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Performance of Tubular Reactor for Producing Biodiesel by Transesterification

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 Prosiding Seminar Nasional Teknik Kimia Indonesia 2015 ISSN
Sustainable Energy and Mineral Processing for National Competitiveness
Yogyakarta, 12-13 Oktober 2015

Performance of Tubular Reactor for Producing Biodiesel by

Transesterification Reaction
Dayu Dian Perwatasari and Tirto Prakoso*

Chemical Engineering Study Program, Faculty of Industrial Technology,

Institut Teknologi Bandung, Jalan Ganesha 10, Bandung, Indonesia
*Corresponding Author : tirto@che.itb.ac.id

Abstract
Biodiesel of fatty acid methyl ester (FAME) is a renewable alternative fuel that can be produced from
vegetable oils or animal fats. Transesterification is the most common method for producing biodiesel
which is a reaction between lipid and alcohol in the presence of a catalyst to form esters and glycerol.
This process is usually done in batches.
This study is focused to overcome the weaknesses of the batch operating system by designing
continuous reactors manifold pipe reactor using a plug flow reactor (PFR) as the basis for the initial
design, as a vessel to carry out the transesterification reaction with RBDPO (Refined Bleached
Deodorized Palm Oil) as raw materials. In addition, the influence of operating conditions consisting
of reactor length, total flow rate of reactant, molar ratio of methanol to oil, reaction temperature and
catalyst concentration on the conversion was investigated as well.
The results showed that continuous pipe reactor designed and operated at the optimum condition
which consists of the total reactant flow rate 9.83 ml / min, methanol to oil molar ratio of 12: 1,
reaction temperature 63 ° C, and the catalyst concentration 2.25 % -b oil on the length of the reactor
300, 420, and 1020 cm able to produce a reaction with high conversion ie a product with ester levels
in the range of 95-97% for biodiesel shortly after leaving the reactor and in the range of 99.4-99.5%
for biodiesel experiencing purification step. Quality of biodiesel after purification also meet quality
standards ISO 7182: 2012 in the value of kinematic viscosity and density at 40 ° C which is in the
range of 2,3-6,0 mm2/s for viscosity and 850-890 kg/m3 for density.
Keywords : biodiesel, transesterification, continuous reactor, tubular reactor

1. Introduction
Biodiesel is defined as fuel that is composed of long-chain monoalkyl esters derived from vegetable
oils or animal fats (Okullo et al., 2012). This renewable alternative fuels show the similar nature and
characteristics to conventional diesel (petrodiesel). Because of this similarity, biodiesel can be used as
a substitute for diesel fuel or more commonly used as a fuel mixer which can be used in various
compression ignition engines without much modification (Lee et al., 2011).
In Indonesia, the use of biodiesel as a fuel mixture are also supported through the minister of Energy
and Mineral Resources Regulation No. 25 Year 2013 which is targeted on January 2016, as much as
20% biodiesel should be in the mixture of petrodiesel for use in the transportation sector and as much
as 30% biodiesel should be in the mixture of petrodiesel for use in the power generation sector.
Moreover, the use of biodiesel as a fuel mixture also has many advantages. The uses of biodiesel also
potentially reduce countries dependence on imported diesel fuel. Meanwhile, in terms of the
environment, biodiesel is CO2 neutral, which means burning biodiesel, does not add to the net CO2
concentration in the air so it does not contribute to global warming. Biodiesel is also biodegradable,
contains no sulfur, and has a better lubrication effect than petrodiesel (Kiss et al., 2008). Another
advantage is the value of cetane number and flash point of biodiesel is higher than petrodiesel so it can
provide a better engine performance as well as safer condition in terms of storage and transportation
than petrodiesel (Kaewta, 2008).
Currently biodiesel is generally produce through transesterification method which is the reaction
between triglycerides and short-chain alcohols with the aid of the presence of a catalyst to form esters
and glycerol. This method is generally carried out in a batch system. Phermpeansin (2011) found that
 Prosiding Seminar Nasional Teknik Kimia Indonesia 2015 ISSN
Sustainable Energy and Mineral Processing for National Competitiveness
Yogyakarta, 12-13 Oktober 2015

batch system has some disadvantages such as require a large reactor size, require a large space,
consume large amounts of energy for the purpose of stirring, and require a quite high fee for its
operations. In addition, the quality of the products produced in each batch of the reactor is sometimes
not uniform.
The study of the biodiesel production process through transesterification reaction using a continuous
system performed as an attempt to find ways to overcome the weaknesses owned by the batch
operating system. The purpose of converting batch system into a continuous system is to reduce the
residence time and volume of the reactor in order to improve the economic value of the process that
took place.
The reactor built in this research manifold continuous tubular reactor using a plug flow reactor type
(PFR) as the basis for the initial design. According to Foon et al. (2004) transesterification reaction is
classified into a second-order non elementary reactions so that the use of PFR type reactor will be
more efficient in terms of reactor volume required to obtain the same degree of conversion compared
to the use of CSTR type reactor.
Raw materials used in this research is palm oil which has undergone a purification process and known
as Refined Bleached Deodorized Palm Oil (RBDPO). The selection of palm oil as a raw material
process based on its very high availability in Indonesia. Indonesia is the world's largest CPO producer.
Indonesia's CPO production is increasing from year to year and reached the amount of 23,521,071
tons in 2012.
The use of continuous operating system in the biodiesel production process has become very
important as an effort to get the process more efficient and economic. Therefore, study about the
reactor dimensions and the optimum process conditions suitable to be used in the continuous reactor is
needed to produce biodiesel with a high conversion rate and meet the prevailing quality standards.

2. Methodology
Research steps undertaken include the design of continuous reactor, the production of biodiesel on a
wide variety of operating conditions, the analysis of biodiesel produced, and the determination of the
optimum operating conditions.
2.1 Equipment and Materials
The raw materials used for biodiesel production is Refined Bleached Deodorized Palm Oil (RBDPO)
representing triglycerides; methanol; and KOH as homogeneous base catalyst. The equipment used in
this research is a set of continuous tubular reactor for the transesterification reaction with ± 4 mm
internal diameter and has three output taps, each of which represents a reactor length of 300, 420, and
1020 cm. The reactor is designed to form a spiral structure and placed submerged in a water bath as a
tool to control the reaction temperature. Other equipment used is the equipment for analysis consisted
of burette, stirrer motors, volumetric pipette, and glass equipment such as glass flask, glass cup,
measuring cups, and erlenmeyer flask. Continuous tubular reactor scheme used is presented in Figure
2.1. The reactor scheme in waterbath is shown in Figure 2.2

Figure 2.1 Schematic diagram of continuous tubular reactor

 Prosiding Seminar Nasional Teknik Kimia Indonesia 2015 ISSN
Sustainable Energy and Mineral Processing for National Competitiveness
Yogyakarta, 12-13 Oktober 2015

2.2 Analysis
Analysis of the resulting biodiesel consists of total and free glycerol content analysis. The value
obtained is then used to calculate the value of bound glycerol content as a value that represents the
number of unconverted components in the reaction. Operating conditions which produce a lowest
value of total and bound glycerol contents for each variation of conditions set as the optimum
conditions. Analysis of glycerol content (total, free and bound), ester content, kinematic viscosity and
density at 40 °C was then performed on biodiesel produced from the optimum conditions to determine
the resulting conversion and the quality.

Figure 2.2 Reactor schematic diagram in the waterbath

2.3 Variation of Experiment Conditions

The variables varied were the length of the reactor, the total flow rate of the reactants, the molar ratio
of methanol to oil, reaction temperature and catalyst concentration. The variable were kept constant
was the type of raw materials used. Flow diagram of the study are presented in Figure 2.3.

Reactor design

Biodiesel production through transesterification reaction with RBDPO as raw material and using 1.25% -w
oil KOH at a reaction temperature of 60°C. Various operation condition used were:
Reactor length : L1 = 300 cm, L2 = 420 cm, L3 = 1020 cm
Total flow rate of reactans : Q1= 9,83; Q2= 18,86; Q3= 32,04 ml/minute
Molar ratio methanol to oil 6:1, 9:1 and 12:1
Biodiesel production using the optimum variation of reactor length, total flow rate of reactans, and molar
ratio methanol to oil. Various operation condition used were:
Reaction temperature: : T1 = 50°C, T2 = 60°C, T3 = 70°C and T4 = 75°C
Catalyst concentration: C1 = 0,75; C2 = 1,25; C3 = 1,75; and C4 = 2,25%--w oil

Total glycerol Free glycerol Bound glycerol

analysis analysis calculation

Optimum operation condition determination

Quality analysis of biodiesel produced at

optimum operation condition

Figure 2.3 Experimental flow diagram

 Prosiding Seminar Nasional Teknik Kimia Indonesia 2015 ISSN
Sustainable Energy and Mineral Processing for National Competitiveness
Yogyakarta, 12-13 Oktober 2015

3. Result and Discussion

The performance of the reactor designed in this study seen from the conversion towards biodiesel
achieved which is represented by the value of the biodiesel bound glycerol content. The reaction
product in the form of biodiesel is analyzed to measure the values of total glycerol and free glycerol
content. Data which obtained subsequently processed to determine the value of the bound glycerol
content.
The value of bound glycerol content is one of the parameters that can be used to analyze the
conversion of triglycerides into biodiesel obtained. This is because the number of triglycerides and
intermediate products in the form of and diglycerides and monoglycerides that are not converted into
methyl esters (biodiesel) in the biodiesel formation reaction reflected through %-w value of biodiesel
bound glycerol content. The smaller the value of biodiesel bound glycerol content, the higher the
conversion into methyl esters achieved. Biodiesel quality requirements based on ISO 7182: 2012 was
had maximum total glycerol content of 0.24%-w and maximum free glycerol content of 0.02%-w or
in other words, biodiesel has a maximum bound glycerol content of 0.22% -w.
Value content of glycerol in biodiesel can be affected by several factors such as the perfection of the
biodiesel formation reaction and the biodiesel purification process (leaching). In line with the purpose
of this study that is to know optimum operating conditions that can be applied to the designed reactor
in order to obtain a high conversion rate into biodiesel, so in this study, the biodiesel washing process
is done with an acid solution. The aim is to stop the transesterification reaction shortly after biodiesel
leaving the reactor as well as to reduce the loss risk of glycerol content due to the purification process
when multi-stage washing with water was done. So it is expected that the value of glycerol content
obtained would actually represent the content of glycerol in biodiesel shortly after leaving the reactor.
3.1 Effect of the reactor length and the residence time
According to Hayyan et al. (2008), the yield of transesterification reaction will increase with the
increasing of the substances residence time. Sufficient residence time required by the reactants to react
to achieve equilibrium. In the reactor used, with a constant value of the reactor cross-sectional
diameter and the reactants flow rate, duration of residence time is influenced by the length of the
reactor itself. The results showed that the lowest value of bound glycerol content in biodiesel obtained
when the reaction was held at 1020 cm reactor length, both for the reaction with methanol to oil molar
ratio of 6:1; 9:1; and 12:1. The lower the value of a bound glycerol content showed the higher
biodiesel conversion into methyl ester obtained in the reaction. Values of biodiesel bound glycerol
content in various reactor lengths can be seen in Figure 3.1.

0.350
Bound Glycerol (%-w)

0.300

0.250 ratio 6:1

ratio 9:1
0.200
ratio 12:1
0.150
200 400 600 800 1000 1200
Reactor Length (cm)

Figure 3.1 Values of biodiesel bound glycerol content in various reactor

3.2 Effect of the total flow rate and molar ratio of methanol to oil
One factor that must be considered in the use of the tubular reactor is the flow rate in the reactor. The
overly high flow rate will result in too short residence time that can cause an imperfection reaction.
Meanwhile, a flow rate that is too slow will cause the formation of a laminar flow in the reactor so
that the turbulent flow is not formed. As a result, a uniform mixture of the reaction solution will not be
 Prosiding Seminar Nasional Teknik Kimia Indonesia 2015 ISSN
Sustainable Energy and Mineral Processing for National Competitiveness
Yogyakarta, 12-13 Oktober 2015

produced. This condition will cause a decrease in the conversion rate of biodiesel (Pengmei et al.,
2010). Therefore, the reaction needs to be carried out at an optimal residence time and optimal stirring
conditions. Both of these can be obtained from the use of the optimum flow rate of the reactants in the
reactor. Figure 3.2. shows the value of biodiesel bound glycerol content at different values of the total
flow rate and the molar ratio of methanol to oil.
0.350
Bound Glycerol (%-w)

0.300

0.250 9,83 ml/min

18,86 ml/min
0.200
32,04 ml/min
0.150
6:1 9:1 12:1
Molar Ratio of Methanol to Oil

Figure 3.2 The value of biodiesel bound glycerol content at different values of
the total flow rate and the molar ratio of methanol to oil

In general, Figure 3.2. shows that the increase in the total flow rate of 9.83 into 18.86 ml/min will
reduce the levels of bound glycerol content of the biodiesel produced in the reaction using methanol to
oil molar ratio of 6:1 and 9:1. However, if the total flow rate increased again to 32.04 ml/min, the
value of biodiesel total glycerol content increased to > 0.3%-w throughout the variation ratio. This
value is above the maximum allowed limit value that is equal to 0.24% -w.
Decreased levels of glycerol content when the first increase in the flow rate can be caused by an
increase in the value of Reynolds number of the flow, so that the effect of mixing be a little better and
the reaction becomes more perfect. However, at a ratio of 6:1 and 9:1 the value of the total and bound
glycerol contents still do not meet the quality standards of biodiesel. When the flow rate was again
improved, the thing that happened was a decrease in the value of biodiesel glycerol content. This
happens because the residence time of substances being very short although the effect of mixing
become even better, so that the reaction has not had time to reach equilibrium.
A combination of reaction conditions consisting of a total flow rate of the reactants and the molar ratio
of methanol to oil that can produce biodiesel with glycerol content that meet the quality standards is
under conditions of flow rate 9.83 ml/min and a ratio of 12:1. In this condition, biodiesel obtained has
a value of total glycerol content of 0.209%-w and bound glycerol content of 0.203%-w.
3.3 Effect of reaction temperature

0.270

0.250
Glycerol (%-w)

0.230
Total
0.210
Bound
0.190
Total max limit
0.170 Bound max limit

0.150
45 55 65 75 85
Temperature (˚C)

Figure 3.3 The value of total and bound glycerol contents of biodiesel
produced at various reaction temperatures
 Prosiding Seminar Nasional Teknik Kimia Indonesia 2015 ISSN
Sustainable Energy and Mineral Processing for National Competitiveness
Yogyakarta, 12-13 Oktober 2015

Figure 3.3. shows the value of total and bound glycerol contents of biodiesel produced at various
reaction temperatures. It can be seen in the graph that below the boiling point of methanol at 64.7 ° C,
rise in temperature will result in decreased levels of total and bound glycerol biodiesel, which means
the reaction running more perfect and the conversions into methyl ester become better.
The value of biodiesel glycerol contents began to meet the required quality standards since operated at
the boiling point > 55 ° C. After passing the boiling point of methanol, the temperature rises initially
led to the decreased levels of biodiesel glycerol content. However, the reaction run at a temperature
above 70 ° C showed increased values of biodiesel glycerol content which means the conversion into
methyl ester decreased.
The increase in temperature will cause an increase in the rate of reaction. However, temperatures that
are too high can lower the reaction yield since high temperatures can trigger a saponification reaction.
The reaction temperature above the boiling point of methanol will transform methanol into the gas
phase, so that the reaction occurs in the reactor are in a two-phase system, the methanol in the gas
phase and triglycerides in the liquid phase. In the two-phase system, the reaction barriers becomes
greater because it is influenced by mass transfer events that can cause a decrease in the reactions
conversion.
3.4 Effect of catalyst concentration
One of the occurrence conditions of transesterification reaction is the presence of a catalyst in the
reaction. Kuworno and Ahiekpor (2010) argued that the higher the concentration of catalyst, the
higher the conversion rate can be achieved. Effect of catalyst concentration on total and bound
glycerol contents of biodiesel can be seen in Figure 3.4.

0.220
0.215
0.210
Glycerol (%-w)

0.205
0.200
Total
0.195
0.190 Bound
0.185
0.180
0 0.5 1 1.5 2 2.5
Catalyst Concentration (%-w oil)

Figure 3.4 Effect of catalyst concentration on total and bound glycerol

contents of biodiesel

Figure 3.4. showed that the use of catalyst concentrations in the range of 0.75 to 2.25%-w oil on
transesterification reactions with temperature conditions of 60 ° C and the total flow rate of ± 9.83
ml/min will produce biodiesel with the value of glycerol content < 0.24% (meets the applicable
quality standards). Another thing that can be concluded that the increased concentration of catalyst in
the reaction will reduce the values of total glycerol and bound glycerol contents. But the increased
concentration in the range of 0.75 to 1.75%-w oil showed only a slight decline in the value of
biodiesel glycerol content.
Meanwhile, when the catalyst concentration increased up to 2.25%-w oil, there will be a significant
decrease in the value of total and bound glycerol contents compared to the previous range, reaching
the final values of 0.191 and 0.184%-w for the concentration of total and bound glycerol content
respectively.
3.5 The optimum process conditions
Based on the data collected previously, the chosen optimum process conditions is a flow rate of 9.83
mL/min, methanol to oil molar ratio of 12:1 and a catalyst concentration of 2.25% as a process
condition that can produce biodiesel with the lowest levels of glycerol. Meanwhile, the selected
 Prosiding Seminar Nasional Teknik Kimia Indonesia 2015 ISSN
Sustainable Energy and Mineral Processing for National Competitiveness
Yogyakarta, 12-13 Oktober 2015

optimum reaction temperature is at a value of 63 °C because the temperature is still below the boiling
point of methanol so that it can prevent any hindrance of mass transfer due to a two-phase reaction
system and still be able to produce biodiesel with glycerol levels that comply the standards quality
regulations.
The resulting biodiesel is then washed in two ways. The first way is stirring the sample with 0.1 N
citric acid solution until reaching a neutral pH as was done in the sampling on previous data. The
second way is a common washing which is usually applied in the purification stages of biodiesel in
the form of multi-stage washing with water until it reaches neutral pH, followed by drying process.
The value of total and bound glycerol content of biodiesel produced in optimum condition with
various reactor length values is presented in Figure 3.5.

0.250
0.230
0.210
Glycerol (%-w)

0.190
0.170 T1
0.150
0.130 B1
0.110 T2
0.090
B2
0.070
0.050
200 400 600 800 1000 1200
Reactor Length (cm)

Note: T1 = Total glycerol content with acid washing, B1 = Bound glycerol content with acid washing
T2 = Total glycerol content with common washing, B2 = Bound glycerol content with common washing

Figure 3.5 The value of total and bound glycerol content of biodiesel
produced in optimum condition with various reactor length values

It can be seen in the graph that all the products of biodiesel produced in the reactor with a length of
300, 420, and 1020 cm shortly after leaving the reactor (experiencing acid leaching) and after
purification stages have a total glycerol and bound glycerol contents that meet the quality standards
ISO 7182:2012 which is less than 0.24%-w and 0.22%-w respectively.
However, the value of glycerol contents of biodiesel which is undergoing a purification process by
multi-stage leaching is lower than that experienced acid leaching. This is in accordance with the value
of biodiesel ester levels on a regular washing which is higher than in acid washing.
Purification stages consisting of multi-stage leaching with water and drying were able to reduce the
glycerol content in biodiesel because either glycerol, monoglycerides, diglycerides and triglycerides
which did not react will dissolve in water that has polar properties. Similarly to what happened with
methanol and a KOH. This leads to biodiesel produced will have a higher ester levels (did not much
contaminated with other compounds).
However, biodiesel with acid leaching representing biodiesel conditions right after leaving the reactor,
also has a fairly high values of ester levels, which is in the range of 95-97%. After purification stage
this value is increased in the range of 99.4 to 99.5%-w. This value meets the applicable quality
requirements which is > 96.5% -w and applies to all existing reactor length.
The results of biodiesel quality analysis after the purification step consisting of kinematic viscosity
and density at 40 °C as shown in Table 3.1. also shows the value that meets the applicable quality
requirements which is in the range of 2.3 to 6.0 mm2 /s for the viscosity and 850-890 kg / m3 for the
density.
 Prosiding Seminar Nasional Teknik Kimia Indonesia 2015 ISSN
Sustainable Energy and Mineral Processing for National Competitiveness
Yogyakarta, 12-13 Oktober 2015

Tabel 3.1 The results of biodiesel quality analysis after the purification

Reactor Length Residence Time Viscocity Density

No
(cm) (minute) (mm2/s) (kg/m3)
1 300 3.79 3.26 855.8
2 420 5.31 3.16 857.3
3 1020 12.89 3.22 859.0

4. Conclusions
Continuous tubular reactor which is designed with an internal diameter of 4 mm and a length of 1020
cm can be used to produce biodiesel with high ester levels through a transesterification reaction. The
optimum process conditions suitable for this reactor is a flow rate of 9.83 mL/min, molar ratio of
methanol to oil 12:1, the catalyst concentration of 2.25%, and the optimum reaction temperature of 63
°C. In this condition, biodiesel produced which then undergo a purification process is able to meet the
applicable quality standards in the value of glycerol content, ester levels, kinematic viscosity and the
density at 40 °C.

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