Review Paper

A review of heterogeneous calcium oxide based catalyst from waste

for biodiesel synthesis
Jasmine Si Jie Ling1 · Yie Hua Tan1 · Nabisab Mujawar Mubarak1 · Jibrail Kansedo1 · Agus Saptoro1 ·
Cirilo Nolasco‑Hipolito2

© Springer Nature Switzerland AG 2019

Abstract
Biodiesel is one of the most promising method to replace the fossil fuels because it is more environmentally friendly.
Nevertheless, biodiesel manufacturing costs are much higher compared to conventional fossil fuels. Thus, the biodiesel
should be synthesizing from reusable wastes to minimize the production cost. Homogeneous catalyst is the most com-
mon catalyst employed in the commercial biodiesel field. However, there are some drawbacks in using homogeneous
catalyst in the reaction such as the difficulties faced in separation process of the homogeneous catalyst from the mixture
of product. The presence of promising current technology has proved that the utilization of heterogeneous catalyst can
assist in overcoming the existing problem of homogeneous catalytic reaction, especially in wastewater generation. The
heterogeneous catalysts are more environmentally friendly, easier to separate and its reusability property. Despite its low
production cost and its beneficial use as an eco-friendly waste recycle method, waste materials may possess qualities
and characteristics that differ from the conventional homogeneous catalyst prior to biodiesel production. This review
paper focused in the recent discovery of the heterogeneous catalyst synthesized from natural bio-waste materials,
especially CaO-based such as eggshells, seashells and bones for biodiesel production. Apart from that, gypsum, part of
the construction waste is proposed as the newly found heterogeneous catalyst. Gypsum exists abundantly due to the
rapid development of the economics where construction and demolition activities are happening daily. The utilization
of these construction waste-based catalysts may able to provide a sustainable route for biodiesel production. This review
will enhance the development and existing scientific data in the area of biodiesel production and the synthesis of CaO-
based catalyst especially the synthesis of CaO-based catalysts from construction material.

Keywords Biodiesel · Biodiesel production · Heterogeneous catalyst · CaO catalyst · Gypsum

1 Introduction Moreover, fossil fuels are considered to be eco-destructive

because they are either indirectly or directly creating many
The worldwide energy crisis is a result of the tremendous problems such as global warming and climate change via
reduction of fossil fuels as the impact of the rapidly rising discharging the greenhouse gases into the atmosphere.
population especially in developing nations. In most of the Presently, global climate change and depletion of natu-
developing countries are primary rely on the fossil fuels to ral resources are drawbacks to relying heavily on fossil
act as the main source of energy. Fossil fuels are certainly fuels resources. Scientists have predicted that the fossil
able to fulfil the global energy mandate of exceeding 90% resources might run out in 2050 due to the high demand
and act as the most reliable energy resources available [1]. and consumption of fossil fuels at one hundred thousand

* Yie Hua Tan, tanyiehua@curtin.edu.my | 1Department of Chemical Engineering, Faculty of Engineering and Science, Curtin University
Malaysia, CDT 250, 98009 Miri, Sarawak, Malaysia. 2Instituto of Biotechnology, Universidad del Papaloapan, Circuito Central #200,
Col. Parque Industrial, C.P. 68301, 68000 Tuxtepec, Oaxaca, Mexico.

SN Applied Sciences (2019) 1:810 | https://doi.org/10.1007/s42452-019-0843-3

Received: 11 March 2019 / Accepted: 26 June 2019 / Published online: 1 July 2019

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times than the natural creation [2]. Besides, the global 2 Biodiesel
demand is projected beyond the double to ~ 30 Terawatt
by the year of 2050 and triple to ~ 46 Terawatt at the end of Biodiesel is an alternative fuel built up from monoalkyl
the century [3]. Furthermore, the price of petroleum prod- esters through either catalyzed or non-catalyzed reac-
uct is quite fluctuating. Thus, the energy alternative—bio- tion of transesterification between triglycerides (oils
fuel derived energy is gradually gaining the global atten- or fats) and light alcohols (methanol or ethanol). The
tion to cater the energy security problems. For instance, triglycerides sources can be virgin or used edible oils
biodiesel has been touted to be a substitute to replace such as soybean oil, palm oil, vegetable oil or sunflower
the existing traditional petroleum-based fuels. Apart from oil. These used vegetable oils can be exploited as the
that, biodiesel is sustainable, biodegradable and eco- oil feedstocks even after been used in cooking. There
friendly [4]. Economical materials such as plant biomass are many advantages of biodiesel, for example, high
with no greenhouse gases emission of biofuels cause it on lubricity, high flash point, low viscosity, biodegradable
stern renewable energy sources to overcome the energy and environmentally friendly and low emission of green-
and environment challenges [5]. Those renewable energy house gases [1]. The physicochemical fuel properties of
resources can be extracted from waste cooking oils, animal biodiesel will differ according to different oil feedstocks
fats or vegetable oils which can produce biodiesel emit- and alcohols used but biodiesel can be fully utilized as
ting less pollutants compared to fossil fuels [6]. an alternative fuel for petroleum-based fuels to meet the
The biodiesel is commonly synthesized through trans- growing energy demands safely and efficiently [10].
esterification reaction with the help of homogeneous cata-
lyst. There are several disadvantages can be found via this
catalytic reaction such as being destructive to the environ-
ment by discharging the alkaline wastewater. There are 3 Biodiesel production
also some limitations for the viable applications such as
the complexity in the synthesis process and also compli- There are two typical types of catalyzed reaction: (1)
cations in conducting the application of homogeneous homogeneous catalyst and (2) heterogeneous catalyst.
catalyst on large-scale factories [7]. The biodiesel production is commercially produced by
Therefore, several researches were suggested to use the homogeneous catalytic reaction with the availability of
heterogeneous catalyst instead of homogeneous catalyst current implemented technology, i.e. transesterification
in the transesterification reaction to obtain biodiesel. [11]. The reaction with the occurrence of homogeneous
Heterogeneous catalyst does provide more advantages catalyst is considered relatively fast and can achieve
when compared to homogeneous catalyst. For example, high conversion in short time. Nevertheless, it has severe
it is environmentally friendly, non-corrosive and able to hitches. The catalyst cannot be regenerated or recovered
achieve higher yield of biodiesel [8]. and must be neutralized then removed right after the
The heterogeneous catalyst can be derived from various completion of reaction. This will eventually generate
waste resources such as construction waste. Construction a large amount of wastewater during the purification
waste can be easily found in any countries, especially the stage [9]. Furthermore, the separation process of homo-
developing countries whereas they built a lot of buildings geneous catalysts from products is challenging and tedi-
to provide shelters to the citizens. The construction waste ous. Thus, this will involve more equipment and hence,
is a pertinent concern in protecting the environment. Tai- cause higher capital cost [7].
wan has generated approximately 1.27 million tonnes of A several promising technologies has implied that
construction waste in 2009 [9]. The construction waste the use of heterogeneous catalyst in the transesterifica-
contains a wide-ranging proportion of municipal solid tion process can help to cater the associated problems
waste. The most common method to dispose construc- faced with homogeneous catalyst. The natural based
tion waste is by landfilling. Hence, the potential to apply of heterogeneous catalysts are mostly non-corrosive and
using construction waste as the derivation for heterogene- environmentally friendly. Separation the heterogeneous
ous catalyst for the production of biodiesel can provide a catalyst from the mixture is much easier than homoge-
cost-effective approach to recycle the waste and eventu- neous catalysts [11]. Besides, the employment of hetero-
ally can reduce the production cost for the biodiesel pro- geneous based catalysts in the transesterification reac-
duction [9]. tion can increase the yield and purity of the produced
biodiesel [8].
Human generates wastes daily, for example con-
struction activities create significant amount of waste

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which will impact the environmental either physically are also 2 main categories of catalysts which are the homo-
or chemically. These environmental impacts will lead to geneous catalyst and heterogeneous catalyst. Most of the
higher energy consumption, greater solid waste gen- biodiesel production are obtained with the assistance of
eration, more pollutions and more greenhouse gases homogeneous catalyst via present technologies, transes-
emission. For example, in 2012, United Kingdom (UK) terification. However, there are many disadvantages using
had produced 100 million tonnes of wastes from con- the homogeneous catalyst in the chemical reaction such
struction activities [12]. Despite that, Malaysia as one as difficulties in separation of the biodiesel mixture and
of the developing countries generates approximately generate a large volume of wastewater [14]. Thus, scien-
twenty-six thousand tonnes of wastes daily from con- tists have further improved the existing technologies, the
struction activities which means there are approximately associated problems are able to be solved by using het-
nine million wasted produced annually [13]. The citizens’ erogeneous catalyst in the biodiesel production process.
awareness of proper managing construction waste is The heterogeneous catalyst can be synthesized from many
considering as low in Malaysia and therefore, lead to an resources such as biomass or non-biomass based, that is
increase in illegal dumping sites. There are few types of construction waste. The benefits and drawbacks of homo-
construction waste, for example, wood, concrete, metals, geneous and heterogeneous catalyst are shown in Table 1.
bricks, drywall, roofing, plastics, cardboard and others. Presently, the research on the heterogeneous catalysts
Some of these construction waste can convert into use- synthesized from biomass or non-biomass are explored
ful material or can be used as the raw material to pro- extensively because of its potential to decrease the capi-
duce heterogeneous CaO based catalyst. For instance, tal production cost. Through high temperature treatment,
gypsum is a waste from false ceiling can be used as the biomass will be chemically transformed into carbonaceous
raw material to synthesize the heterogeneous CaO based material and this carbon based material which contain the
catalyst to produce biodiesel. Moreover, waste reuse and anticipated functional groups can be as a catalyst [20].
recycling allow to fully utilize these wastes and will even- Besides that, the calcium carbonate content in some of the
tually reduce the waste disposal. biomass waste can be converted to calcium oxide based
catalyst to be applied in transesterification process [21].
Calcium oxide component (CaO) is non-corrosive, eco-
4 Biodiesel catalyst friendly and abundantly. It is easily to handle due to the
advantages of its low solubility, high alkalinity and most
There are many types of technology that can be used to importantly, it can be reused after the reaction. Hence, it
produce biodiesel. For instance, transesterification reac- has been defined as one of the most frequent used het-
tion between edible or non-edible oil with alcohols such as erogeneous catalyst in biodiesel production [22]. CaO can
methanol with or without the presence of catalyst. There be derived from natural resources such as cement-based

Table 1  Comparison of homogeneous and heterogeneous catalyst based on advantages and disadvantages
Type of catalyst Advantages Hitches

Homogeneous base catalyst There is no water formation in transesterification There is occurrence of saponification when the free
process [15] fatty acids composition in the oil is more than 2 wt%
Alkaline catalytic (2 steps) transesterification reac- which will decrease the biodiesel yield and cause dif-
tion from waste vegetable oil is economical in ficulties in purification process [15]
producing biodiesel [16] There will be more wastewater eliminated through
Sodium hydroxide (NaOH) and potassium hydrox- purification stage [18]
ide (KOH) are easy obtainable and economically The catalyst can only be used once
feasible [17] High sensitivity towards free fatty acids content [17]
The reaction occurred at trivial reaction which
reduce the usage of energy [15]
The rate of reaction is roughly 4000 times faster than
transesterification process using acidic catalyst [17]
Heterogeneous base catalyst The catalyst is reusable and recyclable [18] The catalyst is poisonous during exposure to ambient
Separation process from product is easier [18] air [17]
The reaction rate is much faster than acid-catalysed The basicity property causes the sensitivity towards
reaction [17] the free fatty acids content to be high [17]
The life span of the catalyst is long [15] There is limitation in diffusion [19]
The reaction happened at mild reaction which even- The transesterification process will require more molar
tually minimize the energy utilization [17] ratio of methanol to oil [19]

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wastes, seashells, eggshells or bones. The calcium oxide and it is mostly daily consumed in most of the nations.
can be derived from calcium carbonate compound via Calcium carbonate is one of the major compounds in a
high temperature calcination process ranging from 700 to chicken eggshell with 96% of oxides [40]. The utilization of
1000 °C [7]. The fully transform temperature for calcination eggshell as a catalyst can indirectly assist in reducing the
process varies according to different calcium carbonate landfill waste which can maintain the clean environment.
waste feedstocks. A summary table of comparison for CaO Besides that, reuse of the waste eggshell can decrease the
catalysts derived from several sources had been tabulated production cost for replacing or purchasing new catalyst
as shown in Table 2. in the biodiesel production.
Several researches showed the use of eggshell as a cata-
4.1 Heterogeneous catalyst derived from eggshell lyst in the transesterification reaction for biodiesel produc-
tion can increase the yield of biodiesel and can ease the
The alkaline earth metal oxides such as calcium oxide separation process [8]. Atadashi et al. [15] have reported
which contains a high level of base is very suitable in syn- that converting eggshell into a heterogeneous catalyst for
thesizing the heterogeneous catalyst. There are several biodiesel production has simplified the purification stage
researches have reported that the calcium oxide is the and thus consumed less water and energy.
most reliable heterogeneous basic catalyst in biodiesel Usually, the obtained eggshell was washed with dis-
synthesis [38]. The calcium oxide is can be easily obtained tilled water for dust and impurities removal [41]. The
in various of low-cost materials or wastes such as eggshell. cleaned eggshell will be dried in an oven at 100 °C over-
This can be act as the heterogeneous catalyst and used in night and the particle size was further reduced using
the biodiesel production with different types of oil feed- grinding mortar. Khemthong et al. [42] has stated that the
stocks and alcohol [39]. high temperature calcination process took place within
Eggshell is plentifully available worldwide as the the temperature range between 500 and 1100 °C in air
chicken egg is the most preferable food for breakfast for 180 min in a muffle furnace. This calcination process

Table 2  Catalytic performance for transesterification process over CaO catalysts derived from different source
Source Catalyst Type of oil Operating conditions Yield (%) References
Type Heat treatment Molar Catalyst Time (min) Temper-
ratio of loading ature
M:O (wt%) (°C)

Chicken egg- CaO 1000 °C, 2 h Soybean 9:1 3 180 65 95 [23]

shells CaO 900 °C, 2 h Karanja 8:1 2.5 150 65 95 [24]
Mud crab CaO 900 °C, 2 h Palm olein 0.5:1 5 150 65 98.8 [25]
Cockle CaO 900 °C, 2 h Palm olein 0.54:1 4.9 180 65 99.4 [26]
Mussel CaO 1050 °C, 2 h Soybean 24:1 12 480 60 94.1 [27]
Clam CaO 900 °C, 3.5 h Waste frying oil 6.03:1 – 360 60 > 89 [28]
CaO 900 °C, 4 h Palm olein 9:1 1 120 65 98.0 [29]
Turkey bones CaO/biological 909.4 °C, 4 h Mustard 9.9:1 4.97 180 70 91.22 [30]
tri-calcium
phosphate
(BTCP)
Bovine bones CaO 350 °C – Soybean 6:1 8 180 65 97.0 [31]
1000 °C, 6 h
Pig bones CaO/ 600 °C, 4 h Palm 9:1 8 90 65 >90 [32]
hydroxyapa-
tite (HAP)
­K2CO3
Sheep bones CaO/ 600 °C, 8 h Canola 12:1 5 300 60 95.18 [33]
hydroxyapa-
tite (HAP)
Cement CaO 450 °C, 3 h Soybean 24:1 4 180 65 98.5 [34]
Dolomite rock CaO 800 °C, 2 h Palm kernel 30:1 6 180 60 99.9 [35]
Lime mud CaO 800 °C Peanut 15:1 6 180 64 94.4 [36]
Red mud CaO 200 °C, 5 h Soybean 24:1 4 189 65 94.0 [37]

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can fully transform the calcium carbonate to calcium oxide impractical and non-economically feasible, in terms of
component. operating cost. There are researches done to overcome
the problems by impregnating the calcined animal bones
4.2 Heterogeneous catalyst derived from seashell in potassium hydroxide aqueous solution to improve the
specific chemical properties of the bones which is much
There are different types of catalyst which can be derived related to increase the heterogeneous catalytic activity
from waste which can reduce the waste disposal and pre- [50].
serve the environment. Calcium oxide is considering as the The obtained animal bones were washed with hot water
high potential solid catalyst used for biodiesel production for ~ 240 min to remove the dust, impurities and cartilages
which can be derived from various sources such as sea- on the bones. Then, it was dried at 110 °C for ~ 5 h. The ani-
shells. These waste seashell sources are cheap and most mal bone particles were further crushed into powder form
importantly is they are eco-friendly [43]. The seashells of using a mechanical grinder. The powder was activated via
some certain species contain greater than 90% of calcium calcination process within temperature of 500–1100 °C.
carbonate which can be used to convert into calcium oxide
through calcination process at the temperature beyond 4.4 Heterogeneous catalyst derived
800 °C [44]. Nevertheless, there is one major concern when from construction waste
using calcium oxide as the heterogeneous catalyst for
biodiesel production. The calcium oxide surface is easily Reusing and recycling is an effective method to reduce the
contaminated by moisture attachment to form calcium landfill size and fully utilize them to produce and develop
hydroxide when exposed to ambient air because of the new products to reduce the dependency of these natural
absorption of carbon dioxide and water [45]. The preven- resources. Daily wastes are produced from either construc-
tion of exposure of calcium oxide to atmosphere after the tion site, industries or households. The construction waste
calcination process is considered to be not practical. Kouzu disposal is normally dumped to landfills or the irresponsi-
et al. [46] reported the heterogeneous catalytic activity of ble contractors will leave them there. There are many types
calcium oxide will be reduced once it exposes to the air as of construction waste can be found, for example, concrete,
short as 3 min. woods, gypsum or bricks. These wastes can be fully utilized
Also, there are a few studies showed the employment to reuse or regenerate as a new beneficial product, such as
of seashells as a heterogeneous catalyst with doping of solid catalyst and so forth.
aluminum and zinc nitrate via dissolution–precipitation For example, the cement-based waste collected from
method. From the studies, the catalyst was calcined at construction site can be further processed into a useful
500 °C reported its surface contains a higher amount of heterogeneous base catalyst to be applied in the produc-
calcium. The nanocrystallites of calcium oxide are well dis- tion of biodiesel. Most of the unwanted concretes are
crete and thus, it has the strongest ability to resist ambient generally handled by burying them and this eventually
air with relative humidity of 73% up to 72 h [47]. will cause a severe environmental pollution. There are 180
million tonnes of shattered concrete generated from con-
4.3 Heterogeneous catalyst derived from bones struction sites annually. Hence, these cement waste can be
transformed into useful item instead of dumping them as a
There are quite a number of wastes can be re-calcined waste [9]. The cement-based waste is considered a promis-
as a solid catalyst in biodiesel production such as animal ing calcium sulphate source due to its high conversion rate
bones. The reutilization of wasted animal bones can be and the presence of metal oxides which further enhance
a cost-effective method to synthesize the heterogeneous the catalytic activity of the triglycerides alcoholysis in
catalyst for biodiesel production [48]. The cost of catalyst biodiesel production [2]. Quartz, portlandite, albite and
is having a direct relationship with the overall production calcite are the major mineral compounds can be found in
cost. Hence, the re-calcined of animal bones as a low-cost concrete which have improve the overall heterogeneous
heterogeneous catalyst can help to reduce the production catalytic activity.
cost of biodiesel synthesis [49]. There are some researches using cement-based waste
The animal bone is considered one of the best source as a solid basic catalyst to increase the transesterifica-
of solid waste which can be used as catalyst due to the tion reaction rate to produce more biodiesel with higher
availability in the countries. The catalyst synthesized from purity. The collected cement waste from the construction
animal bones has shown a good consistency and hetero- and demolition activities was grounded and then calcined
geneous catalytic performance in the transesterification at high temperature to be further applied into biodiesel
process but required higher catalyst loading with a longer as a solid catalyst. Gimbun et al. [4] has showed that the
reaction time. Hence, the usage of animal bones become cement can be fully utilized as a heterogeneous catalyst

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and achieved a conversion of 95% in presence of excess further assist the nation to move from an oil-based econ-
oil at temperature of 60 °C and reaction time of 180 min. omy towards a circular economy. A comprehensive analy-
While, the 5 wt% catalyst loading has accomplished the sis of the gypsum-based heterogeneous catalyst is crucial
highest conversion of 96.9% when the calcination tem- to be investigated to understand the heterogeneous cat-
perature was set at 700 °C with a reaction temperature of alytic activity and characterization before implementing
65 °C and reaction time of 480 min [4]. The physiochemi- this into biodiesel production. Nevertheless, there are lim-
cal properties of the produced biodiesel are able to meet ited researches investigated the feasibility of construction
the range of specifications identified by the international waste in biodiesel production. The physiochemical proper-
biodiesel standard, ASTM D6751. ties of the construction waste catalyst are believed to have
an impact in the conversion of biodiesel by having a bet-
4.5 Heterogeneous catalyst derived from gypsum ter particle size, porosity and effective functional group.
Thus, it is significant to find the optimum calcination tem-
Gypsum, a part of the construction waste is not fully perature and operating conditions to produce biodiesel
exploit yet in the biodiesel field. Chemically, gypsum is a with maximum yield. This review is hoped to able to give
common natural sulphate mineral with a chemical formula an insight in deriving the heterogeneous calcium oxide-
of ­CaSO4·2H2O and this calcium sulphate component can based catalyst derived from different type of wastes such
be transformed into calcium oxide via the ordinary high as gypsum which acts as the waste from construction site
temperature calcination process by eliminating sulphur and they are able to act as efficient reusable basic catalyst
dioxide gas. It can be found as a waste from construction to be employed in biodiesel production. To conclude, this
site. For example, gypsum is appeared as a by-product review has successfully offered an insight to the various
when titanium (IV) oxide is extracted from ilmenite ores possibilities and opportunities of reusing different kind of
using digestion of sulphuric acid [51]. Subsequently, the wastes and huge possibility construction waste gypsum
unused acid will be treated by calcium carbonate to neu- catalyst to be implemented in the near future. The future
tralize the mixture. Huntsman Tioxide is one of the most of biodiesel synthesis has also gained a potential method
well-known company in manufacturing titanium dioxide of advancement to be more economically affordable by
­( TiO2) worldwide [52]. The annual capacity of this plant classes of society alike as an attempt to reduce harmful
in Malaysia is approximately 56 thousand metric tonnes. emissions that are currently liberated through the use of
Thus, plant is indirectly producing approximately 400 fossil-based products.
thousand tonnes of gypsum as by product per year [34].
Hence, it can be concluded gypsum is abundantly in Acknowledgements The authors gratefully acknowledge the sup-
port from Curtin University Malaysia. This work was supported by the
Malaysia and suitable to act as an alternative to be used as FRGS Grant Scheme, Contract No: FRGS/1/2016/TK07/UNIMAS/01/2
a raw source to synthesize the calcium oxide based hetero- and Code No. F02/FRGS/1490/2016 granted financial resource from
geneous catalyst in biodiesel production. Apart from that, Ministry of Education, Malaysia.
the gypsum waste can be found at construction site. Same
procedure is proposed, i.e. crush and high temperature Compliance with ethical standards
calcination are able to produce the efficient solid catalyst
for transesterification reaction between the oil and alcohol Conflict of interest The authors declare that they have no conflict of
interest.
in a batch of reactor system.

5 Conclusions
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