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Transesterification of Mixture of Castor Oil and Sunflower Oil in Millichannel

Reactor: FAME Yield and Flow Behaviour

Article  in  Procedia Engineering · December 2016

DOI: 10.1016/j.proeng.2016.06.487

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Procedia Engineering 148 (2016) 378 – 384

4th International Conference on Process Engineering and Advanced Materials

Transesterification of Mixture of Castor Oil and Sunflower Oil in

Millichannel Reactor: FAME Yield and Flow Behaviour
Muhammad Fitri Jamila,*, Yoshimitsu Uemuraa, Katsuki Kusakabeb, Olumide Bolarinwa
Ayodelea, Noridah Osmana, Nik Muhammad Nik Ab Majidd, Suzana Yusupc
a
Centre for Biofuel and Biochemical Research (CBBR), Universiti Teknologi PETRONAS, Bandar Seri Iskandar, 31750, Perak, Malaysia.
b
Department of Nanoscience, Sojo University 4-22-1 Ikeda, Nishi-ku, Kumamoto 860-0082, Japan.
c
Department of Chemical Engineering, Universiti Teknologi PETRONAS, Bandar Seri Iskandar 31750 Perak, Malaysia.
d
Institute of Tropical Forestry and Forest Products (INTROP), Universiti Putra Malaysia 43400 Serdang, Selangor, Malaysia.

Abstract

Transesterification of castor oil, sunflower oil and mixture of both oils were conducted in a millichannel reactor with 1.6 mm
internal diameter. The flow behavior of the sample in millichannel reactor was observed. Both of the oil was mixed from 100 mL
of castor oil until 20 mL of castor oil with total amount of 100 mL solution before used in the reaction. The alkali catalyst was
mixed together with methanol before entering the reactor. In this study, the behavior of the flow pattern inside the millichannel
reactor was observed under fixed parameters which are 21:1 methanol-to-oil molar ratio, 5.4 wt% of KOH concentration in
methanol, 180 s of residence time and 60 oC of temperature. The FFA value of both the oils was less than 2 mg-KOH/g-oil. The
viscosity and density of the oils were determined before and after mixing the oils. The flow behaviour of the castor oil formed
parallel flow throughout the reactor while sunflower oil formed slug flow in the reactor. When the volume of castor oil is reduced
from 100 mL to 20 mL, the flow behaviours of the mixture oil were changed from slug flow at upstream to parallel flow at
downstream. The formation of slug flow in the reactor improved the biodiesel yield: 88.4% of FAME yield.

©
© 2016
2016TheTheAuthors. Published
Authors. by by
Published Elsevier Ltd.Ltd.
Elsevier This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
Peer-review under responsibility of the organizing committee of ICPEAM 2016.
Peer-review under responsibility of the organizing committee of ICPEAM 2016
Keywords: biodiesel; transesterification; millichannel reactor; castor oil

* Corresponding author. Tel.: +605-368-7645; fax: +605-368-7648.

E-mail address: fitrijamil90@gmail.com

1877-7058 © 2016 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
Peer-review under responsibility of the organizing committee of ICPEAM 2016
doi:10.1016/j.proeng.2016.06.487
 Muhammad Fitri Jamil et al. / Procedia Engineering 148 (2016) 378 – 384 379

1. Introduction

Biodiesel production has been widely studied due to the depletion of fossil fuel and increasing awareness to
reduce global warming. Production of biodiesel using millichannel reactor was becoming a topic of discussions
among researchers on its efficiency and practicality for continuous production that giving many advantages
including rate of reaction and yield improvement and energy efficiency [1]. Millichannel reactor enhances the mass
transfer rate between the reagents due to high interfacial surface area and internal circulation flow throughout the
reactor [2]. The slug flow produce mono dispersed aqueous droplets with average diameter 130-550 µm will raise
the mass transfer rate 10-1000 times higher compared to the traditional liquid-liquid systems and increase the
surface-to-volume ratios in the reactor [3, 4].
Synthesizing of biodiesel using millichannel reactor has been reported in many papers about high conversion of
the reaction with different feedstock. Norita et al. [5] reported the optimum parameter of the microtube reactor for
palm oil biodiesel reached 91% of fatty acid methyl ester (FAME) yield. Besides, Guan et al. [6] reported 100% of
conversion for the optimum parameter of transesterification of sunflower oil in microtube reactor. The conversion of
soybean oil conducted by Masoud et al. [7] showed the production of 89% methyl ester from transesterification in
microtube reactor for 0.43 min which are higher compared to conventional batch reactor. However, the efficiency of
the microreactor can be affected if the high viscosity liquid was used because it can stop the flow or produce annular
flow which reduces the contact surface between the reagents [4, 8].
Castor oil is non-edible oil that has high oil content around 35 – 55% which has potential to be feedstock for the
biodiesel production but it is one of the vegetable oils which have highest viscosity and molecular weight [9]. The
production of biodiesel from castor oil shows a promising result in conventional batch reactor which is 92% of oil
conversion [10]. There is no study about the transesterification of castor oil in millichannel reactor to observe the
efficiency of the reactor to be compared with batch reactor.
In this study, the flow patterns of castor oil (CO), sunflower oil (SO) and the mixture of both oil with different
mixing ratio of CO and SO were investigated. The viscosity of CO is high compared to SO which will produce
different flow patterns in millichannel reactor. This study has two objectives (1) to observe the flow patterns when
using CO, SO and mixture of the two oils; and (2) to relate the effect of flow patterns in millichannel reactor with
the FAME yield.

2. Materials and Methods

2.1. Materials

Commercial castor oil (CO) was purchased from India and sunflower oil (SO) with brand Zucchi was purchased
from Japan convenience store to be the feedstock for the transesterification reactions. Super dehydrated methanol,
potassium hydroxide pellet, acetic acid, phloxine B was obtained from Wako Pure Chemical Ind. Ltd. Japan.
Hexane and acetone were obtained from Wako Pure Chemical Ind. Ltd. Japan as the solvent for GC analysis.
Linoleic acid methyl ester was used as the standard for FAME yield. A transparent Teflon (FEP) tube with inner
diameter of 1.6 mm was used for as a millichannel reactor for transesterification reaction and observation of the
flow pattern.

2.2. Biodiesel Production

A schematic diagram of experimental setup is shown in Figure 2.1. The glass syringe was used as the feeder to
the reactor with T-shaped joint as the mixer for methanol and oil before going into the reactor. Potassium hydroxide
was mixed with methanol with concentration of 5.4 wt%. The CO was stirred together with SO with different
volume which are 80 mL CO: 20 mL SO, 60mL CO: 40mL SO, 40mL CO: 60mL SO and 20mL CO: 80mL SO for
the observation of the flow patterns. The pure castor oil and sunflower oil also being used in the observation of the
flow patterns. The molar ratio of the methanol and oil mixture was adjusted to 21:1 by adjusting the flow rates. The
total liquid flow in the reactor was 40.2 ml/hr. The product was collected in a beaker fill with 10mL of 10% acetic
acid to terminate the reaction.
380 Muhammad Fitri Jamil et al. / Procedia Engineering 148 (2016) 378 – 384

Acetic Acid
Aqueous
Solution

Figure 1: Experimental Setup for Microtube Reactor

The collected product was centrifuged at 4500 rpm for 15 minutes. The upper layer (FAME) was taken and
rinsed for 3 times to wash the leftover methanol and potassium hydroxide in the FAME. 0.1mL of product was
diluted in 3mL of mixture of 30% of acetone and 70% of hexane for analysis. The composition of fatty acid methyl
ester was analysed using Shimadzu 2014 Gas Chromatography with Flame Ionization detector using packed column
filled with Unisole 3000 at temperature of 220 oC. The FAME yield of the biodiesel was calculated as follows:

஺೔
‫ ݈݀݁݅ݕܧܯܣܨ‬ൌ  ൈ ͳͲͲΨ (1)
஺೚

Where ‫ܣ‬௜ is area of FAME peak in the sample, ‫ܣ‬௢ is area of Linoleic Acid Methyl Ester peak.

2.3. Flow Behaviour Observation

The flow patterns were observed through the transparent Teflon tube in millichannel reactor by taking the
pictures of the flow using a digital single lens reflex camera Nikon D40. The methanol was dyed with inert red
phloxine B to obtain clear images of the flow behavior in millichannel reactor. The dye used is inert and did not
affect the reaction in the reactor [6].

3. Results and Discussions

3.1. Feedstock Characterization

Commercial castor oil and sunflower oil were used in the experiment to investigate the flow pattern and FAME
yield in millichannel reactor. Both feedstock had different viscosity and density. Table 1 shows the density and
viscosity of castor oil, sunflower oil and the mixture of both oils for reduction of viscosity in the castor oil. The
result showed that the viscosity of oil reduced as the fraction of SO increases.
 Muhammad Fitri Jamil et al. / Procedia Engineering 148 (2016) 378 – 384 381

Table 1: The density and viscosity of castor oil, sunflower oil and its mixture

Sample No. Sample Name Density (g/ml)

Viscosity Kinematic Viscosity
(mPa.s) (mm2/s)
1 Castor Oil (CO) 0.9579 585.00 610.74
2 80CO:20SO 0.9514 226.67 238.26
3 60CO:40SO 0.9392 150.00 159.72
4 40CO:60SO 0.9307 101.20 108.74
5 20CO:80SO 0.9207 65.20 70.82
6 Sunflower Oil (SO) 0.9156 45.38 49.56

3.2. Flow Behaviour of Castor Oil, Sunflower Oil and Its Mixture

Figure 2 and 3 shows the difference flow behaviour between castor oil which has high viscosity and sunflower
oil which has low viscosity. The flow behaviour of castor oil shows parallel flow (Figure 4) between two reagents in
the tube which is methanol at the top layer and oil at the bottom layer while the flow behaviour of sunflower oil
produces slug flow (Figure 5) throughout the reactor. The parallel flow behaviour occurs due to high viscosity of
castor oil.

in out in out
Two layer flow Slug flow

Figure 2: Flow Pattern for Castor Oil with 5.4 wt% KOH Figure 3: Flow Pattern for Sunflower Oil with 5.4 wt% KOH

MeOH

Oil
Figure 4: Parallel Flow Behaviour Figure 5: Slug Flow Behaviour

The flow behaviour was then observed by mixing both oils with different ratios until the slug flow is observed.
Figure 6, 7, 8 and 9 show the flow behaviour of the different mixture of castor oil and sunflower oil. Based on the
observation, the mixture of 40 mL castor oil: 60 mL sunflower oil and 20 mL castor oil: 80 mL sunflower oil start to
form slug flow at upstream of the millichannel reactor and become parallel flow again at downstream. The slug flow
formation increased the FAME yield in the product and increase the mass transfer between the reagents instead of
diffusion between them through parallel flow behaviour.
382 Muhammad Fitri Jamil et al. / Procedia Engineering 148 (2016) 378 – 384

in Two layer flow out in Two layer flow out

Figure 6: Flow Pattern for 80%CO: 20%SO with 5.4 wt% KOH Figure 7: Flow Pattern for 60%CO: 40%SO with 5.4 wt% KOH

in out in out

Slug flow Slug flow

Two layer flow

Two layer flow

Figure 8: Flow Pattern for 40%CO: 60%SO with 5.4 wt% KOH Figure 9: Flow Pattern for 20%CO: 80%SO with 5.4 wt% KOH

The parallel flow behaviour formed throughout the reactor when 80% CO: 20% SO and 60% CO: 40% SO were
used. In 40% CO: 60% SO and 20% CO: 80% SO mixture, the slug flow formed at upstream and parallel flow
formed at downstream. The slug flow form only quarter part of the reactor when 40% CO: 60% SO mixture was
used while the slug flow formed almost half part of upstream when using 20% CO: 80% SO mixture.

3.3. FAME Yield

The product formed from each mixing ratio was then examined by using GC-FID to analyse the conversion to
fatty acid methyl ester. The different in flow behaviour increase the FAME yield in the product. The result can be
explained based on the phenomena of parallel flow behavior in the millichannel which have less mass transfer
between the reagent and they are contacting each other between the separation layers only. The formation of slug
flow in millichannel reactor helps to increase the mass transfer between the reagents that improve the FAME yield.
 Muhammad Fitri Jamil et al. / Procedia Engineering 148 (2016) 378 – 384 383

100
90 98.9
88.4
80
FAME Yield (%) 70
60
50
44.6
40
30
25.4
20
10
7.6 8.8
0
0 20 40 60 80 100
Sunflower oil content (vol%) in castor oil

Figure 10: FAME yield for mixture of castor oil and sunflower oil

4. Conclusions

The study of flow behaviour of castor oil, sunflower oil and their mixture showed that the formation of slug flow
start to form when the mixture was 40 mL of castor oil and 60 mL of sunflower oil. The formation of slug flow
increased the FAME yield in the product because the mass transfer between the reagents is increased and help to
increase the reaction. The best mixture castor oil and sunflower oil is at 80 mL of sunflower oil and 20 mL of castor
oil which give result 88.4% of FAME yield.

5. Acknowledgement

This research was supported by the Ministry of Education Exploratory Research Grant Scheme (Biodiesel
production by transesterification technique using new feedstock castor bean species) and Mitsubishi Corporation
Education Trust Fund.

6. References

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Reactors during Biodiesel Production from Waste Cooking Oil, American Institution of Chemical Engineering
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[2] G. Guan, K. Kusakabe, K. Moriyama, N. Sakurai, Continuous production of biodiesel using a microtube
reactor, Chemical Engineering Transactions, 2008 (14) 237-244.
[3] T. Sankarshana, V. Kalyan, U Virendra, C.E. Alemayehu, Reaction Performance in Micro and Milli Tubes,
Proceedings of the World Congress on Engineering and Computer Science, 2012 (2).
[4] J. N. Sovago, M Bente, Microreactors: A New Concept for Chemical Synthesis and Technological Feasibility
(Review), Material Science and Engineering, 2014 (39) 89-101.
[5] W.N. Wan Ab Rashid, Y. Uemura, K. Kusakabe, N. Osman, B. Abdullah, Synthesis of Biodiesel from Palm
Oil in Capillary Millichannel Reactor: Effect of Temperature, Methanol to Oil Molar Ration, and KOH
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[6] G. Guan, K. Kusakabe, K. Moriyama, N. Sakurai, Transesterification of Sunflower Oil with Methanol in a
Microtube Reactor, Industial Engineering Chemical Resources, 2009 (48) 1357-1363.
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