Fuel 306 (2021) 121632

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Fuel
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Full Length Article

A review on nano-catalysts and biochar-based catalysts for

biofuel production
Karthik Velusamy a, Jamunarani Devanand b, Ponnusamy Senthil Kumar c, *,
Kalaivani Soundarajan d, Veena Sivasubramanian e, Jaisankar Sindhu a, Dai-Viet N. Vo f
a
Department of Industrial Biotechnology, Government College of Technology, Coimbatore 641013, India
b
Department of Mechanical Engineering, Government Polytechnic College, Coimbatore 641014, India
c
Department of Chemical Engineering, Sri Sivasubramaniya Nadar College of Engineering, Chennai 603 110, India
d
Department of Electronics and Communication Engineering, Government Polytechnic College, Coimbatore 641014, India
e
Department of Mechanical Engineering, Government Polytechnic College for Women, Coimbatore 641044, India
f
Center of Excellence for Green Energy and Environmental Nanomaterials (CE@GrEEN), Nguyen Tat Thanh University, Ho Chi Minh City, Viet Nam

A R T I C L E I N F O A B S T R A C T

Keywords: Necessity and exploitation of fossil fuels is unstoppable in meeting humanity’s needs despite being a small and
Biofuels scarce resource. The use of different renewable feedstock materials are vital in the satisfaction of large-scale
Homogeneous catalysts demand for renewable energy sources without creating environmental problems in order to satisfy energy de­
Heterogeneous catalysts
mand. In this context we covered the production of biofuels from a variety of feedstocks using pyrolysis, direct
Nanocatalysts
blending, micro-emulsion, trans-esterification (biodiesel production techniques) and hydrolysis, acidogenesis,
Synthesis techniques
Renewable energy acetogenesis, methanogenesis (biogas production techniques) and pyrolysis, thermochemical liquefaction (bio-
oil production techniques) along with the focus on increasing biofuel production using nanocatalysts and
biochar-based catalysts and the techniques for creating those catalysts. Torrefaction, pyrolysis, hydrothermal
carbonization, hydrothermal liquefaction, and gasification are the key methods used to make biochar. Slow
pyrolysis and hydrothermal carbonisation are the best methods to produce high-yield biochar. Biochar’s catalytic
activity is influenced by pyrolysis temperature, pyrolysis time, transition metals, and biomass to water mass
ratio. However, there are some noteworthy challenges associated with biofuel development. The cost of feed­
stock and the option of convenient technology for efficient fuel production, the availability of commercially
viable nanoparticles, a biological understanding of the nanomaterial and protein system, and microorganism
compatibility levels involving enzymes and nanomaterials are all discussed repeatedly.

1. Introduction than 2.7 Million Barrels Oil every day (MMbed) in 2023. Asia is the
leading consumer growth for biofuels as a result of growing transport
Fuels are in high demand for a variety of activities, including fuel use. Biofuels are the major drivers for biofuel usage in the world­
transportation, not only in urban areas but also in rural areas these days. wide transport industry. Brazil, China, Europe and the US, which
Meanwhile, crude oil prices are rising, and fossil fuel resources are constitute around 90% of worldwide biofuel use, according to the IEA,
diminishing, all of which have a significant environmental impact. As a are the leaders in biofuels consumption. While Asian consumption will
result, researchers are currently paying attention to an alternative for grow in the early 2020 s, several nations across the world take measures
fossil fuels in order to meet society’s demands through renewable re­ to enhance their overall energy mix using biofuels. [2]
sources. Presently 4.7 percent of the output of liquid transport fuel The concept of biofuel production and use, has been debated for
comes from regenerative sources. Biodiesel, bio-oil, and biogas pro­ many years, but is less efficient to produce and use because advanced
duction are prioritised on this list. [1] techniques are not incorporated in easy steps[3]. Fermentation, trans­
According to the 2017 medium-term report on renewable of IEA, esterification, gasification, quick and slow pyrolysis are involved.
global output of biofuels is expected to rise by roughly 16% to higher Typically, gasification includes the incomplete oxidation of biomass into

* Corresponding author.
E-mail address: [email protected] (P. Senthil Kumar).

https://doi.org/10.1016/j.fuel.2021.121632
Received 13 May 2021; Received in revised form 15 July 2021; Accepted 1 August 2021
Available online 11 August 2021
0016-2361/© 2021 Elsevier Ltd. All rights reserved.
K. Velusamy et al. Fuel 306 (2021) 121632

high-temperature fuel vapours (>800 ◦ C). It generates a combination of

CO, H2, CO2 and certain light hydrocarbons generally using air or steam.
The thermal pretreatment of biomass in a temperature variation be­
tween 200 and 300 ◦ C in an oxygen-free environment is the torrefaction.
[94]
Fast pyrolysis is used for procedures with an intensive heat treatment
duration of extremely brief residency at 400–600 ◦ C from 0.5 to 3 s.
Biomass is quickly cooked to a high temperature when there is no ox­
ygen in the quick pyrolysis process. Typically, quick pyrolysis generates
60 percent to 75 percent of oils with 15percent to 25 percent of the solids
(mostly charcoal) and 10 percent to 20 percent of the gas phase ac­
cording to the feedstock implemented.[4]
Since thousand years, slow pyrolysis has been utilised to elevate
production of biofuels at small temperatures and poor heating rates. The
vapour residence period is therefore excessive (5 min to 30 min) and
components continue to react with one other throughout the vapour
phase, which leads to solid char and other fluids production.[4]. Cata­
lysts play a very crucial role in all of these processes. The presence of
catalysts usually improves the manufacturing process in order to easily Fig. 1. Classification of Magnetic nano particles.
access the desired product.
There are two classifications of catalysts: homogeneous catalyst 2.1.1. Metals/Alloys based nanoparticles for biofuel production :
bases / acids and heterogeneous base / acid. In the production of bio­ A few examples of metal-based magnetic nanparticles are Cu-Co, Au/
fuels, homogeneous catalysts like KOH , H2SO4 and NAOH are used. Ag, and Mg/Al. Chen has shown that Cu-Co is active with a catalytic
However, the disadvantage of using this type of catalyst is that it is dimensions of 60 nm for direct heating, with reaction rates of up to
difficult to recover and the separation process involves a large number of 99.40 percent[13]. In the same vein Au/Ag with catalyst dimensions of
steps. To overcome this limitation, heterogeneous base/acid catalysts 28 nm was active with reaction rates of up to 86.90 per cent[14]. Deng
are used. The benefits of using a heterogeneous catalyst include easy has shown that the co-precipitation method is used with Mg/Al catalysts
separation, little or no corrosion, and low environmental pollution with size of 7.3 nm with reaction rates of up to 95,20%.[15]
(Wang et al., 2019).
Researchers are currently focusing on green catalysts. Green cata­ 2.1.2. Metal oxide based nanoparticles for biofuel production :
lysts are those that are made from biomass and are typically inexpensive A few instances include CaO,MgO, MgO–AlO3, CaO–Al2O3 based on
and reusable. Biochar-based catalysts and nanocatalysts realise re­ metal oxide magnetic nanoparticles. CaO or MgO are often doped with
searchers dreams of producing biofuels that are both effective and base mixed metal oxide to enhance their catalytic activity. The catalysts
friendly to the environment and society [5,6]. Biochar can be turned into are showing enhanced activity in the conversion to biofuel. The sol–gel
a catalyst for the production of biofuel as a porous carbonate compound techniques were used to generate the MgO–AlO3 and CaO–Al2O3 cata­
formed from different biomass. Biochar-based catalysts are useful lysts. These catalysts have been shown to be efficient during the trans­
because they contain inorganic groups such as K and Fe on their surface, esterification of lipids from microalgae.
which can be used in tar cracking, as well as other functional groups that [16]
aid in the adsorption of metal precursors. As a result, the emphasis is
shifted to nano catalysts and biochar-based catalysts. The advantages of 2.1.3. Iron based nanoparticles for biofuel production:
using nano and biochar-based catalysts include simple catalyst synthe­ 90 percent of the response yield was reached with Fe3O4 as a catalyst
sis, low cost, easy disposal, reusable properties, and increased biofuel and 11.2 nm dimension and co-precipitation.[17]Feyzi also produced a
yield[3,7,8]. ferrite-based Cs/Al/ Fe3O4 catalyst dimension of 30–35 nm utilising the
Biochar can be generated from lignocellulosic biomass, non- precipitation technique, with reaction yields up to 94.80%. [18]
lignocellulosic biomass, and lignin-based biomass. All of these bio­
masses are converted to biochar via pyrolysis, carbonization, and gasi­
fication. Biochar-based materials and nano catalysts are used for 2.2. Techniques
refinery process catalysis, biofuel production, and air pollution control
[9,10]. As a consequence, this review provides a clear picture of the Novel nanocatalysts are created using techniques like co-
purpose of selecting biochar-based catalysts and nano catalysts for precipitation, the sol–gel process and metal impregnation. The vast
biofuel production, as well as the various techniques for producing these majority of them are solid acid homogeneous/heterogeneous nano­
catalysts and their effective role as a catalyst. catalysts and solid base homogeneous/heterogeneous nanocatalysts
[19]. Table 1 lists recently manufactured nano catalysts derived from
2. Synthesis techniques of novel nano catalysts various feedstock sources.

2.1. Source 2.3. Characteristics

Nano catalysts are valued for their ease of manufacture, adaptability, For numerous applications, including catalysis, the unique physics
unique properties, and, most importantly, their role as a catalyst in the and chemical characteristics of nanoscience make nanoparticles highly
production of biofuels. Magnetic nanoparticles are frequently used in attractive. Magnetic nanoparticles are characterised by a high volume-
the synthesis of nanocatalysts. Fig. 1 depicts how they are generally to-surface ratio, quantum properties, and other chemicals because of
classified into four classes. Several modifications are made to the sur­ their tiny size. An extra feature of Magnetic nanoparticle is that the
faces of nano catalysts in order for them to be effective in biofuel syn­ particles that are immobilised may be readily removed without harmful
thesis processes [11,12]. The sizes and techniques of synthesis of various impact by using appropriate magnetic fields as a very helpful catalyst
magnetic nanoparticles (Metals, Alloys, Metaloxides, Ferrites) utilised in [20].
biofuel generation are mentioned below. Electronic structure: The energy level of a nanocrystal is distinct, and

2
K. Velusamy et al. Fuel 306 (2021) 121632

Table 1 reaction products and by-products, and they can be again used over four
Production of nano catalysts from different sources. times in a row without losing catalytic activity.[23]; Konwar et al.,
S. Nano catalysts Preparation and catalytic activity Reference 2014).
No

1. Au/α-Fe2O3 Modified co-precipitation method [79] 3. Synthesis techniques of biochar-based catalyst

Hybrid Pt/HZSM- Lower metal support interaction and high
5 catalytic activity Given its potential and eco-friendliness, biochar is abundantly used
2. Pt/Meso-MFI Ni/ Enhanced deoxygenation and in a variety of fields, especially biofuel production, by modifying its
HZSM-5 aromatization
90% bio-oil conversion in the feed
surface. Biochar has recently been identified as a green catalyst for the
Chitosan- [57] development of biofuels. Because of the potentials of biochar-based
palladium(II) Co-precipitation method catalyst, it would be a viable alternative to metal-based catalyst and
complex fossil fuel-driven carbon catalyst.[9,24].
3. TiO2/PrSO3H The graphing of propyl sulfonic acid [12]
groups into a mixed TiO2 help step
results in 98.3% of methyl esters in fatty 3.1. Source
acids (FAME). Without losing catalytic
ability, this solid acid nano catalyst may Any simple raw biomass can be converted into useful biochar, which
be re-used.
can be used in diverse fields like agriculture, biofuel processing, and
4. K/ZrO2/γ-Fe2O3 Soybean oil is converted to solid base [80]
nano catalyst by sol–gel method. The gel- catalysis. Contents such as hemicellulose, cellulose, lignin, and ash
sol KOH/(Zr(OH)4-Fe(OH)3) is content can differ depending on the form of feedstock. Biochar with a
impregnated with zirconium hydroxide high content of lignin , like pine and spruce wood, will have a high
and aqueous KOH solution.
porosity and a strong carbon fixed material , while lignocellulosic
5. Mn/IH Co-precipitation method [8182]
biomass with cellulose, hemicellulose, and lignin content will have a
6. RHC/K2O/Ni By impregnation method, rice husk is high graphite structure and stability.[25]. Examples of lignocellulosic
converted to magnetic nano catalyst biomass are agricultural wastes, forest residue and non-lignocellulosic
biomass are animal and poultry manure, sewage sludge and algae[26].
The kind of biomass used for producing biochar is given in Table 2.
its density and distance are much bigger and less than the appropriate
levels of a single atom or a minute atomic cluster. They are also known
3.2. Techniques
as quantum points due to their different amounts of energy. The nano­
crystals Valance band (VB) consists of atomic interactions of the highest
Torrefaction, hydrothermal carbonization and liquefaction, Pyroly­
concentration. [2120]
sis and gasification are the main techniques used in the processing of
Geometric structure: The structure of nanoclusters is the first and
biochar, as shown in Table 3.
most important problem to be determined. In most situations, the bulk
Torrefaction is a moderate pretreatment process carried out before
crystallography of a material cannot explain the structures of NPs. When
pyrolysis or gasification at temperatures preceding 200 to 300 ◦ C. The
examining nanometric dimensional atomic clusters, they are often
heating process for biomass in the absence of Oxygen, over 300 ◦ C for
thickly packed; consequently, they are anticipated to exhibit high uni­
biochar production, is characterized by pyrolysis. Carbonization of
formity and consist of atomic shells appropriate to the related symmetry.
biomass occurs at 300–800 ◦ C in the ancient technique slow pyrolysis,
When interpreting a cluster with a limited atoms, the bonding
and biochar is obtained as a main product with a 35–50 percent yield.
(maximum compactness) and surface energy should be maximised and
However, it has disadvantages such as high time consumption and poor
reduced. Small groups containing tens of atoms of various shapes (tet­
energy efficiency. The thermal breakdown of low-energy biomass takes
rahedron, hexahedron, octahedron). . [20] . [22]
Melting temperature: Because surface atoms are co-ordinatively
unsaturated, they have a high surface energy in a system with only a Table 2
few hundred atoms. The feature that the surface energy in fluid state is Different feedstocks and methods used for producing biochar and biochar-based
catalysts.
always lesser than in solid state is the key to understanding this melting
point . Surface atoms move in dynamic fluid phase to reduce area of the Feedstock Biochar Catalyst Type of Reference
production production catalyst
surface and undesirable surface links. Strong, solid-state binding ge­
method method
ometries create step by step surfaces with edge and corner high energy
atoms. The entire surface energy is decreased by melting. The smaller Peanut shell,
Glucose, [833]
the nanocrystal, the greater the contribution of surface energy to sys­ Oathull, Carbonization Sulfonation Solid-
tem’s total energy, and greater the melting temperature reduction. The Coconut acid
link between the nanoparticles dimensions and melting point strongly shell,
verifies the concept that the melting point drops as the particle size falls. Vegetable oil
asphalt
[22]
Irul wood saw Slow pyrolysis Sulfonation Solid- [5]
The surface of nanoparticles can be changed with acid groups such as dust acid
–SO3H to produce solid acid homogeneous/heterogeneous nano­
catalysts. Solid base heterogeneous nano catalysts were proven to be Shelled Palm
effective for industrial biofuel production because they can be recycled kernel , Carbonization Calcination Solid- (Zhao et al.,
Pamelo peel Wet- alkali 2018)
three to five times. Nano catalysts are unique in that they have stronger impregnation
magnetic properties, can be easily isolated, recycled. Sulfoalkylating
agents increase the surface activity of nano catalysts.[11]. The salini­
zation process, chemical treatments, polymer grafting, ligand exchange Husk of Rice Carbonization Chemical Solid- [84]
activation acid
technique, and ozonolysis can all be used to increase the pore size of
Peat Carbonization Wet- Solid- (Wang et al.,
prepared nano catalysts. Since the esterification and transesterification impregnation alkali 2019)
reaction rates are temperature dependent, high fatty acid methyl esters Banana Carbonization Wet- Solid- (Jitjamnong
yields are easily obtained. These nanocatalysts are easily recovered from impregnation alkali et al., 2020)

3
K. Velusamy et al. Fuel 306 (2021) 121632

Table 3
Classes of feedstock.
Classes Feed stock Types of oil References

Fisrt Generation Edible oil Safflower, rapeseed cardoon, coconut, soybean, sunflower, olive, almond and canola oil [85,86,87]
Second Generation Non-edible oil Waste frying oils, jatropha, palm, and linseed oils,Lard, chicken fat fish fat, beef, and duck tallow kitchen waste. [88,50]
Third Generation Algae Microorganisms yeast [45;49]

place in the rapid pyrolysis process with bio-oil the principal product at influenced by factors such as pyrolysis temperature, pyrolysis duration,
temperatures of 400–600 ◦ C.In either case, pyrolysis is a low-cost pro­ transition metals and biomass to water mass ratio. Biochar-based cata­
cess with low emissions of greenhouse gases.[9,3]. lysts are thermally and mechanically stable, have a stable structure, are
Slow pyrolysis nevertheless has some technical implications, which chemically inert, and biodegradable[33,34]. Fig. 2 depicts the methods
have made good quality bio-oil production improbable. The sluggish used to prepare biochar and biochar-based catalyst. Modification is done
process of cracking the primary product is a result of a high time spent by gasifying agents such as steam, CO2 for physical modification and by
residing and might have severe effects on the production and quality of activators such as H3PO4, ZnCl2, H2O2, alkali metal activators for
bio-oil. In addition, lengthy stay and minimal heat transmission require chemical modification.
an additional amount of energy[27,28]
Similarly fast pyrolysis also has some technological restrictions 3.3.1. Characteristics of diverse biochar catalysts
Heterogeneous biochar catalysts are easily distinguishable from
• Low thermal stability and oil corrodibility and oil solids other reactant mixtures. Bifunctional catalytic agents Processes both
• Increased viscosity over time by char catalysis esterification and transesterification. Reuasble type biochar catalysts
• Char dissolved alkali are concentrated in oil and pyrolytic water can be used more than once .Highly porous biochar catalsyst have a
generation occurs higher number of pores on their surface. Even when exposed to high
temperatures , non –graphitizable biochar catalysts do not form crystals
Hydrothermal carbonization is a process that takes place in a reactor (Chi et al., 2020),[35]a).
that is shut, at temperatures between 180 and 250 ◦ C when water is
present. Hydrothermal carbonization produces biochar with a larger 4. Novel nano catalysts and biochar-based catalyst in biofuel
number of functional groups on its surface and spherical particles of production
micro scale and few pores. In the gasification process, carbon-based
feedstock is heated to temperatures greater than 800 ◦ C when steam, We are facing increased depletion of fossil fuels due to unplanned use
air or CO2 are present [3]. of energy resources for transportation and industry. The use of biolog­
The most effective biochar processing methods are slow pyrolysis ically available feedstocks for biofuel production has gained traction in
and hydrothermal carbonization that delivers high biochar output. The scientific circles in this regard. At the intersection of homogeneous and
production of bio-oil and synthetical gas uses generally for flash heterogeneous catalysis, the use of nanocatalysts is revealing fresh
carbonization, torrefaction and gasification technology.[29–30]. After effective ways to manufacture sustainable environment friendly biofuels
making minor changes to the surface groups, the resulting biochar [36,37]. Their solid state makes them modifiable and their particle size
proves to be an effective catalyst that can be used in biofuel production. which is nanometric allows them to have high activities comparable to
Physical activation, chemical activation, gas activation, metal impreg­ homogeneous catalysts, as well as novel and special catalytic conduct
nation, sulfonation, surface amination, and surface oxidation are all not possible with solids larger than nanometers. In addition, the usage of
methods for activating biochar.[10]. active magnetic materials has resulted in the creation of nano catalysts
Physical activation of biochar is done by gasifying agents such as that can be recovered using magnetic fields. The most recent advances in
CO2, steam exceeding temperature 700 ◦ C to boost the pore size and area the development of highly active, durable advanced biofuels, inexpen­
of surface. Chemical activation of biochar is done by adding activators sive, and recyclable nanocatalysts and biochar-based catalysts are dis­
such as alkali metal activators, H3PO4, H2O2, ZnCl2 and K2CO3 [31]. cussed in this context.[38,39].
This form of activation can result in active pores even at low tempera­
tures. Another process for producing porous biochar by hydrothermal
4.1. Biofuel production in presence of nano catalysts
carbonization is nano casting[3]. Metal compounds co-calcinated
biomass like platinum, copper, and ruthenium is performed by the
4.1.1. Biodiesel
process of impregnation of metals to bind metals atpowered positions on
Biodiesel has proven to be an effective fuel candidate to meet the
biochar. Sulfonating is a surface activation method in which biochar
world’s potential demand for power due to its characteristics. Bio­
with both strong and weak sulfonic acid groups can improve catalyst
diesel’s promising specific features include biodegradability, environ­
efficiency in acid-driven reactions. Sulfonation can be used to create
mental friendliness, low toxic levels, high combustion effectiveness, and
solid-acid catalysts. Steam treatment can also be used to enable biochar
lower sulfur oxide and nitrogen oxide emissions when burned[40].There
by heating it for 1 h at 700–850 ◦ C[10]. Catalysts for biochar can be
are three major classes of feedstock which are relatively quick to plan
made using one of three methods: one-step, two-step, or preformed
and protective to the environment is represented in Table 3 and the
metals are covered with biomass, and carbonized.
different strategies for biodiesel production is given in Table 4.

3.3. Characterization 4.1.2. Bio-oil

Because of its high density of energy and easiness of storage or
Biochar-based catalysts are favored because they produce a very transport compared to gasoline, Bio-oil is seen as an appealing feedstock
good metal support interaction between the metal and the carbon. It has to replace fossil fuel for generation of power .Bio-oil is also biodegrad­
the ability to regenerate, to provide continuous operation and effec­ able, CO2 or greenhouse gas neutral, and contains far less nitrogen oxide
tiveness at high temperatures, and it is also inexpensive and suitable. and sulfur oxide when combusted in an engine than petroleum-based
The biochar’s surface functionality results in catalytic efficiency. Its fuel. As a result, bio-oil is a green fuel that is also good for the envi­
catalytic activity in tar cracking is primarily due to inorganic groups ronment [41].
such as potassium and iron.[7,32,10,3]. Catalytical activity in biochar is The main constituents of wood, cellulose, hemicelluloses and lignin

4
K. Velusamy et al. Fuel 306 (2021) 121632

Fig. 2. Methods involved in producing biochar-based catalyst.

Table 4
Biodiesel production strategies.
Method Advantages Disadvantages Reference

Direct Blending No necessity for any chemical or extra processing Not suitable for long-term use
Highly viscous compared to standard petrol [89]
Low volatility.

Micro- Simple procedure Incomplete combustion [67]

emulsification Suitable for oil with a lot of viscosity Release of large amounts of carbon dioxide
Trans- Mild reaction conditions Production of waste water [9078]
esterification- High conversion rate Formation of by-products, and treatment of
• Base catalyst Ability to manufacture on a wide scale fatty acid deficiency
• Acid catalyst
Pyrolysis
No need for further isolation or purification step
Effective and pollution-free so the fuel treated by this process which could be use directly in Equipment is costly
diesel engine without any modification. Biodiesel purity is poor due to residue
contamination

have distinct bio-mass compositions. The potential of biomass to 4.1.3. Biogas

generate high heating value (HHV) bio-oil is determined by its elemental Nanoparticles are dissociated in a controlled manner in an environ­
composition such as Carbon, Hydrogen, Oxygen, Nitrogen, and Sulphur, ment in the absence of oxygen and fed to micro biotic organisms that are
ash content, moisture content[42,43]. Various kinds of feedstocks used responsible for depletion of organic matter, a function that they are well
to produce bio-oil are given in Table 5. The thermochemical techniques suited for. As a result, the production of biogas can be increased by up to
used for producing bio-oil is illustrated in Fig. 3. Thermochemical 200%[44].
techniques such as pyrolysis and liquefaction transform biomass into
bio-oil .The main difference in the temperature range for pyrolysis and
liquefaction are 400–600 ◦ C and 250–400 ◦ C respectively. 4.2. Nano catalyst role in biofuel production process

4.2.1. Biodiesel
Researchers have applied numerous catalysts in the development/
synthesis of biodiesel, including catalytic acids homogeneous/hetero­
geneous, uniform/heterogeneous basic catalyst biocatalysts and nano­
Table 5
Kinds of feedstocks/biomass to produce bio-oil. catalysts. Despite being the method of choice, when oil of low-grade is
used, transesterification of acid catalysts requires higher oil molar ratios
Biomass type Bio oil yield(wt Temperature References
of alcohol[45]. Because of its reusability, wide availability, ease of
%) (◦ C)
separation from product, and longer life time, transesterification using
Wood sawdust 74 650 [9136]
heterogeneous base catalysts has been found to be cost effective in mild
Grape bagasse 27.6 550
Pine wood 50.0 450 [92] conditions[46,47]. However, solid alkaline catalysts must be extensively
Rice husks 60.0 450 [93] investigated and optimized in order to minimize saponification and
Pinewood sawdust 75 500 [9495] overcome diffusion limitations, resulting in higher yield. In comparison
Municipal,livestock,wood to acid-catalyzed transesterification, base-catalyzed transesterification
waste 39.7 500
is extensively used in industrial output because of the high fatty acid

5
K. Velusamy et al. Fuel 306 (2021) 121632

Fig. 3. Bio-oil transformation thermochemical methods.

methyl esters yield in a brief reaction time[48]. Recent biodiesel pro­ To improve catalytic efficiency, metaloxides mixed with base cata­
duction formed with ionic liquids that are supported by nanoporous lysts are usually coated with MgO or CaO. In the development of bio­
materials with special focus on the use of IL-nano porous materials diesel, catalysts are very active. The use of raw materials with free
tunable characteristics.[49]. fattyacid content is considered important in these catalytic processes;
To have a more environmentally friendly process and meet envi­ otherwise, base catalyst poisoning will occur.[52].
ronmental needs, enzyme catalysts must be created. The process has the In transesterification, potassium hydroxide, sodium hydroxide, and
ability to produce a high-quality commodity comparable to Petro-diesel sodium methoxide are utilised. It is an alcohol-oil reaction that occurs in
fuel which highlight the use of carbon-oriented catalysts to produce the collaboration of a base catalyst. To get the best biodiesel yield, re­
biodiesel from carbohydrate or biomass precursors[50]. Table 6 high­ action temperature is maintained at 500–600 ◦ C. The temperature of
lights the comparison of homogenous/ heterogeneous/bio/nano reaction should be below than the point of boiling of methanol. Meth­
catalysts. anol will otherwise be discarded due to vaporization. The stirring
Various nanocatalysts such as zeolites, single metal oxides, hydro­ method with 1300 rpm is used in the process to increase the rate of
talcite, and assisted alkalimetal/metalion have been shown to have high reaction through dynamic mixing. It will take nearly an hour to com­
biodiesel production performance. Metal-oxide catalysts mixed with plete the reaction [53]. Catalysts used in transesterification process, co-
solids are those that have more than two metal oxides in their compo­ precipitation process and mixing process are shown in Tables 7– 9
sition.[51] respectively.

Table 6
Comparison of different catalysts used in biodiesel production.
Types Homogenous Heterogeneous Biocatalysts Nanocatalysts

Advantages Base catalyst produces good kinetics: high Environmentally friendly, non-corrosive, Biodiesel is made from free High reactivity,
performance and give high return in short and recyclable, resulting in less disposal fatty acids (FFA).
period issues. Product separation is easier, Good electivity, and the optimum
The base catalysts respond 4000 times as selectivity is higher, and catalyst life is Low reaction temperature, yield
rapidly as the transesterification of longer. water insensitive
catalysed acids Separation goods are easy to
Insensitive to free fatty acids and water, separate.
Base methoxides are better than acid heterogeneous catalyze both The basic inherent catalytic activity
hydroxides esterification and transesterification Catalysts with a higher yield and selectivity can be easily
simultaneously. than basecatalysts regulated by altering the physical
Acid catalysts can be used for both and chemical properties of the
esterification and transesterification Catalysts that are catalysts
simultaneously homogeneous or
heterogeneous may be used.
Disadvantages Acid catalysts are corrosive and produce a A high alcohol to oil ratio, as well as a In the presence of methanol, Saponification
very slow rate of reaction. high temperature and pressure, are the enzyme is inhibited, and Catalyst DeactivationLow rate of
required. additional supportive solvents reaction
can be required as a medium.
Acid catalysts necessitate a higher molar
ratio of methanol to gasoline, a higher Acidic catalysts have a lower acid site
temperature, a higher acid concentration, concentration, a lower microporosity,
and more waste from the neutralization and a higher cost than simple catalysts.
reaction.
Reference [96,38] [97,98] [99] [100]

6
K. Velusamy et al. Fuel 306 (2021) 121632

Table 7 Table 8
Different source of catalyst used in transesterification process. Different source of catalyst used in co-precipitation process.
Source Catalyst Process description Reference Source Catalyst Process description Reference
2+
Soyabean Nanoferrite Looked at how Cu ions [101102] Waste cooking Magnesium To create nanostructured [10498]
catalysts influence the oil oxide (MgO) magnesium oxidecatalysts for
morphology, magnetism, catalysts biodiesel production from
and structure of waste cooking oil.93.3%
NiO.5ZnO.5Fe2O4 biodiesel was generated after a
nanoferrite catalysts, as one-hour reaction at 65 ◦ C
well as how this affects adding 2 wt% MgO with a 1:24
the catalyst’s behaviour Beef KF-Al2O3 oil-to-methanol molar ratio.
in the transesterification processing nanocatalyst
of soybean oil to fatty industrial The biodiesel yield was 97%.
acids esters containing sludge The nanocatalyst could be
Chicoreusbrunneus Heterogeneous methyl. It led to increase recycled seven times without
shells CaO in biodiesel yield by losing its efficacy. The high
nanocatalyst 5.5–85%, suggesting efficiency was due to the
that these nanoferrite nanocatalyst’s increased
Cu2+ doped surface area as well as the
NiO.5ZnO.5Fe2O4 ultrasonic wave effect.
catalysts may be used in Waste cooking Fe3O4@Al2O3 An effective Fe3O4@Al2O3 [105]
the biodiesel industry. oil nanocatalyst nanocatalyst was prepared by
co-precipitation method which
Thermal decomposition can be used to transform waste
technique to make cooking oil into fatty acids
heterogeneous CaO methyl esters. The procedure
nanocatalyst by began with the development of
calcined, hydrated, and a magnetic suspension
dehydrated containing Fe3O4
Chicoreusbrunneus shells. nanoparticles, which was then
Commercial CaO was mixed with
also calcinated at aluminiumisopropoxide and
elevated temperatures of sonicated for two hours.
900 ◦ C in order to
remove toxins. In a
desiccator, both
nanocatalysts maintain Table 9
their catalytic activity Different source of catalyst used in mixing process.
high.
Source Catalyst Process description Reference
Empty palm oil fruit Solid nano Palm oil fruit bunches [103]
fiber catalyst were washed, dried, and
burned to ashes. The Palm oil CaO-X CaO-X nanocatalysts were [106107]
K2O-enriched ash was nanocatalysts prepared as sol–gel samples
then exposed to 600 ◦ C by mixing process and used to
calcination to create trans esterify palm oil. The
nanoparticles with more Pechini process, which
active sites. involves the use of dissolved
calcium led to the formation
of 81%fatty acids methyl
To begin with prepare a two-component complex carrier, the use of esters in just 3 h.
co-precipitation is to create elevated acidic or simple catalysts. To make Discarded Strontium oxide
cooking oil (SRO) The combination of urea and
a mesoporous basic nanocatalyst, the carrier is impregnated with a solid
nanocatalyst oxide of strontium to form a
salt. This method produces nanocatalysts that easily detach from the consistent solution that was
final product[54]. then heated to 900 ◦ C. When
Metal oxide mixture catalysts are made by mixing metal oxide mix­ fueled in compression
ignition (CI) diesel, the
tures. Oxides are combined with a significant amount of the active
properties are quite similar to
component such as metals. This results in a catalyst with a less surface conventional fuel
area and more basic active sites concentration. Impregnation is often Soybean oil Calcium oxide Used sol–gel mixing process. [105]
used to ensure the formation of more active catalysts. Mixed oxide of nano catalysts They synthesized fatty acids
Calium and Nickel , for example, was first packed as a carrier before methyl estersin 97.61% ouput
from soybean oil at
being impregnated with KF to create an improved nanocatalyst[55].
temperature 60 ◦ C for 2 h

4.2.2. Bio-oil
In general, bio-oil is strongly acidic pH of 2–3 and oxygenated. As a reduction in emissions. Thus, less acidic materials may be more bene­
consequence deoxygenation of bio-oil is needed to boost its properties, ficial in upgrading bio-oils[57].
such as lowering acidity and increasing both the higher heating value Many studies have recently centered on basic metal oxides in
and stability (Nagoles-Delgodo et al., 2020). The oxygenates in bio-oil biomass catalytic quick pyrolysis. (Bhandari et al., 2014b). Even when
vapors would be catalytically converted simultaneously with pyrolysis only 5 wt% Calcium Oxide was used, the Calcium Oxide catalyst dis­
in catalytic quick pyrolysis (CFP).[56])published a comprehensive played the most positive acid reduction physical results of the bio-oil
analysis of catalytic quick pyrolysis, highlighting the importance of the among the three catalysts used. The use of CaO, on the contrary,
catalytic reactions that may occur in catalytic quick pyrolysis. HZSM-5 is resulted in an gain in water content. Despite the fact that all three cat­
a zeolite catalyst that has been extensively researched for catalytic py­ alysts were capable of deoxygenation, the MgO catalyst performed
rolysis. Nonetheless, the use of the ZSM-5 zeolite catalyst resulted in a slightly better. The amount of hydrosugars decreased the most and the

7
K. Velusamy et al. Fuel 306 (2021) 121632

amount of furan compounds increased after the introduction of 10 wt% not been systematically characterised and the safety standards for using
MgO catalysts[58]. such catalysts are generally lacking which causes nanotoxicity to
At 350 ◦ C, different heterogeneous catalysts were used to hydro­ humans and ecosystem. Almost all nanocatalysts generally generate
thermally liquefy the microalgae nannochloropsis sp. Hydrothermal both in vitro and in vivo harmful effects at a particular level. The main
liquefaction of microalgae with heterogeneous catalysts, for example, reasons for nanotoxicity seem to be Reactive Oxygen Species (ROS) and
improved product consistency. Except for zeolite, the crude bio-oils cell signaling disturbances. Furthermore, the toxicity of nanoparticles is
formed by these catalysts were easy to flow than the biocrudes pro­ determined by the variables of particle size and the surface function­
duced by noncatalyzed liquefaction [59]. ality. (Polshettiwa et al.,2010)
An effective hydrodeoxygenation catalyst on silica combined as a
hydrodeoxygenation substratum of cyclohexane in a batch reaction 4.3. Biofuel production in presence of biochar-based catalysts
extremely scattered palladium and ultra-fine molybdenum phosphate
nanoparticles under mild conditions which gives 100% conversion and Biochar-based materials have recently been researched for refinery
97.5% selectivity. Importantly, using timber and feedstocks from bark, catalysis such as syngas cleaning and conversion, biodiesel processing,
the synthesized catalyst could efficiently hydrodeoxygenate biomass and air pollution control. Important characteristics can depend on the
with proven efficiency and oil yields.[60]. application, such as particulate pressure, porosity and composition of
minerals[9,67].
4.2.3. Biogas
A documentation was made on the anaerobic digestive process of 4.3.1. Biodiesel/Bio-oil
livestock manure and its effect on metallic oxide productivity and Biodiesel has been generated using biochar-based catalysts. Esters
biogas. (Luna del Risco et al). CuO nanoparticles had a greater impact on are biofuels made from free fatty acids, alcohol and glycerides. Bio-oil
the experiment beyond the other research compounds. Day 14 is regu­ formation process is shown in Fig. 4.
lated by the whole biogas generated and was reduced by 30% due to a Dong et al studied that for three runs at 100 ◦ C, sulfonated biochar
Cu concentrate of 15 mg/L. At concentrations ranging between 120 and maintained a high free fatty acids transition of 97–98 percent from 19
240 mg/L,CuO reduced biogas production by 19 and 60 percent . [61]. distilled microalgal oil in methanol. Major chlorophyll and phospho­
Methane formation can be boosted by a iron nano oxide because of lipids in specific biomass, such as microalgae, can impair the catalyst
the presence of Fe3C and (Fe3O4 NPs).Fe3O4 nanoparticles with a and reduce biodiesel efficiency, so they have to be extracted beforehand.
diameter of 7 nm were applied to an garbage digester in the absence of [668].
oxygen at 100 ppm for 60 days at 37 ◦ C. Methane generation was These findings demonstrated the biochar catalyst’s suitability for
increased by 234% and 180% increase in biogas production was ach­ biofuel production through esterification. Another study found that after
ieved using nanoparticles[62]. Abdelsalam et al. found that Ni nano sulfonation by 99% H2SO4, powered carbon had elevated esterification
particles with 2 mg/L and 17 nm were the most successful nano parti­ activity than biochar catalysts which has 97 vs 70% conversion, owing
cleswith methane yield of 78.53% and biogas output of 116.76%. At 28 to the more volume of pore. [69].
nm size and 1 mg/L concentrate , CO increased biogas production by The transesterification method is more reliant on heavy Bronsted
71% and methane production by 45.92%[63]. acidity than esterification. Fuming H2SO4-modified biochar with more
Gasification of Asphodelus tenuifolius and Chenopodium album using –SO3H groups resulted in significant amounts of products, a match for
nanomaterials as catalysts. Nanocatalysts made of nickel and cobalt gross biodiesel output of 10%[6]. It was also discovered that as the area
nanoparticles were used to speed up biochemical reactions and generate of the catalyst surface increased, so did the output.
these products at lower temperatures of 400 ◦ C in a muffle furnace. This suggests that energy supply will boost transesterification ac­
Biodiesel was found to contain 65.47% esters, indicating that it is of tivity, which may be related to triglyceride miscibility in methanol at
higher quality than commonly processed biodiesel, which contains elevated temperatures. It was shown that after sulfonated biochar was
15–20% esters. Biogas derived from mixed weed biomass resulted in used to pre-esterify microalgal oil, CaO was applied for subsequent
yield of 3.76% methane, 8.32% propane, 50.16% ethene, 3.12% pro­ transesterification, resulting in a 99% fatty acid methyl ester yield. It is
pyne, and 34.64% methanol, according to gas chromatography-mass easier environmentally friendly to use biochar made from biomass rich
spectrometry research. The current findings clearly demonstrated in CaCO3. According to an optimization and kinetic analysis, the latter
increased quality of the product and efficiency in terms of energy in the can produce nearly 100% fatty acid methyl ester under ideal conditions
gasification of weed biomass [64]. [68,70].

4.2.4. Advantages of nanocatalysts 4.3.2. Biogas

Nanocatalysts have some distinct benefits compared to normal cat­ Tar reformation involves converting a hydrocarbon blend including
alysts, for example an improved mix with reactives and simple segre­ phenolic, olefin and polycyclic aromas that will inevitably become
gation from the reaction mix, because of their insolubilities in different useful syngas during biomass and pyrolysis gasification. Biochar, along
solvents. In addition, the catalytic reactions and selection of nano­ with traditional catalysts, can be efficient for the tar reform, including
catalyst is facilitated by the adaptation of the chemical and physical calcium magnesium carbonate dolomites, olivins.[71].
characteristics[65]. Nanocatalysts use can contribute to better energy Hydrogen is another sustainable alternative to fossil fuels given its
and economic efficiency. For example, a cellulose hydrolysis nano­ minimal emissions, which may be created by biogas reforms. During
catalyst has been shown to be stable, economical, very active, and se­ biomass pyrolysis/gasification, Biochar improves the hydrogen gener­
lective. Nanocatalysts have also been used to achieve much lower ation. [72]. Biogas production using gasification of different lignocel­
chemical waste and an improved use of feedstock. In the light of the lulosic biomass has been addressed in Fig. 5. The addition of unmodified
many potential benefits of nanocatalysts, refineries, petrochemical biological biochar as catalyst during the pyrolysis of microalgae facili­
plants, pharmaceutical industries, chemical industry, food processing tated the synthesis and selectivity of hydrogen by 1.37 and 1.59 and is
and environmental applications have been applied. The worldwide seen in Table 10. respectively.
nanocatalyst market is projected to hit 6 billion USD by 2019, according
to the Global Industry Analysts.[66] 4.3.3. Advantages of biochar based catalysts
The goal is to make the production of biofuels ideal for low costs,
4.2.5. Disadvantages of nanocatalysts broad-scale areas, functional group adaption etc. as a heterogeneous
In contrast to conventional catalysts, the risks of nanomaterials have catalyst. Biochar has a robust structure, outstanding thermal and

8
K. Velusamy et al. Fuel 306 (2021) 121632

Fig. 4. The production process of bio-oil.

Fig. 5. Biogas production.

mechanical stability, chemical hierarchies of the biomass structure are catalysts development are still found in early stages only. So, there is a
not very inherent to biochar as a superior catalyst for diverse catalytic need for developing a method that can increase catalytic performance.
applications. Biochar is also very stable. [3] In order to build up in a large scale, researchers are focusing on the
Biochar based catalysts may be i) easily isolated from other reactive modification that can be carried out in biochar-based and nano materials
compounds ii) bifunctional catalytics i.e. esterification and Trans­ for their application in future fields including catalysis, energy storage
esterification iii) extremely porous (iv) not crystal forming even when and conservation, environmental pollution and even in chromato­
exposed to high temperatures. graphic separation [74]; Mian et al., 2019).
Biochar stands high, because of its low cost, eco-friendly, easy
manufacturing method, re-usability and biodegradable compatibility in i) New species or biomass can extend the spectrum of accessible raw
comparison with other commercially available, strong catalysts.[73] materials in biofuel production (including algae, mushrooms,
yeast and other microbes). [3]
4.3.4. Disadvantages of biochar based catalysts ii) In addition, it was noted that during development of NBCs the
Disadvantages include i) Research data are only limited available, ii) researchers focused mainly on Fe3O4 NMs. Additional new mag­
Process control is relatively complex, iii) High operating temperatures, netic materials like ferrofluids can be explored for the same
iv) Energy intensive drying before pyrolysis, v) The necessity to treat results.
flue gas vi) The vapour phase lose of Nitrogen vii) Potential organic iii) Toxicological issues regarding nano catalysts, on the other hand,
contaminant formation in biochars, like polycyclic aromatic hydrocar­ are a hot topic of debate, and overcoming the toxicity effects will
bons, dioxins and furan[73] necessitate comprehensive research in future.[75]
iv) In addition to this, the industrial manufacture of biochar-based
5. Future perspectives catalysts in a biomass refinery may be linked with the biofuel
production, to ensure a more integrated and sustainable use
In spite of many applications, biochar-based catalysts and nano process of biomass. However, most case studies have not

9
K. Velusamy et al. Fuel 306 (2021) 121632

Table 10 6. Conclusion
Different biomass used in hydrogen production process.
Biomass/ Biochar Conversion Temperature Reference Nano catalysts have the ability to improve overall performance in
feed stock catalyst efficiency (◦ C) biofuel and biochemical production. They have a large region and cat­
treatments (%) alytic functionalities, which aids in the resolution of issues like resis­
Wood Constant 70% 1000 [10810911063] tance to mass transfer, accelerated disabling and inefficiency. Overall,
oxidation by conversion the nano catalysts are important not only for producing commercial
CO2 and H2O biofuel, but also for manufacturing, through the flexible bio-refinery
Stalk of in the
cotton pyrolysis gas 800
model, cellulosic combustibles, green chemicals and other bio-based
Procreation 92% materials. The latest nano catalysts have many benefits, including
with Ni Conversion their ability to improve the performance of heterogeneous traditional
(NO3)2⋅6H2O catalytical approaches as the best catalyst for heterogeneous catalytic
Waste solution The
analysis. Nanocatalysts used in biofuel processing are numerous in terms
activated Applied Fe2O3 presence of
sludge (100 mg/g) 100 mg/g of toxicity, but there is no question that further extensive study is
Nanoparticles Fe2O3 NP necessary on the toxicity of different biofuel nano catalysts. Nano­
for methane increased to particles have the ability to qualitatively and quantitatively revolu­
production 117% of tionise biofuel production in order to meet the next energy demands.
Livestock control
raw production.
The cost of the synthesis of nanoparticles must also be weighed in order
manure to produce economic biofuels. This expense could modify the whole
Applied Ni, Ni NPs manufacturing process of biofuels.
Fe3O4, Co, Fe produced
nanoparticles the largest
CRediT authorship contribution statement
significant
biogas and
methane Karthik Velusamy: Writing - review & editing, Data curation,
output Formal analysis. Jamunarani Devanand: Writing - review & editing,
compared
Data curation, Formal analysis. Ponnusamy Senthilkumar: Concep­
to Co, Fe
and Fe3O4
tualization, Validation, Supervision. Kalaivani Soundarajan: Re­
NPs and the sources, Visualization. Veena Sivasubramanian: Investigation, Formal
control analysis. Jaisankar Sindhu: Resources, Visualization. Dai-Viet N. Vo:
Resources, Visualization.

conducted a comparison between the synthesised biofuels and

the conventional fuels. This component of research should also be Declaration of Competing Interest
focused in future since this characteristic is important in order to
gain an insight into the functioning potential of prepared bio­ The authors declare that they have no known competing financial
fuels.(RuiShan et al., 2020) interests or personal relationships that could have appeared to influence
v) At the level of laboratory study are still biochar catalysts. For the work reported in this paper.
future industrial application, a purpose-based synthesis and
modification is required. This may be done through the combi­ References
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