yields increase with increasing reaction power.
However, the microwave output must not be too high as it may damage the organic molecules. The
optimal reaction conditions are 0.75 wt% CH3ONa catalyst, a methanol-to-oil molar ratio of 6, a reaction
time of 3 min, and a microwave power of 750 W.
Crown Copyright 2011 Published by Elsevier Ltd. All rights reserved.

Keywords:
Waste cooking oil
Microwave
Sodium methoxide
Biodiesel yields
Transesterication

1. Introduction
The development of biodiesel is being driven by the need to
reduce emissions from diesel engines without modifying them.
Biodiesel can be produced from animal fats or vegetable oils with
methanol or ethanol as the catalyst via a transesterication reaction. The main advantages of using biodiesel are renewability,
lower exhaust gas emissions, and biodegradability. Furthermore,
biodiesel does not contribute to a net rise in carbon dioxide in the
atmosphere and consequently to the greenhouse effect [1]. Several
states in the US are currently pushing for a greater use of biodiesel,
and the US federal government is using a tax credit as an incentive
to aid its development [2]. When biodiesel is used as alternative
fuel in diesel engines, it can reduce emissions of hydrocarbons
(HCs), carbon monoxide (CO), sulfur oxide (SO2), polycyclic
aromatic hydrocarbons (PAHs), and polychlorinated dibenzo-pdioxin/dibenzofurans (PCDD/Fs) [3e15]. Although there have
been mixed results for reductions of particulate matter (PM) in the
literature [16], most studies (>90%) found a decrease in emissions
of PM when using biodiesel. Although previous studies indicated
that emissions of nitrogen oxides (NOx) from biodiesel showed an

* Corresponding author. Tel.: 886 7 5252000x4412; fax: 886 7 5254412.

E-mail addresses: yclin@faculty.nsysu.edu.tw, yuanchung.lin@gmail.com
(Y.-C. Lin).

increase in brake-specic NOx emissions of up to 15% [17e21], the

problem of high NOx emissions from biodiesel-diesel engines can
be mitigated by the use of low-temperature combustion or selective catalytic reduction [22e27].
The major obstacle to biodiesel commercialization is its high
cost, which is approximately 1.5 times higher than that of petroleum diesel fuel due to the cost of vegetable oil [28e31]. Biodiesel
made from waste cooking oil can be used to effectively reduce the
raw material cost as well as solve the problem of waste oil disposal
[30,32e37]. Lapuerta et al. (2008) tested biodiesel from waste
cooking oils in a direct-injection (DI) diesel commercial engine
under a set of engine operating conditions corresponding to typical
road conditions. Compared to conventional low-sulfur diesel fuel,
a sharp decrease was observed in both smoke and PM emissions
when the biodiesel concentration was increased [16]. Di et al.
(2009) investigated a four-cylinder DI diesel engine using ultralow-sulfur diesel, biodiesel from waste cooking oil, and their
blends, and examined emissions under ve engine loads at an
engine speed of 1800 rev min
1. They found that HC and CO
emissions decreased whereas NOx and NO2 emissions increased
with increasing biodiesel fraction. For unregulated gaseous emissions, the emissions of formaldehyde, 1,3-butadiene, toluene, and
xylene decreased with increasing biodiesel concentration in blends,
whereas emissions of acetaldehyde and benzene increased [38].
Ozsezen et al. (2009) investigated a DI diesel engine fueled with
biodiesels from waste cooking oil operating at a constant engine

0360-5442/$ e see front matter Crown Copyright 2011 Published by Elsevier Ltd. All rights reserved.
doi:10.1016/j.energy.2011.12.020

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K.-S. Chen et al. / Energy 38 (2012) 151e156

speed (1500 rpm) under the full load condition of the engine, and
found that biodiesels had reduced emissions of CO and HCs, as well
as smoke opacity, but had increased NOx emissions compared to
those of petroleum-based diesel fuel [39].
Another way to reduce the cost of biodiesel is to increase biodiesel yields. Reaction temperature, reaction time, catalyst amount,
and the alcohol-to-oil ratio are important parameters in biodiesel
production. Catalytic reactions can use alkali catalysts, acid catalysts, or enzymatic transesterication, of which the rst achieves
the best results. Biodiesel can be produced at a lower temperature
and shorter reaction time with an alkali catalyst compared to those
required for an acid catalyst [40e43]. The conventional heating of
a sample has a few signicant drawbacks, such as heterogenic
heating of the surface, limitations dependent on the thermal
conductivity of materials, specic heat, and density when
compared to microwave irradiation [44,45], and thus many
research groups have recently focused on the latter approach.
Previous studies indicated that microwave-assisted chemical
reactions are better than those obtained using other synthetic
techniques and that microwave heating systems can increase the
reaction rate, product yields, and purity of products [46e58].
Leadbeater and Stencel (2006) concluded that a 1:6 triolein/
methanol ratio, 5 wt% KOH, and a 1 min reaction time are the
optimal reaction parameters for 25-W microwave heating,
achieving a biodiesel yield of 98% [50]. They carried out the
microwave-assisted transesterication of cottonseed oil in the
presence of methanol and potassium hydroxide (KOH), and found
that a 7 min reaction time, a 333 K temperature, and a 1.5%
catalysteoil ratio were the optimal reaction parameters for
microwave heating. Similar results were found for conventional
heating, but with a 30 min of reaction time; the biodiesel yield and
purity were in the ranges of 89.5e92.7% and 78.9e99.8%, respectively [52]. Rapeseed oil was converted to biodiesel via transesterication using microwave heating, with a yield of 88.3e93.7%
[59]. Lertsathapornsuk et al. (2008) found that the continuous
conversion of waste frying palm oil to ethyl ester was over 97% with
an ethanol-to-oil molar ratio of 12:1, 3.0% NaOH (in ethanol), a 30 s
residence time, and a microwave power of 800 W [60]. Suppalakpanya et al. (2010a) concluded that the optimal reaction
parameters for the transesterication process aided by microwave
heating are a molar ratio of palm oil to ethanol of 1:8.5, 1.5 wt%
KOH/oil, a reaction time of 5 min, and a microwave power of 70 W
[61]. They also concluded that a molar ratio of free fatty acid (FFA)
to ethanol of 1:24 with 4 wt% H2SO4/FFA, a microwave power of
70 W, and a reaction time of 60 min are the optimal reaction
parameters for the transesterication process aided by microwave
heating [62]. Furthermore, the microwave heating method has
been shown to be more energy-efcient than a conventional
heating method for the transesterication reaction [51,63].
Although there has been a lot of research into improving the yields
of biodiesel from waste cooking oil and into the use of microwave
heating systems for improving the yield of biodiesel in general, the
topic of increasing the yields of waste-cooking-oil biodiesel using
a microwave heating system and CH3ONa has seldom been
addressed. This study thus investigates the yields of biodiesel made
from waste cooking oil with a microwave heating system. Additionally, the effects of catalyst type, amount of catalyst, reaction time,
molar ratio of methanol to oil, and microwave power are investigated.

was less than 2 mg of KOH g
1. Methanol, NaOH, and CH3ONa were
high-performance liquid chromatography (HPLC) grade. The
experimental setup is shown in Fig. 1. A microwave synthesis
reactor (NN-S235, Panasonic Co., Ltd., Taiwan), equipped with
a mechanical stirrer and a condenser (LC-10, Hi-point Co., Ltd,
Taiwan) was used for microwave reactions. The stirrer was operated at 600 rpm with a magnetic nucleus. Various catalysts
(CH3ONa and NaOH), reaction times (1e6 min), methanol-to-oil
molar ratios (3, 6, 9, 12, 15), and reaction powers (200, 350, 500,
650, 750 W) were tested. A conventional heating system (HTS1003, Laboratory & Medical Supplies Co., Ltd., Japan) equipped with
a mechanical stirrer and a condenser (LC-10, Hi-point Co., Ltd,
Taiwan) was used for the conventional heating reactions.
2.2. Separation and purication
If methyl ester content is higher than 90%, we though that
transestrication has occurred. After the end of the transesterication process, the mixture was separated by the centrifuge
(CN-1040; Hsiangtai, Taiwan) under 2000 rpm for 10 min resulting
in the formation of an upper phase consisting of methyl esters and
a lower phase containing glycerin. Excess methanol in the methyl
ester phase was evaporated by heater at 80  C. Then catalyst was
removed by adding silica gel and the impurities were removed by
water. Then biodiesel was obtained.
2.3. Product analysis
The analytic method of methyl ester content in this study followed Taiwan CNS15051 (Chinese National Standards). A GC (gas
chromatography; GC-6890, Agilent, USA) system equipped with
a FID (ame ionization detector) was used to determine methyl
ester content. The temperature of the injection port and detector
were set at 250 and 260  C, respectively. The oven temperature was
programmed to initiate at 50  C for 2min, then the temperature was
raised to 150  C at a rate of 10  C min
1, held there for 2 min. Then
the temperature was raised to 200  C at a rate of 4  C min
1, held
there for 4 min, and nally increased to 230  C at a rate of
1  C min
1 and held there for 5 min. The injection volume was 1 mL
in the split-less injection mode. The capillary column was an HPINNOWAX 19091N-133, 30 m  0.25 mm I.D, and the lm

2. Experimental section
2.1. Transesterication procedures
The waste cooking oil used in this study was obtained from
a fast-food restaurant in Taiwan. The acid value of waste cooking oil

Fig. 1. Experimental setup.

K.-S. Chen et al. / Energy 38 (2012) 151e156

153

thickness was 0.25 mm. The spilled rate was 1:60. The velocity of
carrier gas (He) was set at 19 cm s
1. Methyl ester content is dened
as follow

3.2. Effects of catalyst type and amounts of catalyst on the yield of

biodiesel under a microwave system

P
A
AEI CEI  VEI
C

 100%
AEI
m

Experiments were carried out using different catalysts in order

to investigate their inuence on yield. The microwave system was
operated with a reaction time of 6 min, a microwave power of
750 W, and a methanol-to-oil molar ratio of 6. Sodium hydroxide
(NaOH) and sodium methoxide (CH3ONa) were used as the catalysts. The fractions of the catalysts were 0.50, 0.75, 1.00, 1.25, and
1.50 wt%, respectively. As shown in Fig. 2, the yields of biodiesel
were 90.5%, 96.2%, 95.6%, 89.0%, and 83.5% for 0.50, 0.75, 1.00, 1.25,
and 1.50 wt% NaOH catalyst, respectively. The yield increased with
increasing amount of catalyst for catalyst concentrations of 0.50 wt
% to 0.75 wt%, and then decreased from 0.75 wt% to 1.50 wt%. The
best yield was obtained with 0.75 wt% NaOH. Similar results were
found for the CH3ONa catalyst, as shown in Fig. 3. The biodiesel
yields were 96.4%, 97.9%, 97.1%, 95.2%, and 90.8% for 0.50, 0.75, 1.00,
1.25, and 1.50 wt% CH3ONa catalyst, respectively. These results
indicate that although excess catalyst might increase the biodiesel
yield, the amount of glycerin produced is also increased due to
saponication, causing a reduction of biodiesel yields. A further
increase in catalyst concentration did not increase the conversion
and led to extra costs due to its removal from the reaction medium
at the end of the process [6,67,68]. Furthermore, Dorado et al.
concluded that the addition of an excessive amount of alkali catalyst gives rise to the formation of an emulsion, which increases
viscosity and leads to the formation of gels. These hinder glycerin
separation, and as a result there is a dilution of the ethyl esters; the
apparent ester yield diminishes [6]. In this study, the best yields
were achieved with 0.75 wt% NaOH and 0.75 wt% CH3ONa for waste
cooking oil. The yields of biodiesel with CH3ONa catalyst were
higher than those for NaOH catalyst. Similarly, Rashid et al. found
that CH3ONa catalyst was the most efcient catalyst tested, followed by NaOH, CH3OK, and KOH [69]. The lowest ester yield was
obtained with hydroxide catalysts, because upon mixing of
sodium- and potassium-hydroxides with methanol, a small amount
of water is often produced, which gives rise to the hydrolysis of
some of the produced esters, resulting in soap formation, thus
leading to lower ester yields [69,70]. Azcan and Danisman (2008)
found that the yields of corn biodiesel with 1 wt% NaOH catalyst
(92.7%) were higher than those with 1 wt% KOH catalyst (90.9%)
with a methanol-to-oil molar ratio of 6 and a reaction time of 3 min
[59]. Leadbeater and Stencel (2006) found that the yields of corn
biodiesel increased with increasing amounts of KOH catalyst,
achieving yields of 93.0%, 96.0%, and 97.0% for 1 wt%, 5 wt%, and
10 wt% KOH catalyst, respectively [50].

P
where C: total fatty acid methyl ester content (mg mg
1); A : sum
of peak area of fatty acid methyl ester from C14 to C24:1; AEI: peak
area of internal standard, palmitic acid methyl ester; CEI: Concentration of palmitic acid methyl ester (mg mL
1); VEI: Volume of
palmitic acid methyl ester (mL
1); m: mass of input biodiesel (g).
Then, biodiesel yield was calculated relative to the initial amount of
waste cooking oil by weight. Similar studies were found
[58,59,61,62].

3. Results and discussion

3.1. Comparison of yield for microwave and conventional heating
The conventional heating was carried out at 65  C, with
a methanol-to-oil molar ratio of 6 and 0.75 wt% CH3ONa. The
microwave heating was carried out at 750 W, with a methanol-tooil molar ratio of 6 and 0.75 wt% CH3ONa. As shown in Table 1, the
biodiesel yield increased with reaction time for conventional
heating. The maximum yield of biodiesel made from waste
cooking oil under conventional heating was 96.6%. For the
microwave system, the biodiesel yield increased with reaction
time from 1 to 3 min, but then decreased from 3 to 5 min. The
maximum yield of biodiesel made from waste cooking oil was
97.9%. The above results indicate that microwave heating has
a signicantly shorter reaction time and a higher yield of biodiesel
compared to those for convention heating. The highly effective
transesterication in the microwave heating system is attributed
to the direct adsorption of the radiation by the OH group of the
reactant. The OH group is directly excited by the microwave
radiation, causing the local temperature around the OH group to
be much higher than that of its environment, far exceeding the
activation energy needed for transesterication [60]. Methanol is
a good microwave radiation absorption material as its dipole
reorients, which can destroy the two-tier structure of the interface
of methanol and oil [46,57], improving the solubility of methanol
and oil and thus enhancing the transesterication reaction. The
above experimental results may be attributed to microwave
localized temperature and pressure, and the microwave absorbing
character to penetrate materials and to produce a volumetrically
distributed heat source [58,60,64e66]. Microwave heating thus
outperforms conventional heating, offering a fast, easy route for
biodiesel production.

110
Waste cooking oil

Method

Reaction time (min)

Yield (%)

Conventional heating

30
45
60
75
90
1
2
3
4
5

86.3
91.5
93.4
94.2
96.6
94.6
95.8
97.9
96.6
92.7

Microwave heating

Yield (%)

105
Table 1
Comparison of biodiesel yields from waste cooking oil under conventional heating
and microwave heating systems.

100

96.2

96.1

95
90.8
90

89.1
83.5

85
80

0.50

0.75
1.00
1.25
Amount of NaOH catalyst (wt%)

1.50

Fig. 2. Effects of the amount of NaOH catalyst on the yield of biodiesel under
a microwave system.

154

K.-S. Chen et al. / Energy 38 (2012) 151e156

120

110

96.4

97.9

95.2

95

90.8

90

0.50

40

0.75
1.00
1.25
1.50
Amount of CH3ONa catalyst (wt%)

95.8

91.6

86.8

80

60

85
80

97.9

100

97.1

Yield (%)

Yield (%)

105
100

Waste cooking oil

Waste cooking oil

50.2

6
9
12
Methanol : Oil (mol/mol)

15

Fig. 3. Effects of the amount of CH3ONa catalyst on the yield of biodiesel under
a microwave system.

Fig. 5. Effects of microwave power on yield under a microwave system with CH3ONa
catalyst.

3.3. Effects of reaction time

Theoretically, each mole of biodiesel is made from 1 mol of methanol and one-third of a mole of triglyceride in the transesterication reaction. However, in practice a higher molar ratio is
needed for the reaction, because the transesterication reaction is
reversible. Furthermore, biodiesel and glycerol are miscible due to
the use of excess methanol [57,71]. In addition, methanol is a strong
medium for absorbing microwaves, and thus the excess methanol
may absorb microwave energy and reduce the microwave power.
Consequently, the molar ratio of methanol to oil should not be
excessive, and 6 was considered the most suitable level in this
experimental system.

Experiments were carried out with 0.75 wt% CH3ONa catalyst,

a microwave power of 750 W, a methanol-to-oil molar ratio of 6,
and various reaction times (1, 2, 3, 4, 5, and 6 min) to investigate the
effects of reaction time on yield. As shown in Fig. 4, the yields of
waste cooking oil biodiesel were 94.6%, 95.8%, 97.9%, 96.6%, 92.7%,
and 91.8% for reaction times of 1, 2, 3, 4, 5, and 6 min, respectively.
An increase in reaction time from 1 to 3 min caused a signicant
increase in biodiesel yield, which then decreased with a further
increase to 6 min. These results may be attributed to the incomplete
transesterication reaction between methanol and oil in the
shorter reaction; the longer reaction had a higher reaction
temperature, resulting in greater solubility of glycerine. Similarly,
Azcan and Danisman (2008) found that the yields of rapeseed oil
biodiesel were 92.2%, 92.7%, and 92.0% for reaction times of 1, 3, and
5 min, respectively, with 1.0 wt% NaOH, a methanol-to-oil molar
ratio of 6, and a microwave power of 1200 W [59].
3.4. Effects of molar ratio of methanol to oil
Experiments were carried out with 0.75 wt% CH3ONa catalyst,
a microwave power of 750 W, a reaction time of 3 min, and various
methanol-to-oil molar ratios (3, 6, 9, 12, and 15) to investigate the
inuence of this ratio on yield. As shown in Fig. 5, an increase in the
molar ratio from 3 to 6 caused a signicant increase in yield from
50.2% to 97.9%; when the molar ratio was further increased to 12,
the yield decreased from 97.9% to 86.8%. Therefore, a molar ratio of
6 is most suitable for the synthesis of waste-cooking-oil biodiesel.

3.5. Effects of microwave power

Experiments were carried out with a 0.75 wt% CH3ONa catalyst,
a reaction time of 3 min, a methanol-to-oil molar ratio of 6, and
various microwave powers (200, 350, 500, 650, and 750 W) to
investigate the effect of microwave power on yield. As shown in
Fig. 6, the yields of waste-cooking-oil biodiesel were 89.4%, 92.8%,
95.8%, 96.5%, and 97.7% for microwave powers of 200, 350, 500, 650,
and 750 W, respectively. The yields of biodiesel increased with
increasing power. Similar results were found in earlier works
[55,63]. For example, Groisman and Gedanken (2008) also
concluded that the efciency of a continuous ow system is lower
than that of laboratory batch ovens at various microwave intensities [55]. However, the microwave output must not be too high, as it
may cause damage to organic molecules such as triglycerides,
which are cleaved to FFA [42]. In addition, Patil et al. (2010) found
that the energy required for the microwave heating method is 23

110

110

Waste cooking oil

100
95

Waste cooking oil

105

94.6

95.8

97.9

100

96.6
92.7

91.8

90
85

Yield (%)

Yield (%)

105

95

89.4

96.5

96.5

500
Power (W)

650

97.9

93.2

90
85

80
1

3
4
Time (min)

Fig. 4. Effects of reaction time on yield under a microwave system with CH3ONa
catalyst.

80

200

350

750

Fig. 6. Effects of molar ratio of methanol to oil on yield under a microwave system
with CH3ONa catalyst.

K.-S. Chen et al. / Energy 38 (2012) 151e156

times lower than that required for the conventional method. These
results suggest that appropriate power dissipation control will
result in effective use of microwave energy and reduce energy
requirements [63].

4. Conclusion
Experimental results indicate that the reaction time was
reduced signicantly and yield of biodiesel was improved due to
the use of microwave heating. Microwave heating can achieve
better performances compared with conventional heating. Biodiesel yields increased with increasing catalyst amount from
0.50 wt% to 0.75 wt% then decreased with increasing catalyst
amount from 0.75 wt% to 1.50 wt%. The best performances were
both under 0.75 wt% NaOH and 0.75 wt% CH3ONa for waste cooking
oil. The yields of biodiesel under CH3ONa catalyst were higher than
those under NaOH catalyst. Although excess catalyst might increase
the biodiesel yield, glycerin increased as well due to saponication
causing the reduction of biodiesel yields. An increase of reaction
time from 1 to 3 min caused a signicant increase in biodiesel yield,
which decrease with a further increase to 6 min. The above results
may be attributed to the incomplete transesterication reaction
between methanol and oil in a shorter reaction, whereas a longer
reaction had a higher reaction temperature, resulting in higher
solubility of glycerine. An increase in the methanol-to-oil molar
ratio from 3 to 6 caused a signicant increase in biodiesel yield,
with then decreased with a further increase to 12. A methanol-tooil molar ratio of 6 is thus suitable for the synthesis of biodiesel. The
biodiesel yield also increased with increasing reaction power,
although the microwave output must not be too high as it may
damage the organic molecules. The optimal reaction conditions are
0.75 wt% CH3ONa catalyst, a methanol-to-oil molar ratio of 6,
a reaction time of 3 min, and a microwave power of 750 W.
Acknowledgments
This research was supported by the National Science Council of
Taiwan under grant NSC 98-2221-E-110-017. The authors gratefully
acknowledge the contributions of Professor Houng-Yung Chens
group, Institute of Marine Biology, National Sun Yat-sen University,
for helping with the yield analysis.
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