A Revew On Trend

Journal of Cleaner Production 355 (2022) 131588
Contents lists available at ScienceDirect
Journal of Cleaner Production

journal homepage: www.elsevier.com/locate/jclepro
A review on latest trends in cleaner biodiesel production: Role of feedstock,

production methods, and catalysts
Pranjal Maheshwari a, Mohd Belal Haider a, **, Mohammad Yusuf b, Jiří Jaromír Klemeš c,
Awais Bokhari c, d, Mukarram Beg e, Amani Al-Othman f, Rakesh Kumar a, ***, Amit K. Jaiswal g, h, *
a
Department of Chemical Engineering and Biochemical Engineering, Rajiv Gandhi Institute of Petroleum Technology, Amethi, Jais, 229304, Uttar Pradesh, India
b
Department of Chemical Engineering, Universiti Teknologi PETRONAS, Bandar Seri Iskandar, 32610, Perak, Malaysia
c
Sustainable Process Integration Laboratory, SPIL, NETME Centre, Faculty of Mechanical Engineering, Brno University of Technology, VUT Brno, Technická 2896/2,
616 00, Brno, Czech Republic
d
Department of Chemical Engineering, COMSATS University Islamabad (CUI), Lahore Campus, 54000, Punjab, Lahore, Pakistan
e
Department of Petroleum Engineering, University Institute of Engineering, Chandigarh University, Mohali, 140413, Punjab, India
f
Department of Chemical Engineering, American University of Sharjah, PO. Box 26666, Sharjah, United Arab Emirates
g
School of Food Science and Environmental Health, Technological University Dublin - City Campus, Central Quad, Grangegorman, Dublin, D07 ADY7, Ireland
h
Environmental Sustainability and Health Institute, Technological University Dublin - City Campus, Grangegorman, Dublin, D07 H6K8, Ireland
A R T I C L E I N F O A B S T R A C T
Handling Editor: Panos Seferlis The rising world population and its corresponding energy demands pose a considerable burden on natural energy
sources. The exploitation of fossil fuels at such an alarming rate blurs the goals of sustainable development and
Keywords: controlling global warming as pledged during the Paris Agreement. Due to the detrimental effects of exhausts
Sustainable development from conventional diesel fuel on the environment, biodiesel has earned significant importance during the last
Global warming
decade. Biodiesel is produced from different feedstocks such as neem oil, palm oil, waste frying oil, vegetable oil,
Biodiesel
animal fat, microbial oil, etc. These feedstocks react with acidic, alkaline, enzymic, homogeneous, heteroge
Deep eutectic solvents
Transesterification neous, and hybrid Deep Eutectic Solvents (DES) catalysts, along with monohydric alcohol via transesterification
reaction. The flexibility in its feedstock and the type of catalysts used, production cost, biodegradable and
renewable nature makes it a promising alternative fuel than conventional diesel. The selection of apt feedstock
and catalyst is the challenging task and governing factor of economic biodiesel production. Green solvents such
as DES have high thermal stability and low volatility and can address the economic and green production issues
significantly as compared to conventional alkali and acid catalysts. This review bridges the gap between the
selection of feedstock and optimal catalyst for the respective feedstock. The exploration of DES fills the gap by
attributing to 3Rs (i.e., recyclability, recovery, and reusability). This review highlights the contemporary trends
and prospects in the selection of the feedstocks, synthesis routes, and catalysts for the transesterification re
actions for biodiesel production.
Abbreviations: DESs, Deep Eutectic Solvents; FAME, Fatty Acid Methyl Ester; FFAs, Free Fatty Acids; TMAH, Tetramethyl ammonium hydroxide; TEA, Trie
thylamine; DEA, Dimethylamine; PTSA, p-toluenesulfonic acid; BTAH, Benzyltrimethyl ammonium hydroxide; TMG, Tetramethyl guanidine; SCMA, Super Critical
Methyl Acetate; CN, Cetane Number; ASTM, American Society for Testing and Materials; EN, European Norm; ILs, Ionic Liquids; ChCl, Choline chloride; DEAC,
Diethylaluminium chloride; HBA, Hydrogen Bond Acceptor; HBD, Hydrogen Bond Donor.
* Corresponding author. School of Food Science and Environmental Health, Technological University Dublin - City Campus, Central Quad, Grangegorman, Dublin,
D07 ADY7, Ireland.
** Corresponding author.
*** Corresponding author.
E-mail addresses: [email protected] (P. Maheshwari), [email protected] (M.B. Haider), [email protected] (R. Kumar), [email protected]
(A.K. Jaiswal).
https://doi.org/10.1016/j.jclepro.2022.131588
Received 7 November 2021; Received in revised form 23 March 2022; Accepted 28 March 2022
Available online 11 April 2022
0959-6526/© 2022 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
P. Maheshwari et al. Journal of Cleaner Production 355 (2022) 131588
1. Introduction
Energy is indispensable for existence, and it has become an absolute

imperative to optimize the pool of limited resources as the demand for
energy sources is escalating at a tremendous rate (Ullah et al., 2016).
After the United States and China, India is the third-largest primary
energy and oil consumer globally, as depicted in Fig. 1. According to the
Ministry of Petroleum and Natural Gas, Government of India, the de
mand for petroleum products would be approximately about 25 × 107 t
in 2022, as shown in Fig. 2 (Tiewsoh et al., 2019). Energy preservation
contributes to reducing the number of airborne pollutants and protects
the environment. To ensure the survival of the human species: the Fig. 2. Projected demand for all petroleum products (Tiewsoh et al., 2019).
relationship between natural capital and the population must be syn
chronized (Ewunie et al., 2021). With the limited pool of sources and has various drawbacks such as dehydration, washing with water (Hajjari
ever-increasing demand for global energy, alternative fuels are the most et al., 2017), and neutralization (Li et al., 2017) is required. Purification
practical way to achieve the rising demand (Iqbal et al., 2021). Re of product by separating glycerol and the catalyst is complex due to soap
searchers have shifted to alternatives in order to compete with this formation (Ullah et al., 2016), which acts as an emulsifier. It is not
ever-increasing demand (Rosdinbinti et al., 2021). Generally the domain economically feasible to use low-quality oil containing a high proportion
of alternative fuels facades the three major challenges i.e., (i) Special of Free Fatty Acids (FFAs) (Farooq and Ramli, 2015) along with regen
handling requirements of the proposed alternative fuels which are pre erating and reusing the catalyst (Ndiaye et al., 2020). Various solid
cariously distinctive from the petroleum fuels, (ii) High price and low catalysts can simultaneously catalyze transesterification and esterifica
energy density of the fuel compared to petroleum-based fuels, and (iii) tion reactions (Gaeta-Bernardi and Parente, 2016), with feedstock hav
An inadequate availability of supply to meet the nationwide re ing high FFAs to obviate saponification. Several lipases (Marín-Suárez
quirements (Waggoner and Dobie, 1994). The concept of circular et al., 2019) and potential solvents like DES (Bewley et al., 2015; Merza
economy (Pan et al., 2015) and generating wealth from waste is of et al., 2018) can also eliminate these limitations.
utmost importance while proceeding with alternative fuels production This review through light on the selection criteria of optimal feed
(Habagil et al., 2020). The biofuels, especially biodiesel, attracted re stock and respective catalyst for biodiesel production. The manuscript
searchers due to their critical advantages over fossil fuels and the flex also discusses the effectiveness of DESs over the conventional solvents
ibility of feedstocks, catalysts (Tayari et al., 2020). Biodiesel as diesel covering the aspects of 3Rs (i.e., recyclability, recovery, and reuse). The
fuel is bio-degradable (Okoye et al., 2020), non-toxic (Garcia et al., review highlights the latest advancements and types of catalysts,
2020), portable, sustainable (Sun and Li, 2020), efficient, and has low transesterification processes, and the effect of operating process pa
sulphur as well as aromatic content (Demirbaş, 2002). It has tremendous rameters on biodiesel production. The optimum and promising solutions
potential as an alternative fuel, due to its crucial characteristics, and to the current hurdles in biodiesel production are suggested.
usage of versatile feedstock i.e., from waste frying oil to cheap
non-edible including the local source (Singh et al., 2020). This is a 2. Need for cleaner biodiesel
promising and economic alternative for diesel fuel and can reduce the
world’s reliance on imported petroleum fuels. The properties such as In developing countries like Brazil, South Africa, and the South Asian
high flash points (Santos et al., 2020), properly formulated intrinsic region, 12–24 GJ/cap of energy consumption is required annually to
lubrication (Elkelawy et al., 2021), reduced exhaust emissions provide a decent standard of living (Yusuf et al., 2021). The energy
(Nogueira et al., 2020) made an extender for combustion in diesel demand will undoubtedly increase in the future scenario, and still, 84%
Compression Ignition Engines (CIEs) (Alagh, 2006). of the world’s energy is produced from fossil fuels (Yusuf et al., 2021).
The consumption of edible oil for technical prospects could signifi The exploitation of fossil fuels on this tremendous scale is never seen
cantly increase oil prices and pose negative consequences on society before in the history of the earth. To limit the ill effect of global warming
(Umana et al., 2020). For these purposes, the search for different raw and achieve the goals of the Paris Agreement, a cleaner and more
materials for biodiesel production is escalated (Brito et al., 2020; Pra economical source of fuel is required. Biodiesel is one such potential
dima et al., 2017). Presently, the application of non-edible oils, micro alternative that could help in lowering the use of fossil fuels. Various
algae (Rawat et al., 2011), and used cooking oil as raw material is of studies have reported the increase in NOx emission with biodiesel blend
deep interest (Niculescu et al.). Alkali catalysis for biodiesel production as compared to diesel but there is inconsistency in pointing out a single
reason for higher NOx emissions. The reasons for higher emissions are
effect of biodiesel on ignition delay, engine technology, adiabatic flame
temperature and timing of injection.
3. Biodiesel
Biodiesel is equivalent to processed diesel fuel that originates from

different bio-sources, and it is a “green biological” ester-based oxygen
ated oil that constitutes organic oils, fats. It is classified chemically as a
combination of long-chain fatty acid monoalkyl esters of fatty acids. It
includes palm oil, lauric oil, stearic oil, soybean oil, oleic oil, sunflower
oil, palmitic oil, rapeseed oil, canola oil and vegetable derivatives. In the
presence of a catalyst, animal fats or vegetable oils with alcohols pro
duces biodiesel and glycerine. For transesterification, methanol is
favored due to its economical cost and availability (Verma and Sharma,
2016). It is a domestic, renewable diesel fuel obtained from natural oils
such as soybean oil. Biodiesel, referred to as ASTM D 6751, consists of a
Fig. 1. Worldwide oil consumption (2018). monoalkyl ester long-chains of fatty acids obtained by animal fats or
2
vegetable oils, designated as B100 (Zhang et al., 2003). (Haas, 2005).

Biodiesel is a pure amber-yellow liquid having viscosity similar to Research on plant-based fuels, which has a bright future, has been
petrodiesel. It costs more to manufacture than petrodiesel, which seems conducted in recent years. Their main disadvantage is that prices are
to be the main preventive factor. The global production of animal fats higher than oil-derived types of diesel. To achieve this, a policy must aim
and vegetable oil is not adequate to substitute the use of liquid fossil fuel at their total tax exemptions (Prankl et al., 2004). The cost of biodiesel
(up to 20–25%) (Graboski and McCormick, 1998). Low viscosity, higher produced from vegetable oil (e.g., pure soya oil) is not surprisingly much
nitrogen oxide emissions (NOx), lower energy content, higher pour point higher than gasoline. It is essential to use approaches to reduce raw
and cloud point, coking of injector, lower engine power and speed, material prices. The use of waste frying oil to manufacture biodiesel is
higher price, and higher wear of engine are the main drawbacks of also an efficient way of lowering the cost of raw materials, as its cost is
biodiesel (Yusuf and Athar, 2015). Operational drawbacks of biodiesel around half the virgin oil price (Encinar et al., 2007). The use of waste
blends include fuel freezing problems in the cold weather, lower energy oils eliminates the pollution issues, as the reuse of these waste grades
capacity, and long-term fuel storage problem due to degradation. The minimizes the government’s waste collection, municipal waste control,
hydrocarbon fuels generally form a coating of tank layers, hoses. These and burden on wastewater treatment plants. Only a small fraction of
deposits loosen by biodiesel blends usually blocks fuel filters. It is a these oils contribute to the manufacturing of soap(Cárdenas et al.,
marginal problem that can be quickly resolved by correct filter main 2021).
tenance after the biodiesel blend is introduced (Wardle, 2003). Nonetheless, considering used frying oils with different properties
such as higher FFAs than raw and processed oils creates issue of lower
4. Sources of biodiesel yield and more catalyst consumption. The hydrolysis of triglycerides
accelerates by the high temperatures used for typical cooking, and water
Biodiesels or Fatty Acid Methyl Ester (FAME) comprises renewable from the food enhances the FFA in the oil. It also creates stability
sources like vegetable oil and fats. Soybean, sunflower, palm, rapeseed, problem in the mixtures and is responsible for higher peroxide values.
canola, cottonseed, and Jatropha have primarily used oils for biodiesel For refined and crude oils, the iodine value, viscosity, density, and
production. As diesel fuel is cheaper than edible vegetable oils, re saponification are different (Folayan et al., 2019). There are many
searchers have continuously explored alternative low-priced biodiesel concerns about optimizing methanolysis or ethanolysis of frying oil. For
sources such as waste vegetable oils and non-edible crude vegetable oils. biodiesel manufacturing, the resolution of these issues is significant.
In the face of great demand and supply gaps of edible oil, it is also not Biodiesel’s cost is minimal when waste-cooking palm oil is feedstock;
feasible to use edible oil to produce Biodiesel in India. Under Indian only feedstock costs approximately 70–95% of the overall cost (Math
conditions, appreciable non-edible oil is produced by cultivating even et al., 2010). The waste cooking oil and non-edible oils for biodiesel
on degraded land (Singh and Singh, 2010). production should be of higher interest than edible oils (Athar and Zaidi,
Although commonly stated, animal fats were not researched to a 2020).
comparable degree as vegetable oils due to their various natural prop
erties. The saturated fatty acids in vegetable oils are lower than animal
4.1. Biodiesel production
fats; hence, they are usually solid at room temperature (Ma and Hanna,
1999). Fig. 3 mentions biodiesel sources as vegetable oil, non-edible oils,
Biodiesel is generally produced through transesterification to form
animal fat and other biomasses. The biodiesel source usually depends on
esters and the by-product glycerol, utilizing a lipid response with alco
cultivations that are suitable for the local climate. In the US, soybean oil
hol—basically, the action of alcohol that displaces an ester called alco
is the most popular foodstuff for biodiesel, while, in Europe and other
holysis (alcohol-cleavage). The reaction is reversible with the
tropical countries, the most common source of biodiesel is rapeseed
stoichiometry of a 1:3 lipid or oil to alcohol ratio, and excess alcohol
(canola) and palm oil (Kim et al., 2018; Umana et al., 2020). Two
shifts the equilibrium towards the forward direction, as seen in Equa
conditions to be fulfilled by biodiesel are low cost of production and
tion (1) (Brito et al., 2020). For the higher yield of the product, this ratio
large-scale development. For example, there is a high production cost of
is typically increased.
refined oils and a low production scale. Due to the easy availability of
non-edible seeds, algae and sewages, they have low production costs TG + 3CH3 OH ⇌Catalyst RCOOCH3 + Glycerol (1)
Fig. 3. Biodiesel feedstock in (a) EU, (b) USA, (c) World (Kim et al., 2018).
3
It constitutes a consecutive sequence of three reversible reactions. high acid values. However, the major disadvantage of the biocatalyst is
The first step consists of transforming triglycerides to diglycerides, their high concentration requirement and long reaction time. The sep
which is followed by conversion of diglycerides to monoglycerides, and aration of the enzyme from the final product after the reaction is difficult
eventually monoglycerides to glycerol. From each reversible step, an which add significant cost in the production of biodiesel.
ester group is obtained, as shown in Equations (2)–(4). (Glisic and
Orlović, 2014). 4.2.4. Homogeneous catalyst
Homogeneous catalysts, including acidic and basic, are widely used
1
Triglyceride + R OH ⇌ Diglycerdie + RCOOR 1
(2)
for biodiesel production. Acid catalysts are less active than the base
catalyst, and a complete contrast is seen in Table 1. When FFAs in the oil
Diglyceride + R1 OH ⇌ Monoglycerdie + RCOOR1 (3)
exceeds 1%, the acid catalyst becomes more efficacious. Usually, acid
catalysts prevent soap foaming. The acids catalyze the esterification of
Monoglycerdie + R1 OH ⇌Glycerol + RCOOR1 (4)
FFAs to form FAME and thereby enhanced biodiesel production.
Compared to base-catalyzed, the acid-catalyzed reaction is slow; there
4.2. Biodiesel catalyst fore, it involves high temperature and pressure (Refaat, 2010). The deep
eutectic solvents (DESs) having acidic nature were also investigated for
Biodiesel are fatty acid methyl esters (FAME) having long chain fatty their potential for biodiesel production. These DESs are shown to ach
acids with lower alkyl esters. As discussed above, they are synthesized ieve more than 90% conversion of biodiesel. Different type of DESs and
by two processes (i) esterification of fatty acids and (ii) trans their effectiveness in converting biodiesel are discussed in detail in
esterification with lower alcohol. It should be noted that in the absence section 8. For alkaline catalysts, the FFAs quality is essential as they
of catalysts, transesterification reactions can occur. They require high react with an alkaline catalyst to form soap. This process restricts the
temperature, pressures, and significant reaction time, in addition to pre reaction and affects biodiesel yield.
and post-treatment steps which increases the overall cost of the entire Several researchers highlighted that if the feedstock’s FFA quantity is
process (Diasakou et al., 1998). Despite the high purity of ester and not more than 1%, and all the materials are almost anhydrous, then the
glycerol (soap-free), it is usually not considered industrial biodiesel due alkali-catalytic transesterification can be carried out. Table 1 highlights
to its high cost. The three catalyst forms are used: alkaline, acidic, and a brief comparison between homogeneous and heterogeneous catalysts.
enzyme catalysts (Thangaraj et al., 2019). The higher conversion of the ester is obtained at comparable to low
temperature and pressure. It also takes lesser time by using a basic
4.2.1. Alkaline catalysts catalyze, which significantly lowers process costs. The alkaline metal
They are the most widely used catalysts for the production of bio hydroxides like KOH and NaOH are less cost-efficient than metal alk
diesel, including alkaline catalysts such as NaOH, KOH, alkaline metals, oxides, and their reactions were faster than the sodium and potassium
and alkaline metal carbonate (e.g., sodium and sodium carbonates). methoxide reactions. They are a good option since they can transform
Their principal advantage is high ester yield under moderate reaction vegetable oil only by increasing the concentration of the catalyst to 1 or
conditions over brief reaction periods (Yan et al., 2014). Alkaline cata 2%. For an anhydrous oil/alcohol mixture, water forms due to the hy
lysts are suitable for oils having low FFAs due to their sensitivity as oils droxide reaction with the alcohol. Table 2 and Table 3 include a list of
with higher FFAs are converted to soap instead of biodiesel. The FFAs various homogeneous base catalysts and acid catalysts reported in the
react with alkaline catalysts leading to formation of soap which curbs literature and a comparison with essential parameters.
the separation of glycerine, biodiesel and water. Therefore, trans
esterification, specifically lower acidic vegetable oils, yields high ester. 4.2.5. Heterogeneous catalysts
The de-acidification must be done before the transesterification of It is well-known that heterogeneous catalysts eliminate extra pro
vegetable oil to reduce this problem. cessing costs, which are involved in homogeneous catalysis and obviate
various pollutant generations. Heterogeneous catalysts also aid fast
4.2.2. Acidic catalysts recycling and reuse, which is leading to an economical green process
Acidic catalysts favour higher efficiency for the esterification of FFAs (Endalew et al., 2011). They can tolerate high FFA content as well as
compared to alkaline catalysts. An acid-catalyzed transesterification moisture content (Liu et al., 2008). In severe reaction conditions, such as
demands the fairly high temperature (~100 ◦ C), pressure (~5 bar) and a high temperature and pressure, heterogeneous catalysts are considered
high amount of alcohol. In comparison to alkaline catalysis, it is often an integral part of biodiesel production. They can be recovered from the
slower. These types of catalysts are particularly favoured for feed oil reaction mixture, stand up to aqueous treatment steps and can be
having very high acid value. The solid acid catalyst has gained much modified to achieve a high level of activity, selectivity, and long lifetime
attention for transesterification of lower quality feeds. Certain catalysts catalysts. The heterogeneous catalysts can conceive the grafting and
have shown simultaneous esterification and transesterification by trapping of the active molecules on or in solid support pores such as
alcoholysis achieving up to 90% conversion (Kulkarni et al., 2006). Most silica, alumina, or ceria. In chemical reactions such as Michael
of the experiments were conducted in the laboratory and their com Condensation, isomerization, Knoevenagel Condensation, aldol
mercialisation is still not possible due to corrosion and side products
formed which adds to the cost in the biodiesel production. The key
benefit of acidic catalytic conversion is the efficient esterification of Table 1
FFAs in vegetable oils, constituting a very high acid value as edible Comparison between Homogeneous and Heterogeneous catalysts.
waste oil. Properties Heterogeneous Homogeneous catalysts
catalysts
4.2.3. Enzymes Rate of Reaction Moderate conversion Rapid and high conversion
Enzymes are also used for biodiesel production, for example lipases Catalyst Reuse Possible Not possible
After Treatment Can be recovered No recovery of catalyst should be
obtained from different microorganisms behave as catalysts (Rangana
neutralized, directing to waste
than et al., 2008). The biocatalyst offers higher conversion of biodiesel chemicals
under moderate temperature, pressure and pH. As compared to alkali or Methodology Continuous fixed-bed Limited use of continuous
acid catalyst in enzymatic biodiesel production, little or no residual or operation possible methodology
soap formed in the end products thereby resulting in high-quality Presence of H2O/ Non-Sensitive Sensitive
Free Fatty Acids
glycerol production. The biocatalyst can be used for feedstocks having
4
Table 2
A comprehensive list of homogeneous base catalysts for alcoholysis.
S Catalyst Used Alcohol Source Alcohol/Oil Molar Temperature (◦ C)/Reaction Yield% References
No. Used Ratio Time (h)
1. NaOH Methanol Sunflower Oil 6:1 60/1 ~97 Brito et al. (2020)
2. Tetramethyl ammonium hydroxide Methanol Cottonseed Oil 6:1 64/2 ~98 Karavalakis et al.
(TMAH) (2010)
3. KOH Ethanol Soyabean Oil 12:1 60/1 ~95 Brito et al. (2020)
4. NaOCH3 Methanol Waste frying Oil 6:1 60/1 ~93 Keera et al. (2011)
5. Tetramethyl guanidine (TMG) Methanol Waste frying Oil 12:1 65/1.5 93.82 Karavalakis et al.,
2011
6. Triethylamine (TEA) Methanol Cottonseed Oil 9:1 190/3 ~55 Karavalakis et al.
(2010)
7. Benzyltrimethyl ammonium Methanol Waste frying Oil 6:1 65/2.5 ~95 Karavalakis et al.
hydroxide (BTAH) (2010)
8. tert-butylamine (t-BA) Methanol Cottonseed Oil 9:1 190/3 62.4 Guan et al. (2009)
9. TEA-KOH Methanol Cotton seed Oil 9:1 192/3 ~94 Peiyong et al. (2010)
10. Dimethylamine (DEA) Methanol Cottonseed Oil 9:1 190/3 ~67 Peiyong et al. (2010)
11. KOH Methanol Madhuca longifolia oil 1:0.35 60/0.5 Saravanan et al.
(2020)
12. KOH Methanol Castor Oil 5.4:1 64/2.5 ~97.82 Aboelazayem et al.
(2018)
13. KOH Methanol Waste Cooking Oil 9.4:1 62.4/2 ~98.26 Mohadesi et al.
(2019)
14. KOH Methanol Elaeagnus angustifolia L 9:1 60/1 ~95 Kaisan et al. (2020)
seed oil
15. NaOH Methanol Citrullus vulgaris seed 5:1 ~70 Efavi et al. (2018)
oil
Table 3
A comprehensive list of homogeneous acid catalysts for alcoholysis.
S Catalyst Used Alcohol Used Source Alcohol/Oil Temperature (◦ C)/ Yield References
No. Molar Ratio Reaction Time (h) %
1. CH3SO3H Ethanol Palm fatty acid 3:1 130/1 ~80 Farag et al.
(2011)
2. H2SO4 Methanol Sunflower Oil + Oleic Acid 6.12:1 55/4 ~96 Marchetti et al.
(2007)
3. C2HF3O2 Methanol Soyabean Oil 20:1 80/6 ~98 Miao et al.
(2009)
4. NaOCH3 Methanol Waste frying Oil 6:1 60/1 ~93 Keera et al.
(2011)
5. AlCl3 Methanol + Tetrahydrofuran Canola Oil 24:1 115/18 ~98 Soriano et al.
(THF) 1:1 (2015)
6. H3PO4 Methanol Palm fatty acid 3:1 130/1 ~51 Athar and Zaidi
(2020)
7. p-toluenesulfonic acid Methanol + dimethyl ether Corn Oil 10:1 80/2 ~97 Guan et al.
(PTSA) (DME) 1:1.17 (2009)
8. HCl Methanol Oleic acid + SunflowerOil + 6:1 60/2 ~88 Farag et al.
Soyabean Oil (2011)
9. H2SO4 Methanol Rice bran Oil – 100/8 ~97 Encinar et al.
(2007)
10. H2SO4 Methanol Neem Oil 6:1 – ~83 Joshi et al.
(2018)
Condensation, oxidation and transesterification; alkali earth metal ox resolve waste disposal problems partially, and the value-added materials
ides, metal transition oxides, mixed metal oxides, ion exchange resins aid a benefit to many processes. Researchers have developed organic
and alkali metal compounds assisted by the alumina or zeolite are used. waste-based solid catalysts such as plantain peeling, wood, cocoon
The SrO (strontium oxide) has high basicity, and due to its solubility, it shells, palm. Banana peels as solid waste catalysts produce the related
doesn’t solubilize in methanol; it retains up to 10 cycles of efficiency oxides of potassium and sodium, as studied by (Betiku et al., 2016).
(Nizami et al., 2020). Solid acid catalysts have lower catalytic activity Drying in a hot-air oven at 80 ◦ C for 48 h and calcining at 700 ◦ C at 4 h
than solid base catalysts. Various solid base catalysts for trans was used to produce a banana peel catalyst. Table 4 and Table 5 sum
esterification include CaO, MgO, SrO, KNO3/Al2O3, K2CO3/Al2O3, marize crucial reaction parameters for the different heterogeneous base
KF/Al2O3, Li/CaO, KF/ZnO, Mg/Al, Lithuanian and Alpine origin zeo and acid catalysts.
lites. Such catalysts produce more than 92% biodiesel yield under
optimal reaction conditions (Kim et al., 2004). 5. Biodiesel processing methods
Low-cost solid wastes used as chemical reaction catalysts have shown
a great potential for efficient biodiesel production studied by Farooq The following methods used to treat the biodiesel are:
et al. A large quantity of calcium carbonate in eggshell can be converted
by calcination to CaO at 900 ◦ C. In the transesterification process, it 5.1. Pyrolysis (thermal cracking)
exhibited high catalytic activity and produced up to 93.5% biodiesel
(Farooq et al., 2018). The application of catalyst waste materials can In the absence of air or oxygen, pyrolysis transforms one material to
5
Table 4
A comprehensive list of heterogeneous base catalysts for alcoholysis.
Catalyst Used Wt.% Alcohol Source Alcohol/Oil Temperature (◦ C)/ Yield% References
Catalyst Used Molar Ratio Reaction Time (h)
Sr3Al2O6 3 Methanol Soyabean Oil 25:1 60/1 ~96 Rashtizadeh et al.

(2014)
CaZn(OH)4 3 Ethanol SunflowerOil 20:1 78/3 ~95 Rubio-Caballero et al.
(2013)
SrO 5 Methanol Olive Oil 6:1 65/.25 ~82 Chen et al. (2012)
K3PO4 5 Methanol Fried Oil 6:1 65/3 ~78 Viola et al. (2012)
Li/CaO 5 Methanol Karanja Oil 6:1 65/1 ~99 Ali et al. (2011)
Capiz Shell, CaO 3 Methanol Palm Oil 8:1 60/6 ~94 Suryaputra et al.
(2013)
Museel Shell, CaO 12 Methanol Soyabean Oil 24:1 60/8 ~94 Correia et al. (2014)
Templated- MgO 3 Methanol Canola Oil 20:1 192/2 ~98 Jeon et al. (2013)
MgAlFe hydrotalcite 3 Methanol Soybean oil 21:1 65/4 ~81 Wang and Yu (2012)
K/Al2O3-Monolith 0.50 Methanol Soybean oil 32:1 120/6 ~60 Brito et al. (2020)
CaO/dolomite catalyst 3 Methanol Microalgae oil 6:1 65/3 ~90 Çakırca and Akın, 2021
KOH–CaO .65 Methanol Waste 7:1 – ~96.44 Sharma et al. (2019)
Cottonseed Oil
Carbon extracted from date seed 4 Methanol Waste Cooking 15:1 65/1.5 ~94.27 Jamil et al. (2021)
modified with Ca and Mg oxides Oil
Hybrid CaO/Al2O3 aerogels 3:1, CaO/ 1 Methanol Waste cooking 1:1 65/4 ~89.9 Kesserwan et al. (2020)
Al2O3 oil
Carbon-based magnesium oxide (MgO) 6 Methanol Castor oil 12:1 75/1 ~96.5 Du et al. (2019)
Table 5
A comprehensive list of heterogeneous acid catalysts for alcoholysis.
Catalyst Used Wt.% Alcohol Source Alcohol/Oil Molar Temperature (◦ C)/Reaction Yield% References
Catalyst Used Ratio Time (h)
HZSM-5 Zeolite 10 Methanol Oleic acid 20:1 100/7 ~81 Vieira et al. (2013)
Fe(HSO4)3 1 Methanol Waste frying 15:1 205/4 ~95 Alhassan et al. (2013)
Oil
30% WO3/AlPO4 5 Methanol Soybean Oil 30:1 180/5 ~73 Xie et al. (2012)
Crude SiO2-Tosic acid 6 Methanol Palm Oil 20:1 140/2 ~65 Melero et al. (2009)
Sulfonated carbon nano-horn 3 Methanol Palmitic acid 33:1 65/5 ~93 Poonjarernsilp et al.
(2014)
Sulfated LaO. 10 Methanol Oleic acid 5:1 100/6 ~95.5 Vieira et al. (2013)
Sulfonated Carbon 7.50 Methanol Polanga Oil 30:1 180/5 ~98.5 Folasegun et al. (2014)
Sulfated LaO/HZSM-5. 10 Methanol Oleic acid 5:1 100/7 ~99.8 Vieira et al. (2013)
30% Tungstosicic acid/Zeolite Hβ – Methanol Soybean oil 4:1 65/8 ~95 Narkhede and Patel
(2013)
Spirulina platensis. β-Strontium 2.5 Methanol Microalgal Oil 12:1 65/2 ~76.34 Singh et al. (2020)
silicate (β-Sr2SiO4).
another using heat or with the help of catalysts (Higman et al., 1973). reaction has been illustrated in Fig. 4. The pyrolysis process for biodiesel
Compared with other cracking methods, the process is quick, less production is obsolete and therefore new processes are now being used
pollution and efficient (Schwab et al., 1988). The thermal degradation for biodiesel production.
5.2. Dilution
For engine operation, vegetable oil is diluted with diesel. In 1980,

Caterpillar Brazil used 10 wt% vegetable oil in pre-combustion chamber
engines to keep total power without variation or engine adjustment. At
that time, 100 wt% vegetable oil was not replaced by diesel, but a
mixture of 20 wt% vegetable oil with 80 wt% diesel fuel succeeded.
Short-term studies have been using a ratio of 50/50. The fuel was
blended by 25 wt% of sunflower oil and 75 wt% of diesel. The low
viscosity is suitable for improved engine efficiency, reducing the pro
portion of fuel.
5.3. Microemulsion
Microemulsion describes a dispersion of optically isotropic fluid

microstructure as a colloidal equilibrium, with measurements typically
1–150 spontaneously produced by two ordinarily immiscible liquids as
well as multiple ionic amphiphiles (Likozar and Levec, 2014). They can
enhance spray characteristics through vaporizing explosively all low
Fig. 4. Triglycerides thermal degradation process (Higman et al., 1973). boiling constituents in micelles. The performance of the engine was the
6
same for the micro-emulsion of 53 wt% sunflower oil and 25 wt% sun conditions. Glycerides and alcohol must be water-free for an alkaline
flower oil in diesel. Micro-emulsion prepared by blending the soya bean catalyzed transesterification, as water partially modifies the reaction to
oil, cetane, 2-octanol and methanol in a ratio of 52.7: 1.0: 33.3: 13.3 also saponification due to soap formation. Many researchers worked on
passed the 200 h-EMA test. feedstocks with high FFAs. However, alkaline catalysts used in most
cases remove FFAs from the process stream as soap. The typical waste
grease contains 10 and 25% FFAs, a much higher level for an alkaline
5.4. Transesterification/Esterification catalyst to produce biodiesel. Some researchers also claim alternate use
of an acid catalyst that is more tolerant of FFAs. Fig. 6 shows the
By far, this is the most favoured method for biodiesel production. It is mechanism of catalyzed acid transesterification of vegetable oil. Pro
a reaction of fatty acid or oil with alcohol resulting in esters and glyc tonation of the ester’s carbonyl group leads to carbocation that creates
erol. The reaction may involve a catalyst or no catalyst. For a non- an intermediate tetrahedral after a nucleophilic attack on alcohol
catalytic reaction, high temperature and pressure is required moreover (Demirbas, 2008). This intermediate remove glycerol forming a new
the yield is low in the non-catalytic process. The catalyst generally ester, and the catalyst is regenerated. An acid catalyst is used due to
strengthens the reaction rate and yield. In the reaction, FFA reacts with more water and FFAs present in triglycerides, while in the presence of an
alcohol to form FAME and water (Murugesan et al., 2009). Due to its alkaline catalyst, transmethylation happens about 4000 times faster
reversible nature, excess alcohol shifts equilibrium towards the forward than catalyzed by a single acidic catalyst (Ganesan et al., 2009).
direction. The primary and secondary alcohols with C1– C8 are used for
transeterification (Formo, 1954). The choice of catalyst is also very 5.4.3. Lipase Catalyst Transesterification
diverse in this case and mostly depends on the conversion, corrosion and Lipase Catalyst Transesterification is similar to alkaline trans
separation of end products obtained. esterification and varies with a catalyst-solvent ratio, stirring, and
catalyst used in this transesterification is lipase. The mechanism illus
5.4.1. Chemistry of the transesterification process trated in Fig. 7 depicts that Lipases have a known ability to function best
Transesterification comprises several consecutive reversible re on long-chain fatty alcohols than short-chain ones. Generally, in systems
actions. Triglycerides gradually convert to diglycerides, monoglycerides with or without solvent, the efficiency of transesterification of methanol
and ultimately glycerol. Each phase in Equations (2)–(4) indicates a (methanolysis) for triglycerides is likely to be lower than ethanol.
mole of ester.
5.4.4. Supercritical method
5.4.2. Alkali catalyzed transesterification Recently, supercritical methods have attracted researchers due to
The reaction mechanism for alkali catalyzed transesterification in several advantages over other methods, such as the absence of catalyst
volves three steps, as depicted in Fig. 5. In the initial stage of the reac (Tan et al., 2011), low residence time (Farobie and Matsumura, 2015a),
tion, methoxide ion (the anion of alcohol) attacks the carbonyl carbon of high rate of reaction (Kusdiana and Saka, 2001), very low sensitivity
TG and forms a tetrahedral intermediate. In the second step, this inter towards FFAs (Zabeti et al., 2009), potential to treat a large range of
mediate reacts with alcohol to form methoxide ion, and finally, in the feedstocks and no pre-treatment (Muppaneni et al., 2012). Initially, this
last step, tetrahedral intermediate results in the formation of a diglyc technology for biodiesel production was employed for methanol and
eride and fatty acid ester (Schuchardt et al., 1998). Alkoxides are formed ethanol (Rathore and Madras, 2007). Recently, this method has gained
by mixing NaOH, KOH, K2CO3 and similar catalysts with alcohol attention due to production without glycerol using dimethyl carbonate
(Demirbas, 2009a). and super-critical methyl acetate (Farobie and Matsumura, 2015b). A
The process of biodiesel production from vegetable oils, using het vast range of reactants with Triglyceride have been reported including
erogeneous catalyst Na/NaOH/Al2O3, has been developed by Kim et al. methyl acetate, methanol, ethanol, and di methyl carbonate.
(2004). This catalyst displayed precisely the same behaviour as tradi
tional homogeneous NaOH catalysts under controlled reaction
Fig. 5. Basic catalytic transesterification mechanism of vegetable oils (Schuchardt et al., 1998).
7
Fig. 6. Acidic catalytic transesterification mechanism of vegetable oils (Demirbas, 2008).
(Elgharbawy et al., 2021). Homogenous base catalyst forms soap that

neutralizes FFAs and could be transformed back into FFAs by the in
clusion of H3PO4 to decanted glycerol and soap mixture from the end
product (Mumtaz et al., 2017).
6.3. Type of alcohols
Methanol is used chiefly for biodiesel because of straightforward

Fig. 7. Lipase catalytic flow map of biodiesel production ((Bajaj et al., 2010)).
extraction from the finished product (John et al., 2021). Methanol has
multiple advantages over other alcohols, such as higher conversion in
6. Factors affecting the biodiesel production the case of waste cooking oils and lower viscosity as compared to other
alcohol-based biofuels (Parthiban et al., 2021). The methanol is cheaper
6.1. Water content than other alcohols, the toxicity of methanol is higher than ethanol. The
ethanol or isopropanol forms an azeotropic mixture with water which
The amount of water present in feedstock accelerates the hydrolysis creates the difficult separation of fuel from alcohol in the distillation
reaction, and at the same time, reduces the formation of ester(Felizardo process (Musa, 2016). In some cases, the reaction mixture is added with
et al., 2007). The water content must be less than 0.5% for a 90% yield of Iso or t-butanol as a solvent to prevent methanol or glycerol inhibition of
biodiesel, which is essential for an acid-catalyzed reaction compared to a lipase. The methanol causes enzyme deactivation, denaturation or in
base-catalyzed reaction (Bogalhos et al., 2012). In acid-catalyzed bio hibition at higher concentration (Norjannah et al., 2016). These issues
diesel production, water obtained as a byproduct inhibits the reaction could be caused by blocking the entry of triglycerides, changes in
and thus decreases engine performance. In most cases, anhydrous so conformation; hence, ethanol is used instead of methanol in most
dium sulfate (Na2SO4) or anhydrous magnesium sulfate remove mois enzymatic reactions (Parthiban et al., 2021).
ture from the product. Water in the oil can be removed by preheating up
to 120◦ C (Marchetti et al., 2007). Certain enzymes require water to be
active as the amount of water is less than the number of water molecules 6.4. Alcohol to oil ratio
in a single layer around the enzyme molecules (Norjannah et al., 2016).
If the raw water is more significant than that, deactivation of the lipase A 3 mol of alcohol and 1 mol of triglyceride are required to produce
lowers the conversion (Kumari et al., 2009). one alkyl ester mole (IŞIK, 2021). The Le-Chateliers principle states that
product formation rate increases with the increasing concentration of
reactants. The rate of product formation increases with higher alcohol
6.2. Free Fatty Acids (FFAs) concentration (Razak et al., 2021). The product formation further in
creases by increasing the alcohol to oil molar ratio. Glycerol and
The higher free content of fatty acids results in soap and water for non-reacted methanol recovery are difficult as it form emulsion through
mation (Adenuga et al., 2021). If the FFA content is over 3%, even a saponification reaction in aqueous medium. During biodiesel production
homogeneous base catalyst is not used in the transesterification reaction two phases are formed due to difference in densities and polarities:
(Chang et al., 2021) and the heterogeneous catalysts solve this issue and upper phase comprises of biodiesel, while other consists of crude glyc
pre-treat FFAs to result in FFA esters with a homogeneous acid or het erol mixture (Rodrigues et al., 2017). Crude glycerol mixture comprises
erogeneous catalyst (El-Gendy et al., 2015). The rate of acid-catalyzed of alcohol, glycerol, water, soaps and non-glycerol organic matter.
reaction is usually slow, and low-temperature conditions are needed Composition of these components may vary as per quality of feedstock.
8
Post-treatment process of crude glycerol mainly involves three steps: (1) enzyme catalysts, reactant should reach from bulk liquid to the surface
neutrilization-removal of soaps and salts, (2) vacuum of the catalyst, so stirring helps the reactant reach the catalyst’s surface
Evaporation-removal of methanol and water, (3) refining-improve pu and into the pores of the catalyst (Madhu et al., 2016). Kumari et al.
rity of glycerol. These post-treatment processes escalates overall cost of (2009) observed that the conversion rate is rising from 100 to 200 rpm,
biodiesel (IŞIK, 2021). Hossain et al. used methanol and NaOH as the but the conversion did not improve significantly at 250 rpm due to the
catalyst for waste sunflower oil transesterification and analyzed shear of the enzyme molecules. Therefore, the optimum speed for bio
different alcohol to oil ratios, finding a maximum conversion of 99% diesel production using enzyme reactions concluded as 200 rpm.
alcohol-to-oil ratios 6:1 (Binhweel et al., 2021; Hossain et al., 2010).
However, the yield was 49.5% in the study of transesterification in waste 6.8. Reaction temperature
canola petroleum by 1: 1 M methanol to oil (Binhweel et al., 2021).
The transesterification reaction is affected considerably by temper
6.5. Catalyst type ature, rate of reaction and product output increases as the temperature
rises. Biodiesel’s viscosity increases as reaction temperature fall below
Recently, different catalysts such as homogenous, heterogeneous and 50 ◦ C. In the case of waste cooking oil, it is pre-heated up to 120 ◦ C, then
enzymes produced alkyl esters. Vicente et al. (2007) have been using cooled down to 60 ◦ C (Daramola et al., 2016). Conversion increases for
several base catalysts and found that the NaOH as a catalyst is the an enzymatic reaction in a temperature zone of 30–55 ◦ C. For Jatropha
quickest among KOH, sodium methoxide and potassium methoxide oil, the highest conversion was reported at 55 ◦ C for lipase as a catalyst
(Refaat et al., 2008). concluded that KOH achieves the best conversion and 50 ◦ C for cottonseed oil (Shah and Gupta, 2007). Freedman et al.
performance among all catalysts mentioned. Various studies used sul (1984) found no change in temperature conversion at 45 ◦ C and 60 ◦ C.
furic acid as a catalyst for FAME production (Vyas et al., 2010), but At 32 ◦ C. The conversion was slightly lower than at 45 ◦ C and 60 ◦ C;
sufficient reaction time and severe reaction conditions are needed. Even conversion slightly increased after 4 h at 32 ◦ C than the conversion
1 mol% of the sulfuric acid can yield up to 99%. Acid catalyst (homo achieved at different temperatures. Refaat et al. (2008) analyzed do
genous/heterogeneous) as raw material for esterification reactions has a mestic and commercial (fresh and waste) oils using KOH as a catalyst
higher content of FFAs (Melero et al., 2009) and can be concurrently and recorded the maximum yield at 65 ◦ C. Liu et al. (2010) determined
used in the esterification and transesterification reactions(Su and Guo, that the reaction time to achieve biodiesel reduces significantly by using
2014). Soap formation and separation of catalyst from end product are radiofrequency heat.
the major problems of homogenous catalysis. Most researchers have
overcome this problem using heterogeneous catalysts, as FFA and 6.9. Reaction time
moisture content in the raw feedstock do not influence the heteroge
neous catalyst (Serio et al., 2007). The slowest reaction among all cat For a higher reaction time, it is feasible to achieve even 99% con
alytic reactions is the enzyme reaction, used for both esterification and version. The conversion is influenced by the availability of reactants in
transesterification reactions (Su and Guo, 2014). Separation of products the reaction mixture. There are chances of a backward reaction if the
becomes easier by using enzyme catalyst, but the crucial task is to pre reaction parameters are not precisely adapted, thereby reduction in
pare catalyst (Macario et al., 2010). conversion. The time required for a lipase-catalyzed reaction varies from
7 to 48 h (Silitonga et al., 2017). Researchers have reported that reaction
6.6. Catalyst concentration time also governs production costs. Al-Widyan and Al-Shyoukh (2002)
have studied that the specific gravity of the product decreases expo
The conversion of oil or fat to biofuel requires high-temperature nentially as reaction time increases, ending as an asymptotic value with
conditions in the absence of a catalyst (Chakraborty et al., 2011). The respect to time (Refaat et al., 2008). found the conversion of 96.10% for
product yield increases as the catalyst concentration rise; it is due to an 1 h, with no noticeable change in biodiesel conversion, for reaction time
improved reaction rate. Conversion falls with the excess amount of between 1 h and 3 h (96.350%), and the reaction time must be optimized
catalyst, which results in higher reaction mixture viscosity (Zhang et al., to bring down production costs.
2012). Many scientists have analyzed various catalyst concentrations
and regulated the catalyst concentration based on product yield and 6.10. pH
catalyst recovery (Chen et al., 2011). have used copper vanadium
phosphate, CuVOP and confirmed that 1.5% of the concentrations of In the reaction, pH is not an essential factor for base/acid catalyst.
catalysts are most effective in producing soybean oil biodiesel. Increased For the lipase catalyst, pH is a crucial factor, as enzymes may decompose
enzyme levels would increase the conversion rate. However, above the at lower or higher pH (Ganesan et al., 2009). investigated the pH effect,
specific threshold, enzyme agglomeration occurs, and the active position and they reported 7 as the optimal pH value for biodiesel production by
on the substrate decreases. (Molaei Dehkordi and Ghasemi, 2012) Jatropha oil using immobilized pseudomonas fluorescence.
analyzed CaO‾ and ZrO2‾, with different molar ratios of Calcium and
Zirconium, as heterogeneous solid catalysts concluded the higher yield 7. Effect of catalysts and different feedstocks on biodiesel
by raising the Ca/Zr ratio, leading to lower catalyst stability. Therefore, conversion
depending on the raw material and catalyst type, the optimum catalyst
concentration varies. Researchers have used both catalytic and non-catalytic routes for
biodiesel production from low-quality feedstock such as Karanja oil,
6.7. Stirrer speed Neem oil. Meher et al. (2006) used KOH as the catalyst for converting
Karanja oil to biodiesel. They produced more than 97% of the biodiesel
To complete the transesterification reaction and improve the pro within 3 h after using the oil to methanol ratio of 1:12, as shown in
duction of the FAME, the mixing of reactants is of great importance Table 6. A thin layer chromatography (TLC) tracks the completion of the
(Chakraborty et al., 2011). Agitation increases the collision between the transesterification reaction; A high-performance liquid chromatography
particles and diffuses particles in a catalytic mixture. On increasing, (HPLC) fitted with a refractive index detector analyses the trans
agitation speed reaction time decreases and conversion increases (Noiroj esterified sample composition. Spheri-5 C-18 column separates meth
et al., 2009). There would be no significant increase in yield beyond a anol (carrier solvent) with a flow rate of 1 mL/min. The injection was 20
certain speed of stirrer. Optimum stirrer speed varies for the different μL and compared by standards of methyl esters, monoglycerides, di
types of feedstock due to unique physical properties. For porous and glycerides, and triglycerides were carried out for peak detection.
9
Table 6
Effect of Catalyst and different Feedstocks on biodiesel conversion.
Sr Feedstock Alcohol Experimental conditions Catalyst Conversion Reference
No.
1 Pongamiapinnata Methanol Oil/Methanol molar ratio of 12:1, 65 ◦ C, 360 rpm, and 3 h KOH >97% Meher et al. (2006)
(Karanja) oil
2 Palm oil Methyl Methyl acetate/Oil molar ratio of 30:1, 400 ◦ C, 220 bar, None 99% Tan et al. (2011)
acetate and 1 h
3 Karanja Methanol 60–65 ◦ C, NaOH Bobade et al. (2012)
1 h (esterification then transesterification)
4 Karanja oil Methanol 6:1 M ratio of MeOH/Oil H2SO4 96.6–97%. Naik et al. (2008)
5 Neem oil Methanol 55 ◦ C, Oil/Methanol molar ratio of 12:1 (NaOH) 92% Radha (2011)
6 Vegetable oils Methanol 250–300 ◦ C None 95% in 10 Demirbas (2008)
min.
7 Neem oil Methanol 50 ◦ C, Methanol/oil ratio of 0.3:1 (Acid esterification and KOH Sathya and Manivannan
Alkaline transesterification) (2013)
8 Palm oil Methanol 64.72 ◦ C, Methanol/Oil Molar ratio 20:1 and 3 h NaAlO2/γ-Al2O3 ~97.65 Zhang et al. (2020)
9 Oleic acid Methanol 160 ◦ C, Methanol/Oil Molar ratio 20:1 and 6 h 25%MoO3/B- ~98 Mohebbi et al. (2020)
ZSM-5
10 Canola oil Methanol 65 ◦ C, Methanol/Oil Molar ratio 12:1 and 6 h KOH/ ~98.8 Kazemifard et al.
Fe3O4@Al2O3 (2018)
11 Sunflower oil Methanol 110 ◦ C, Methanol/Oil Molar ratio 12:1 and 4 h MgO/MgFe2O4 ~91.2 Alaei et al. (2018)
A single-stage method performed by (Tan et al., 2011) showed the ranges, sediment, the residue of carbon, sulfur concentration, presence
ability of supercritical methyl acetate (SCMA) to synthesize FAME and of glycerine and phosphorus (Refaat, 2009). The physical and chemical
value-added triacetin. Triacetin is an essential biodiesel additive that properties of biodiesel varied in accordance with the fatty acid compo
enhances the properties of FAME in cold environments. The producing sition (Ali et al., 2013).
FAME and triacetin together is very insightful and economical rather
than two separate reactions incurring higher production costs. At 8.1. Viscosity
400 ◦ C, a reaction time of 30 and 60 min yields 99 wt% of FAME and
triacetin. The SCMA process has a high tolerance for impurities like FFAs Viscosity plays a crucial role in fuel injection and spray atomization,
and water, usually available in waste oils/fats. mainly when a rise in viscosity affects fuel fluidity at low temperatures
It is also possible to use low-cost waste instead of high-quality refined (Krisnangkura et al., 2006). Biodiesel’s viscosity is 10–15 times higher
oil as a source of triglycerides. Bobade et al. (2012) used NaOH as a than fossil-fuel diesel due to its high molecular mass and complex
catalyst for Esterification, followed by the transesterification of the chemical composition (Kerschbaum and Rinke, 2004). Biodiesel is
Karanja oil. Naik et al. (2008) used sulfuric acid as the acid catalyst highly viscous at low temperatures or even solidifies, which results in
(Naik et al., 2008), resulting in a 97% conversion for oil to methanol the compromised mechanical stability of the pump drive systems (Yuan
ratio of 1:6. Researchers have also used different feedstocks such as et al., 2009). In accordance with ASTM D445 and EN ISO 3104, the
waste vegetable oil, palm oil, and neem oil to produce biodiesel. Neem maximum appropriate viscosity value is 1.9–6.0 mm2/s and 3.5–5.0
oil has been extensively used as the feedstock by the researchers with mm2/s (Lapuerta et al., 2008).
NaOH and KOH as a catalyst, achieving 92% conversion of the biodiesel.
Neem oil, a novel feedstock for biodiesel production, was used by
8.2. Fuel density and relative density
(Radha, 2011); they studied the effect of neem oil to methanol molar
ratio, acid & alkaline catalysts on transesterification. NOME (Neem Oil
The fuel density is the weight per unit volume; high-energy oils form
Methyl Ester) blended diesel emits less smoke and CO but higher NOX
a thick layer on the surface (Yuan et al., 2009). The biodiesel density
emissions than standard fossil fuel due to fuel’s oxygen content. More
measured at the reference temperature of 15 or 20 ◦ C complies with EN
than 15% of NOME-diesel mixtures produced low atomization and
ISO 3675/12 185 and ASTM D1298 under reference norm (Albuquerque
inadequate combustion in the engine. Table 6 includes various
et al., 2009). Calculation of relative density requires the mass to volume
non-edible oils and the effect of catalyst on conversion.
conversions, flow calculations and viscosity. The relative density of
biodiesel is a measure of homogeneity in biodiesel tanks (Pratas et al.,
8. Properties and qualities of biodiesel
2011).
The different sources of biodiesel is produce by varying the qualities

and properties of biodiesel. There is a need to normalize the quality of 8.3. Flashpoint
biodiesel to provide smooth engine operations (Zhou et al., 2003). The
Austria became the first country to set standards for esters as diesel fuel Flashpoint for a fuel sample is the lowest temperature at which liquid
obtained from rapeseed oil. In Italy, France, the Czech Republic, Ger fuel offer sufficient vapours to ignite when an ignition source is bought
many and the USA, standard qualities and properties of biodiesel were near the surface of liquid fuel and gives momentary flash. If this flash
defined (Atabani et al., 2012). Biodiesel’s properties and characteristics continues for more than 5 s, it is known as a fire point. The fuel volatility
must satisfy universal biodiesel specifications. These specifications are varies inversely with flashpoints. Biodiesel must have a flash point
compliant with the American Society for Testing and Materials (ASTM above the prescribed diesel fuel limit that is safe for transport, handling
6751-3) or the European Biodiesel Fuel Standards (EN 14 214) (Atadashi and storage (Kaisan et al., 2020). Flashpoint is higher than 150 ◦ C for
et al., 2010). The Czech Republic (ČSN), German (DIN 51 606), and biomass diesel, with flashpoint being 55–66 ◦ C for conventional diesel.
Austrian (ON) standards exist as well. Some of these properties are ce The flashpoint values for Fatty Acid Methyl Esters have been found
tane number, flash and fire point, calorific value, acid value, cloud and significantly below their vegetable oils (Lvarez et al., 2019). The flash
pour point, density, viscosity, ash content, copper corrosion, distillate point limit is 93 ◦ C in ASTM D93 and 120◦ C in EN ISO 3679 (Mejía et al.,
2013).
10
8.4. Pour point, cloud point, and cold filter plugging point 8.9. Acid value (AV) or Acid number
The low-temperature properties of biodiesel are critical for flow and FFA is a monocarboxylic acid saturated or unsaturated in fat, oil or
engine operation as fuel may be partially or fully solidified, leading to grass naturally without being attached to the backbone of glycerol (Pua
fuel hunger, starter problems, driving and damage to the engine due to et al., 2012a, 2012b). The increased acid value is a higher FFA level in an
inadequate lubrication (Echim et al., 2012). The cloud point is the engine fuel supply chain that induces extreme corrosion. The acid value
temperature at which when the fuel gets chilled, resulting in a cloudy or is defined as the milligram of KOH needed to neutralize 1 g of FAME.
hazy appearance due to the formation of wax crystal (Yuan et al., 2017). ASTM D664 and EN 14104 calculates the acid value. A maximum acid
Pour point is the temperature at which the complete wax out of solution value of 0.50 mg of KOH was accepted for both standards for biodiesel
is sufficient to gel the fuel, and fuel ceases its flow. The ASTM D2500, EN (Wang et al., 2017).
ISO 23 015 and D97 are used for the calculation of pour point. The cloud
point and pour point of biodiesel is higher than conventional diesel 8.10. Free glycerine
(Hájek et al., 2006). The temperature at which the test filter begins to
plug as the fuel components have started crystallizing is the cool filter The amount of glycerol leftover in the finished biodiesel is free
drop-in point (CFPP) (Giakoumis and Sarakatsanis, 2018). CFPP reflects glycerol. The free glycerol in biodiesel varies according to the
its winter weather efficiency as a proxy for the low-temperature oper manufacturing process. During washing of ester product, glycerol may
ability of fuels. At low operating temperatures, fuels thickening creates a remain in biodiesel due to inefficient separation. Glycerol is insoluble in
problem in the flow, affecting fuel lines, pumps, and injectors. CFPP biodiesel, and it is easy to settle or centrifuge nearly all the glycerol. Free
determines the filterability cap for fuels, which has a greater correlation glycerol may cause coking injections and fuel damage (Alves et al.,
with biodiesel and diesel than the cloud level. ASTM D6371 is used to 2016). The ASTM specification restricts the overall glycerol of the final
calculate the CFPP (Sarin et al., 2010). biodiesel commodity should be less than 0.24 %. A gas chromatograph
measures free glycerin in ASTM D6584 and EN 14105/14106. The
8.5. Cetane number maximum permissible amount of free glycerine is 0.02% (Falahati and
Tremblay, 2012).
The cetane number (CN) of fuels indicates the ignition features or the
capacity for automatic ignition after injection. The higher CN value is 8.11. Total glycerine
also related to better ignition efficiency and lower ignition delay. CN is
one of the most significant factors for ethyl or methyl ester using bio The cumulative amount of triglyceride residue in methyl esters is
diesel (Ramadhas et al., 2006). Increasing the length of the fatty acid total glycerine; hence the sum of free glycerine, monoglycerides, di
chain and saturation, CN increases. A higher CN is the indicator of lesser glycerides and triglycerides are total glycerin. A molecule of a methyl
time between ignition and fuel injection initiation into the engine ester of fatty acid gets produced in each reaction stage. If the reaction is
combustion chamber. Biodiesel has higher CN than traditional gasoline, incomplete, the reaction mixture is supposed to contain triglycerides,
which indicates better performance in combustion. ASTM D613 and EN diglycerides and monoglycerides (Silva et al., 2012). All these com
ISO 5165 has defined CN of diesel as 47 and 51.0 min (Giakoumis and pounds already have a non-released glycerol molecule referred to as
Sarakatsanis, 2018). bound glycerol in these compounds. The sum of free glycerol and
bounded glycerol is called total glycerol. According to ASTM D 6584 and
EN 14105 specifications, total glycerol in final biodiesel must be less
8.6. Titre
than 0.24% and 0.25% (McNeil et al., 2012).
Titre is known as the temperature at which solidified oil changes to
8.12. Carbon residue
fluid fuel. Titre is vital because the biodiesel production process is a
liquid operation, and oils with high Titre needs heating, raising energy
After combustion, the carbon depositing property of fuel is the
demand and production cost for a biodiesel plant (Hu et al., 2019).
measure of carbon residue. Carbon contamination strongly links with
fatty acids, soap, glyceride, polymers and inorganic impurities (Kaisan
8.7. Oxidation stability of fuel et al., 2020). While not just carbon contamination, all the criteria
include the word ‘carbon residue’. The limitation of the ASTM D4530
One of the valuable factors for evaluating biodiesel quality includes and EN ISO10370 norms for carbon residue is 0.05% and 0.30% (Lin
the oxidation properties of the fuel. The possible reactivity with air and and Li, 2009).
the need for antioxidants are indicators of oxidation stability (Pullen and
Saeed, 2012). Oxidation occurs due to the inclusion of unsaturated fatty 8.13. Ash of sulfate
acid chains in molecules, which reacts immediately upon exposure to
air. Due to the chemical composition of biodiesel, it is more sensitive to Ash material identifies inorganic contaminants such as rough solids,
oxidative degradation than fossil diesel fuel. In ASTM D6751 and EN 14 catalyst remains and soluble metal soap in fuel. An ignition, burning,
214 Rancimat method is oxidation stabilization requirements. For ASTM and the treatment with sulfuric acid determines the percentage of
D6751, IP (110◦ C) at least 3 h is sufficient, while EN 14 214 defines a sulfated ash present in biodiesel (Chaves et al., 2010). The ASTM D874
more stringent limit of 6 h or more (Yaakob et al., 2014). standard allows a maximum of 0.02% of the sulfated ash extracted from
the samples (Hansen et al., 2013).
8.8. Lubrication properties of fuel
8.14. Visual inspection
Atadashi et al. (2010) suggested that biodiesel significantly increases
the lubricity of diesel fuel, and improves engine life. Lapuerta et al. Visual inspection determines to amount of water and particulates in
(2008) claimed that FAME’s drawbacks depend on the degradability, the biodiesel. The haze value is calculated by putting a chart behind a
glycerol content, and cold flow properties and contribute to forming transparent bio-diesel bottle, which refers to how six separate photos of
deposits, but it has better lubrication properties. A high value of bio haze levels between 1 and 6 equate the axes. Where 1 signifies the least
diesel lubricant property could reduce friction loss and improve brake particulate level and six indicates the highest. Hence, haze 1 signifies the
efficiency (Dunn and Bagby, 1995). fuel is clearest (no particulates and water), and Haze 6 signifies cloudy
11
fuel (Tang et al., 2008). The ASTM D4176 is generally used to determine hydrogen bond donor and hydrogen bond acceptor in a fixed molar
visual biodiesel inspection (Zimmer et al., 2013) ratio. The DESs so formed have melting points lower than either of
hydrogen bond donor or hydrogen bond acceptor. The lower melting
point of DESs is due to the hydrogen bond formation between the
8.15. Presence of metals in biodiesel
hydrogen bond donor and acceptor. DESs are considered as designer
solvents since depending on the application DESs, they can be tailored
According to ASTM D6751, should be below 10 ppm and combined
made by combining different types of hydrogen bond donor and
Ca, and Mg should be below 5 ppm. ASTM D4951 decides phosphorus
acceptor. DESs could be the catalyst for biodiesel production reaction
existence while EN Norm 14538 decides calcium and magnesium traces
and green solvents for extraction of FAME (Lu et al., 2016). For single
(Chaves et al., 2010).
and multiple-step methods, DESs are used as catalysts (Mamtani et al.,
2021). In the second process, feedstock containing high FFA accom
9. Use of deep eutectic solvents (DESs) in production of biodiesel
panies alkaline catalytic transesterification after esterification (Alomar
et al., 2016). DESs are used to improve the catalytic capability of catalyst
DESs play an influential role in biodiesel production like Ionic Liq
or biocatalyst by using them as a co-solvent with them (Škulcová et al.,
uids (ILs). DES are considered as ILs analogue having greener properties
2016). They may also reduce side reactions (e.g. saponification) and
such as high thermal and chemical stability, non-corrosiveness, and
simplify the separation of catalyst and purification of the final product
negligible vapour pressure (Haider et al., 2021). DESs are formed by the
Table 7
Usage of DESs as a catalyst in the production of biodiesel.
Raw Reactor type, Alcohol Methanol DES amount Other catalyst Temperature, Optimum reaction Conversion Reference
material size cm3/ to oil molar (wt%) amt wt% (to oil ◦
C conditions (C) or yield
agitation speed, ratio weight) (Y)/time, h
rpm
Soybean oil Round-bottom CH3OH 10:1–30:1 ChCl:ZnCl2 – 50–90 70 ◦ C,10 wt%, 16:1 54.52(C)/72 Long et al.
flask/100 (1:2)/10.0 (2010)
wt%
Palm oil Three-neck CH3OH 10:1–15:1 ChCl:ZnCl2 95.0% H2SO4/ 65 65 ◦ C,2.5 wt%, 15:1 70.4 (Y)/4 Zhang et al.
flask (1:2)/ 20.0 wt% 67.4 (Y)/4 (2016)
0.5–2.5 wt% 92.0 (Y)/4
ChCl:FeCl3 89.5 (Y)//4
(1:2)/
0.5–2.5 wt%
ChCl:ZnCl2
(1:2)/2.5 wt
%
ChCl:FeCl3
(1:2)/2.5 wt
%
Palm oil, Batch reactor/ CH3OH 4:1–20:1 DEAC:PTSA – 40–80 I stage: 60 ◦ C,8:1,0.75 wt 97.0 (Y)/0.5 Hayyan et al.
(9.5% motor driven, (1:3)/ %,200 rpm (2013b)
FFA) 100–500 0.25–3.5 wt
%
Esterified 10:1 KOH/1.0 wt% 60 II stage:60 ◦ C,10:1,1.0 wt 84.0 (Y)/1 Hayyan et al.
oil (0.7% % catalyst,400 rpm (2013b)
FFA
Palm oil, Reactor CH3OH 3:1–20:1 ChCl:PTSA – 40–70 I stage:60 ◦ C,10:1, 0.75 97.0 (Y)/0.5 Hayyan et al.
(9.0% (1:3)/ wt%, (2014)
FFA) 0.25–3.50 wt
%
Esterified Batch, 1500/ 10:1 – KOH/1.0 wt% 60 II stage:60 ◦ C,10:1,1.0 wt 92.0(Y)/1 Hayyan et al.
oil (<1% mechanical, % cat (2014)
FFA) 400
Palm oil – CH3OH 1:1–20:1 P-DES (1:3)/ 40–80 I stage:60 ◦ C,10:1,1.0 wt 96.0 (Y)/0.5 Elgharbawy
(9.3% 0.25–3.5 wt %, 300 rpm et al. (2021)
FFA) %
Esterified – CH3OH 10:1 – KOH/1.0 wt% 60 II stage:60 ◦ C,10:1,1.0 wt 89.84 (Y)/1 Zhang et al.
oil % cat,400 rpm (2016)
(0.88%
FFA)
Rapeseed Batch/plumb CH3OH 14.28:1 ChCl: 8.07 wt% CaO 65 65 ◦ C, 14.28:1; 10.74 wt 91.9 (Y)/3 Huang et al.
oil stirrer, 400 glycerol (commercial) %,8.07 wt% CaO; (2013)
(1:2)/10.74
wt%
Miglyol Micro-reaction CH3OH ChOAc: Novozym 435/ 50 50 ◦ C,1.0 mL mixture of 97.0 (C)/3 Gu et al.
812 vessel, 5/gentle glycerol 27.3 wt% DES and CH3OH 27.3 wt (2015)
(1:1.5) % lipase;
Soybean oil Micro-reaction CH3OH ChCl: Novozym 435/ 50 7:3 (v/v) of DES and 88.0 (C)/24 Zhao et al.
vessel, 5/mild glycerol (1:2) 20.0–60.0 wt% CH3OH, 40.0 wt% lipase, (2013)
M. pinnata Round bottom CH3OH 3 mL/mg ChOAc: P. expansum 50 50 ◦ C,3 mL methanol/mg 7.6 (C)/48 Huang et al.
seed flask/stirrer, oil glycerol lipase/1.0 wt% oil; 7 mL DES/g oil; 1.0 54.8 (C)/48 (2013)
220 (1:2)/7 mL Novozym 435/ wt% lipase; 44.8 (C)/48
DES/g oil 1.0 wt%
Lipozyme
TLIM/1.0 wt%
12
(Sander et al., 2018). Many DESs are capable of removing glycerine and or sucrose facilitate phase separation and enables DESs to be recycled
remaining catalyst from the mixture (Kadapure et al., 2017). (Kalhor and Ghandi, 2019). The hydrophobic DESs are easier than hy
drophilic DES to be recovered by membrane technology (Procentese
9.1. Deep eutectic solvents in transesterification as catalysts et al., 2015).
DESs have recently gained attention to be used as a catalyst in

9.3. Recovery of deep eutectic solvents
various applications. Since the DESs are composed of hydrogen bond
donor and hydrogen bond acceptor mixed in a fixed molar ratio. DESs
DESs recovery depends upon the system’s phase; for a bi-phase or
are also used as a catalyst for transesterification reaction for biodiesel
multi-phase system, recovery becomes more straightforward (Petračić
production, as shown in Table 7. Long et al. studied methanolysis of
et al., n.d.). In transesterification of Rapeseed oil using NaOH as catalyst
soybean oil with the Lewis acid catalyst, Choline chloride: Zinc chloride
and ChCl: glycerol as cosolvent, after completion of the reaction, a
(1:2) (Long et al., 2010). Major advantages of this DES include ease of
biphasic system forms, and further separation occurs (Gu et al., 2015).
preparation (Haider et al., 2018), cost-effectiveness (Maheshwari et al.,
For DES recovery, methanol evaporates by freezing the mixture at 0 ◦ C
2021), less water sensitivity (Maheshwari et al., 2021) and the
(Shahbaz et al., 2011a), followed by the centrifugation of DES. For the
requirement of mild reaction parameters (Haider et al., 2019). For
formation of FAME using CaO catalyst and DES (ChCl: glycerol, 1:2),
transesterification of palm oil by Choline chloride (ChCl): Zinc chloride
three layers form after completing the reaction. (Lee et al., 2016). The
(1:2) and Choline chloride: Ferric chloride (1:2), the yield of 67.4% and
top layer contains ester; the middle layer contains a mixture of DES,
70.4% were achieved (Mohammad Fauzi and Amin, 2012). As ChCl
glycerol, and methanol; the bottom layer has CaO. This filtered catalyst
ZnCl‾5 has added H2SO4 (95% volume), ester production has risen to
is washed with ethanol and dried at 70 ◦ C for 24 h(Huang et al., 2013).
92.0% (Disale et al., 2012). In bio catalyzed biodiesel production, DESs
Two layers of the DES-containing mixture are formed in the short span of
have advantages such as low cost, non-toxicity, biodegradability, and
30 s and separate the insoluble DES-methanol-glycerol system from
more compatibility over lipase (Kim et al., 2016).
FAMEs. In the top phase, the desired product exists, while DES, glycerol
In dual step processes, DESs comprised of esterification of crude oil
and methanol are present in the lower phase, and Novozym 435 exists
palms having high FFA, followed by transesterification using KOH as the
between these layers (Liu et al., 2019). Water and diethyl ether used for
catalyst (Hayyan et al., 2013b). decreased oil FFAs from 10% to 1% by
washing the enzyme obtained after filtration from the reaction mixture
pre-treatment using DEAC: PTSA (1:3). Researchers have also used
is further dried.
P-DES (molar ratio 1:3) (Hayyan et al., 2014) for the reduction of the
amounts of FFAs in the oil from 9.3% to less than 2.0% and ChCl:
p-toluenesulfate acid (1:3 M ratio) (Shahbaz et al., 2011b) to decrease 9.4. Reuse of DESs
FFA from 9.1% to less than 1.0%. Many DESs are efficient in biodiesel
production along with other catalysts. Choline Chloride: glycerol (1:2) Even after being used several times, no notable decrease in the cat
removes idle layers of calcium carbonates and calcium hydroxide to alytic activity of many reused DESs is detected (Hayyan et al., 2013a,
activate commercial CaO (Huang et al., 2013). Biodiesel production 2014; Liu and Wang, 2018). The catalytic literature on recycled DESs
from rapeseed oil with Calcined CaO provides the FAME conversion of discussed in Table 8 highlights the applications of several DESs, con
86.9% and 94.8.0% in the absence and presence of the DES (Huang version of initial and final levels, the total number of cycles used and
et al., 2013). Non-calcinated CaO does not work effectively (4.0% yield), yield at the first and final run.
but the ester yield increases to 91.9% when used with DES (Reyero et al.,
2014). DESs can act in various forms, such as catalyst, solvent promoter, Table 8
and co-solvent in transesterification/esterification reactions. For Recycled DESs used in Biodiesel production.
example: due to the weakly acidic nature of Zn2Cl5‾ low conversion is DES Feedstock Alcohol No. of Conversion (C) or Reference
obtained by DES, ChCl: ZnCl2 (1:2) (Shahbaz et al., 2011b). CH3OH and cycles yield (Y) %
Choline chloride (ChCl): Glycerol (1:2) mixture dissolves deactivated First Final
layers of calcium hydroxide and calcium carbonates from the CaO cycle cycle
catalyst surface due to their high solubility to make better contact be DEAC: Palm oil, CH3OH 4 93.0 87.0 Hayyan
tween CaO and the reactants (Huang et al., 2013). Moreover, in the PTSA low grade (Y) (Y) et al.
NaOH-catalyzed transesterification process of rapeseed oil same DES is (1:3) (2013b)
used due to the immiscibility of FAME in DES/methanol mixture, con P-DES Palm oil, CH3OH 4 91 (C) <80.0 Liu and
(1:3) low grade (C) Wang
tact between NaOH and FAME significantly reduced (Avhad and Mar
(2018)
chetti, 2016). ChCl:PTSA Palm oil, CH3OH 3 95.82 94.8 Hayyan
(1:3) crude (Y) (Y) et al.
9.2. Recyclability of DESs (2014)
ChCl: Rapeseed CH3OH 5 92 (Y) 85.0 Huang
Glycerol oil (Y) et al.
In successive steps, recyclability involves the separation, purification (1:2) (2013)
and reuse of DESs (Tang et al., 2020). In the recycling of DESs, they are ChCl: Soybean CH3OH 4 88.0 79.0 Zhao et al.
separated from the final mixture of unreacted feedstock and product and Glycerol oil (C) (C) (2013)
purified before reuse. It has a significant effect on the economic and (1:2)
TBAC-AA Palmitic CH3OH 94.3 Lee et al.
environmental aspects of manufacturing processes (Homan et al., 2017).
– –
(1:2) acid (C) (2016)
DESs usually cost more than organic solvents and significantly influence Imidazole- IBAc Iso 6 – 92.5 Qin et al.
overall process cost (Wu et al., 2009), so recovering, reusing, and PTSA butanol (C) (2019)
recycling DESs make them more economical. The waste catalyst disposal (1:2)
ChCl-CSA Sludge CH3OH 2 96.5 Hayyan
can have adverse environmental effects. The composition and combi –
Palm Oil (C) et al.
nation of hydrogen bond donor (HBD) and hydrogen bond acceptor + Crude (2014)
(HBA) of DESs strongly influence recycling (Ling et al., 2020). Hydro Palm Oil
phobic DESs are more suitable for chemical reactions since a multi-phase CTAB- Lauric C2H5OH 6 – 85.2 Liu et al.
system forms at the end of the reaction (Petračić et al., n.d.). Biphasic PTSA Acid (C) (2019)
(1:3)
systems formed by the addition of hydrophilic DESs with potassium salt
13
The catalytic system with 95 vol% of H2SO4 and Choline Chloride: such as glycerol. The review highlighted the potential of various DESs
Zinc chloride (1:2) used for palm oil transesterification is isolated from over conventional solvents. DESs may play a vital role in bringing down
the reaction mixture by freezing, centrifugation and successfully re the cost as they are synthesized in-house, whereas Ionic Liquids are
generated (Bjelić et al., 2020). At the end of 5 runs, the ester yield de much costlier than DESs. The proper combination of HBA, HBD, along
creases by 30.0%. In biodiesel production from low-grade palm oil, N, with recyclability and reusability of DESs, will lower down cost drasti
N-diethylenethanol ammonium chloride, and p-toluenesulfonic acid cally (Chen and Mu, 2021). There is very limited literature available on
(PTSA)monohydrate (Hayyan et al., 2013b) have good recyclability. the economic prospects of DESs for cleaner biodiesel production.
Choline chloride and p-toluenesulfonic acid monohydrate (molar ratio Recently, various studies used different feedstock sources to calcu
1:3) do not suffer a substantial loss of activity after 3 runs (conversion late the total cost of biodiesel production. For instance, the total esti
level 89.0%, yield 95.0%) (Rasul et al., 2014). In rapeseed oil meth mated process cost of biodiesel from the crude palm oil was calculated as
anolysis, ChCl: glycerol activated commercial CaO (1:2) guarantees a 0.819 USD/L while the highest total cost to the feedstock cost was 0.723
FAME conversion of 85% after 5 runs without addition to DES (Troter USD. The lowest total production cost using tallow was 0.623 USD/L,
et al., 2018). In soybean oil, methanolysis, which has an enzyme used 4 which incorporates the cost of feedstock as 0.4 USD/L (Demirbas,
times without any significant loss of activity, is consistent with Novozym 2009b).
435 (Zhao et al., 2013). According to the total cost estimate by the National Renewable En
ergy Laboratory in the United States, the cost of cleaner biodiesel pro
10. Prospects and perspective duced from algae was in the range of 0.523–0.84 USD/L. Moreover, the
total cost of produced biodiesel was around 0.72–0.97 USD/L in 2019 as
The current energy scenario shows that biodiesel as one of the key calculated by different sources from government databases and various
component for reducing the energy dependence on fossil fuels. The sellers (Chen and Mu, 2021). The trend depicts that there is a marginal
production and consumption of biodiesel have grown significantly over difference in the price of biodiesel production since the last decade. The
the years and this trend will keep on growing keeping into the view on inclusion of reusable solvents like DESs along with non-edible oils can
sustainable development and energy norms. For example, in several bring down costs.
countries such as India mixing biodiesel with diesel has already become
the norms and newer policies are framed to reduce fossil fuels depen 12. Conclusions and recommendations
dence. The cost of biodiesel is still more compared to mineral oil and this
need to be minimized. The researchers are focused more on finding the Biodiesel emerged as a potential alternative fuel to reduce the
economical feedstocks and the catalyst. dependence on fossil fuels. It will not only reduce anthropogenic emis
Despite various research in searching the economical feedstocks and sions but also has the potential to boost the local economy. This review
catalysts for biodiesel production, there are still some limitations. The aimed at the use of non-edible oils as the potential feedstock and dis
principal barrier for biodiesel production is its feedstocks which cussion of various catalysts for cleaner biodiesel production. The choice
contribute maximum to its cost. Ideal feedstock should not only be of feedstocks is a key factor for deciding the quality and the cost of
readily available in abundance but it should also not cause the food vs biodiesel produced. Non-edible oil is a potential feedstock for biodiesel
fuel debate. This can be achieved through the low-quality feedstocks production to reduce the dependency on edible oil to avoid the fuel vs
which should be readily available and requires less land for cultivation. food battle. Even though many non-edible oils are key candidates for the
The major limitation for the feedstocks is their availability. The feedstocks, their availability is the major issue. Waste cooking oil can be
distributed feedstock sources make it difficult to control the biodiesel emerged as the economically viable and sustainable feedstock for bio
quality. Unlike developed countries where edible oil is abundant, for diesel production.
developing countries waste cooking oil can emerge as one of the key DESs has shown potential to be used as solvent and catalyst for
feedstock for biodiesel production. The economical feedstocks with their biodiesel production having a significantly lower cost than ionic liquids.
constant availability are still needed to investigated and depend signif They have shown catalytic activity similar to conventional catalysts. In
icantly on the country. the future, such solvents will play a crucial role in cleaner production in
The choice of catalyst is also a key parameter for defining the bio a sustainable manner. The DESs could be critical solvents and act as
diesel cost. Even though researchers are working on developing various perfect enzymatic catalysts depending on HBA and HBD for cleaner
catalysts but the feasibility of the catalyst still needs to be decided based biodiesel production from waste oils. To reduce overall cost, DESs are
on pilot plant performance. The catalyst cost can be minimized by using economical and green solvents. P-toluenesulfonic acid-based DESs
a catalyst that is easy to synthesize and requires minimum to no puri observed the highest conversion (~95%) in transesterification among all
fication step. The DESs emmerged as one of the potential alternatives for the discussed DESs. Another important aspect of work could be the use
biodiesel production. However, the raw material cost along with the of water in different proportions along with different combinations of
separation of catalyst from the product formed as well as purification of HBA and HBD, which could drastically reduce the viscosity of the sol
biodiesel is a major challenge that needs to be investigated and should vents and enhance the operability and mass transfer.
require a minimum cost. The catalyst should not be degraded and can be
used for multiple times with high selectivity. DESs being designer sol Declaration of competing interest
vents offer opportunities for developing new materials having desirable
properties keeping in view the sustainable development. Major studies The authors declare that they have no known competing financial
focused on studying the common properties of DESs instead of devel interests or personal relationships that could have appeared to influence
oping new methods and tools to screen the DESs. There is a very poor the work reported in this paper.
understanding of the molecular aspects of DESs for biodiesel production.
Moreover, life cycle analysis and economic analysis for biodiesel pro Acknowledgement
duction using DESs is almost absent.
This research has been supported by the project Sustainable Process
11. Economical perspective Integration Laboratory – SPIL, funded as project No. CZ.02.1.01/0.0/
0.0/15_003/0000456, the Operational Programme Research, Develop
The economic performance of reviewed cleaner biodiesel domi ment and Education of the Czech Ministry of Education, Youth and
nantly depends on two factors: (1) cost of feedstock and catalysts and (2) Sports by EU European Structural and Investment Funds, Operational
market selling price of the cleaner biodiesel and various by-products Programme Research, Development and Education.
14
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Journal of Cleaner Production 355 (2022) 131588

Contents lists available at ScienceDirect

Journal of Cleaner Production

A review on latest trends in cleaner biodiesel production: Role of feedstock,

Energy is indispensable for existence, and it has become an absolute

Biodiesel is equivalent to processed diesel fuel that originates from

vegetable oils, designated as B100 (Zhang et al., 2003). (Haas, 2005).

Sr3Al2O6 3 Methanol Soyabean Oil 25:1 60/1 ~96 Rashtizadeh et al.

For engine operation, vegetable oil is diluted with diesel. In 1980,

Microemulsion describes a dispersion of optically isotropic fluid

Fig. 6. Acidic catalytic transesterification mechanism of vegetable oils (Demirbas, 2008).

(Elgharbawy et al., 2021). Homogenous base catalyst forms soap that

6.3. Type of alcohols

Methanol is used chiefly for biodiesel because of straightforward

The different sources of biodiesel is produce by varying the qualities

DESs have recently gained attention to be used as a catalyst in

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