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Zeolite synthesis from low-cost materials and environmental applications: A

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DOI: 10.1016/j.envadv.2020.100019

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Contents lists available at ScienceDirect

Environmental Advances
journal homepage: www.elsevier.com/locate/envadv

Zeolite synthesis from low-cost materials and environmental applications:

A review
Abdul Khaleque a, Md Masruck Alam b, Mozammel Hoque b, Shuvodip Mondal a,
Jahid Bin Haider a, Bentuo Xu c, M.A.H. Johir d, Aneek Krishna Karmakar b, J.L. Zhou d,
Mohammad Boshir Ahmed b,d,e,∗, Mohammad Ali Moni f
a
Department of Applied Chemistry and Chemical Engineering, Bangabandhu Sheikh Mujibur Rahman Science and Technology University, Gopalganj 8100, Bangladesh
b
Department of Applied Chemistry and Chemical Engineering, University of Rajshahi, Rajshahi 6205, Bangladesh
c
School of Life and Environmental Science, Wenzhou University, Wenzhou 325035, China
d
Center for Green Technologies, School of Civil and Environmental Engineering, University of Technology Sydney, 15, Broadway, Sydney, NSW 2007, Australia
e
School of Materials Science and Engineering, Gwangju Institute of Science and Technology, Gwangju 61005, Republic of Korea
f
WHO Collaborating Centre on eHealth, UNSW Digital Health, School of Public Health and Community Medicine, Faculty of Medicine, UNSW Sydney, Australia

a r t i c l e i n f o a b s t r a c t

Keywords: Zeolites with the three-dimensional structures occur naturally or can be synthesized in the laboratory. Zeolites
Low-cost raw materials have versatile applications such as environmental remediation, catalytic activity, biotechnological application,
Tetrahedral structure gas sensing and medicinal applications. Although, naturally occurring zeolites are readily available, nowadays,
Modified zeolite
more emphasis is given on the synthesis of the zeolites due to their easy synthesis in the pure form, better ion
Hydrothermal method
exchange capabilities and uniform in size. Recently, much attention has also been paid on how zeolite is being syn-
Environmental application
thesized from low-cost material (e.g., rice husk), particularly, by resolving the major environmental issues. Hence,
the main purpose of this review is to make an effective resolution of zeolite synthesis methods together with po-
tential applications in environmental engineering. Among different synthesis methods, hydrothermal method is
commonly found to be used widely in the synthesis of various zeolites from inexpensive raw materials such as
fly ash, rice husk ash, blast furnace slag, municipal solid waste, paper sludge, lithium slag and kaolin. Besides,
future expectation in the field of synthetic zeolites research is also included.

1. Introduction
Zeolites, a member of the microporous crystalline aluminosilicates
family, also known as “molecular sieves” (Auerbach et al., 2004). Zeo-
lite has the three-dimensional structures which are composed of the net-
works of [SiO4 ]4− and [AlO4 ]5− tetrahedral linked to each other with
oxygen atoms (Fig. 1a) (Chiang and Chao, 2001). Depending on the
structural type, cages are formed by connecting the pore openings of
defined sizes (i.e., 0.3-1.0 nm) in the tetrahedral structures. Therefore,
a neutral structure is produced by neutralizing the negative charge on
the lattice by the positive charge of the cations (Cejka, 2007). The gen-
eral chemical composition of a zeolite is Ma/b[(AlO2 )a(SiO2 )y].cH2 O,
where M represents either an alkali metal or an alkaline earth metal
cation, b represents the valence earth metal cation, c is the amount of
water of crystallization per unit cell and a and y represent the total num-
ber of the [SiO4 ]4− and [AlO4 ]5- tetrahedral in a unit cell of the zeolite,
respectively (Chiang and Chao, 2001; Lakiss et al., 2020). The ratio y/a
ranges from 1.0 to 5.0. But, this value can be changed based on the
structure. For example, silica-based zeolite has value of 10.0 to 100.
Zeolites occur naturally as well as it can be prepared in the labora-
tory. Zeolites are usually divided into two main categories: natural (e.g.,
clinoptilolite, mordenite and garronite), and the synthetic zeolite (e.g.,
zeolite A, P, X and Y) (Oruji et al., 2018; Metropoulos et al., 1993).
At present, there are over two hundred types of zeolites. These are
based on the silica-alumina ratio. It was found that natural zeolites have
better resistivity and thermal stability in the different environments.
Their thermal stability and chemical resistance increase with the in-
crease of silica-alumina ratio as well as in the presence of alkali cations
in the zeolite framework (Büchel et al., 2008; Georgiev et al., 2009). A
lattice unit, which is the building block of the repeating units and the
relationship between the tetrahedral primary building unit (PBU) and
secondary building unit (SBU) structure, is shown in Fig. 1b. The SBU
is basically the main unit of the zeolite framework. Until now, there are
nine known SBUs available (Lakiss et al., 2020).

∗
Corresponding author at: Department of Applied Chemistry and Chemical Engineering, University of Rajshahi, Rajshahi 6205, Bangladesh.
E-mail address: Mohammad.Ahmed@gist.ac.kr (M.B. Ahmed).

https://doi.org/10.1016/j.envadv.2020.100019
Received 14 August 2020; Received in revised form 11 October 2020; Accepted 24 October 2020
2666-7657/© 2020 The Author(s). Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/)
A. Khaleque, M.M. Alam, M. Hoque et al.
Nowadays, zeolites have much potential ranges of applications in-
cluding technical, environmental, industrial, commercial, agricultural,
cracking and alkylation processes, and biomedical due to their porous
character and their ion-exchange properties (Yilmaz and Müller, 2009).
Naturally occurring zeolites are used as materials for the construction
and paper industry (Feng and Peng, 2005). They are also used in agri-
culture and other applications. Laboratory synthesized zeolites with de-
fined pore sizes have a wide variety of applications in adsorbents, cata-
lysts or molecular sieves and catalysts of oil refineries (Minachev et al.,
1966), removing radioactive contaminants (Malekpour et al., 2008) and
laundry (Fruijtier-Pölloth, 2009). Synthetic zeolites have many added
advantages. For example, synthetic zeolite is synthesized in an ex-
tremely pure form and uniform in size together with better ion exchange
capabilities (Auerbach et al., 2004).
Commercially, synthetic zeolites are used in massive quantity than
natural zeolite due to the high purity of crystalline products and the
uniformity of particle sizes (Breck, 1984). Besides, synthetic zeolites are
made commercially for specific uses (Moshoeshoe et al., 2017). They
are also used as chemical sensors in industrial process control, environ-
mental mitigation, including heavy metals removal, gas capture, indoor
air-quality monitoring, medical monitoring and so many. Hence, syn-
thetic zeolites have drawn a great deal of interest among researchers and
scientists due to their high flexibility and well adaptability. Synthetic
zeolites offer more benefits than natural zeolite. For example, synthetic
zeolite is favored to control the certain reactions such as the control of
N2 O emissions (Ates et al., 2011). In addition, synthetic zeolite has ex-
cellent ability in the removal of radioactive wastes than natural zeolite
(Moamen et al., 2015; Lonin et al., 2015), greater adsorption capacity
for removing various toxic metal ions (e.g., Cr3+ , Ni2+ , Zn2+ , Cu2+ , and
Cd2+ ) (He et al., 2016). Furthermore, synthetic zeolites have larger pore
volume than that of natural zeolite, which is more favorable for trap-
ping various contaminants from air and water (Bandura et al., 2015).
Due to the enormous benefits of synthetic zeolite over other zeolites, it
is going to replace the natural zeolites for a variety of applications. Con-
sidering the potential advantages and applicability, there are already a
few review articles on different types of zeolites and their application.
For example, Belviso (2008) reviewed the synthesis of zeolite from coal
and biomass-based raw materials. However, to our best knowledge, spe-
cific review article on the sufficient resolution of zeolite synthesis and
potential environmental applications is rare.
Therefore, the main objective of this review is to provide an up-
to-date overview of the properties of conventional synthetic zeolite
preparatory methods from low-cost wastes, less-valuable and abounded
source of raw materials. This review also emphasized the potential en-
vironmental applications of synthetic zeolite. Finally, associated chal-
Environmental Advances 2 (2020) 100019
Fig. 1. Diagram of the assembly of SiO4 and
AlO4 tetrahedral (a); and the channel and rela-
tionship between tetrahedral PBU and SBU units.
lenges in the synthesis of synthetic zeolite together with future recom-
mendations have also been included.
2. Properties of synthetic zeolites
Synthetic zeolites are highly pure with uniform crystal size and use-
ful for particular industrial applications. In contrast, natural zeolites
contain different foreign materials which have a no uniform crystal size.
Natural zeolite takes several days to decades to create, while synthetic
zeolites can be prepared in the laboratory from a few hours to a few
days with controllable pore size, surface characteristics of the adsorbent
and excellent thermal stability. However, at a slightly higher cost, this
makes a much more uniform product than naturally occurring zeolites.
Synthetic zeolite can be synthesized from various sources with different
chemical compositions and physic-chemical properties (Table 1). The
crystal size of synthetic zeolites is typically found in the range of 1.0–
10.0 μm while the density varies in between 2.0 to 23.0 g/cm3 . Syn-
thetic zeolites bulk specific gravity lies in between 0.80 and 0.90 g/cm3
(Breck, 1984). Optically, the refractive indices of synthetic zeolite are
ranging between 1.47 and 1.52. Zeolite has a water absorption capacity
of 45.0 to 75.0 ml/100 g (Smit and Maesen, 2008). Thermal stability can
reach at a desirable stage by reduction Al content or higher maintaining
higher Si/Al ratio (Zhao et al., 1998; Metintas et al., 2010).
Synthetic zeolite types A, zeolite P, zeolite X and zeolite Y differ
mainly due to the content of aluminum (as alumina) can influence
the crystal structure and the ion-exchange selectivity of the zeolite
molecule. Generally, the ion-exchange capacity as well as rate disso-
lution increase with the increase of alumina content as well as sodium
content. Besides, zeolites may get hydrolyze at lower pH (below 4.0),
therefore, their crystal structure may destroy by releasing the sodium
ion, silicic acid, and aluminum salt. However, the aqueous suspension
of zeolite is found to be in the alkaline region (i.e., at a pH of 10–10.5).
Zeolite A consists of sodalite cages which is connected with the double
4-rings cuboidal-shaped crystals (Fig. 2a).
Zeolite type P is unique in characteristics which is belonging the
gismondine family (Fig. 2b). Zeolite types X and Y belong to the family
of faujasite-type structure (FAU). In contrast to zeolite type X, Y has
higher Si/Al ratio >1-1.5. However, these zeolites are more spherical.
They have cuboctahedron building blocks which are linked to a faujasite
structure via hexagonal prisms. They have a larger pore diameter (∼0.74
nm) and high surface area. Hence, they are capable of exchanging more
ions like calcium and magnesium. They have a wide range of industrial
applications (Zhdanov et al., 1990).
 A. Khaleque, M.M. Alam, M. Hoque et al.
Table 1
Properties of most commonly used synthetic zeolites.

Framework Cationic Typical unit cell formula Window Channel Cation exchange Application Ref.
form diameter (nm) capacity (meq/g)

A Na Na12 [(AlO2 )12 (SiO2 )12 ] 8-ring (obstructed) 0.38 5.3 Warm mix asphalt, formulation of detergents and (Feng and Peng, 2005, Amoni et al., 2019, Bajpai and
Ca Ca2 Na2 [(AlO2 )12 (SiO2 )12 ] 8-ring (free) 0.44 swine wastewater treatment. Radioactive Tyagi, 2007, Mathias et al., 1996, Malekpour et al.,
K K12 [(AlO2 )12 (SiO2 )12 ] 8-ring (obstructed) 0.29 contaminants removal, gas adsorption, catalyst. 2008, Solache-Ríos, 2001)
P Na Na6 (AlO2 )6 (SiO2 )6 •5 H2 O GIS (gismondine) ca. 0.3 Wastewater treatment, agriculture (Cardoso et al., 2015, Cardoso et al., 2015,
Nissen et al., 2000)
X Na Na86 [(AlO2 )86 (SiO2 )106 ] 12-ring 0.84 4.5 Biotechnology, energy storage, gas adsorption, catalyst (Khodaverdi et al., 2016, Storch et al., 2008, Su and
Ca Ca40 Na6 [(AlO2 )86 (SiO2 )106 ] 12-ring 0.8 in the chemical industry Lu, 2012) (Feng and Peng, 2005,
Sr, Ba Sr21 Ba22 [(AlO2 )86 (SiO2 )106 ] 12-ring 0.8 Solache-Ríos, 2001)
Y Na Na56 [(AlO2 )56 (SiO2 )136 ] 12-ring 0.8 3.26 Petrochemical, Biotechnology, Oil refining (Solache-Ríos, 2001, Khodaverdi et al., 2016,
K K56 (AlO2 )56 (SiO2 )136 ] 12-ring 0.8 Degnan, 2000, Corma et al., 2002)
Mordenite Ag Ag8 [(AlO2 )8 (SiO2 )40 ] 12-ring 0.7 Gas adsorption, catalysis (Bajpai, 1986)
H H8 [(AlO2 )8 (SiO2 )40 ]
Silicate - (SiO2 )96 10-ring 0.6
ZSM-5 Na Na3 [(AlO2 )3 (SiO2 )93 ] 10-ring 0.6 2.07 Petrochemical (Solache-Ríos, 2001, Vermeiren and Gilson, 2009)

Environmental Advances 2 (2020) 100019

A. Khaleque, M.M. Alam, M. Hoque et al.
3. Methods of synthetic zeolite synthesis
Zeolites can be synthesized from different raw materials which can
be either natural or man-made. However, all raw materials are not suit-
able for synthesizing the zeolite from the economic point of view. Hence,
raw materials should have some properties. They should be cheap, read-
ily available, low production cost, selectivity, high production yield, and
less abundance of foreign substances. Till now, various physicochemical
and solvothermal methods have been adopted and developed to pro-
duce synthetic zeolites such as hydrothermal method (Sugano et al.,
2005), alkali-fusion method (Wajima et al., 2008), sol-gel method
(Tsujiguchi et al., 2014), and alkali-leaching method (Shoppert et al.,
2017). However, the choice of the synthesis approach depends on which
type of zeolite will produce. Each method has some advantages and few
limitations which are represented in Table 2. Following subsections de-
scribe different synthetic routes of zeolite from various raw materials.
3.1. Solvothermal method
Solvothermal synthetic method is the general term of using a solvent
by which zeolites can be synthesized. Water is by far the crucial solvent;
hence there is a unique term “hydrothermal” to define its use. How-
ever, many organic solvents such as alcohols (e.g., methanol, ethanol,
pentanol), ethylene glycol, hydrocarbons and pyridine have been used
successfully for the synthesis of zeolite (Sangeetha and Baskar, 2016;
Bibby and Dale, 1985). As with water these molecular solvents produce
significant autogenous pressure at elevated temperature. The properties
of the solvent used in this method can be either nonpolar or hydropho-
bic and hydrophilic polar solvent. In case of using ionic solvent (ionic
liquids), this term is assigned as ionothermal. Hence, all hydrothermal
and ionothermal methods are basically solvothermal method, while all
the solvothermal methods are not (Johnson and Arshad, 2014). Never-
theless, basic difference among them solvents remain in molecular form
in both solvothermal and hydrothermal while ionic in ionothermal syn-
thesis method. The ionic nature of ionic liquids reports specific proper-
Environmental Advances 2 (2020) 100019
Fig. 2. Zeolite A framework type and SEM image (a);
and zeolite P framework type and SEM image (b)
(Fruijtier-Pölloth, 2009).
ties such as low vapor pressures (Luo et al., 2008). A general schematic
representation of solvothermal processes is shown in Fig. 3.
The solvothermal methods not only depend on the temperature and
pressure but also on other factors such as reactant sources, composition,
silica and alkali ratio, ageing time, alkalinity, stirring conditions, inor-
ganic cations, seeding time, and solvent (Johnson and Arshad, 2014;
Abdullahi et al., 2017). Hence, this method offers easy and precise con-
trol of size, shape distribution, crystalline of the final zeolite product
through the proper adjusting the parameters (Table 3) (Kulkarni, 2007;
Smart and Moore, 2012). There have been multiple previous attempts to
synthesis zeolite via a solvothermal method. For instance, Takako et al.
(2012) reported the preparation of lithosite (−LIT) type aluminosili-
cate zeolites by the solvothermal treatment of low-silica zeolite pow-
ders dispersed in alcohol-containing KOH, and the mixture was treated
at 200−250°C for 15−120 h without stirring. Cui et al. (2014) devel-
oped zeolite omega from magadiite with well crystal structure and high
purity via solvothermal approach. However, it is convenient to use dif-
ferent synthesis method combinedly such as hydrothermal-solvothermal
(Setthaya et al., 2016) and microwave-assisted solvothermal method
(Jamil et al., 2016). For example, Jamil et al. (2016) illustrated the
ZSM-22 zeolite synthesis via a microwave-assisted solvothermal fabri-
cation method using different co-solvents such as ethanol, 2-propanol,
glycerol and ethylene glycol. In another study, Setthaya et al. (2016)
prepared Faujasite and P1 zeolites by the utilization of the hydrother-
mal and solvothermal method using the SiO2 and Al2 O3 sources from
rice husk ash and metakaolin, respectively. If alcohol is used as media
for zeolite synthesis, then nucleation rate and crystal growth of zeolite
particles are greatly affected. Despite the success of this work in cer-
tain aspects, it still suffers from using different organic solvents which
are environmentally harmful, energetic and time-consuming approaches
(Table 2) (Chen and Tang, 2019). However, this method is getting pop-
ular day by day.
3.1.1. Hydrothermal method
The hydrothermal technique is considered as the primary route of
the synthesis of zeolites (Rabenau, 1985). This approach is nothing but
 A. Khaleque, M.M. Alam, M. Hoque et al.
Table 2
An overview of different zeolite synthesis strategies from various raw materials.

Synthesis Reaction
method Raw materials Auxiliary materials condition Type of zeolite Advantages Limitations Ref.

Hydrothermal BFS HCl, H2 O, NaOH, 90°C for 2 h Zeolite NaA High Reactivity, low Expensive autoclave, (Sugano et al., 2005)
method NaAlO2 pollution and energy corrosive slurries
Rice husk ash H2 O, NaOH, Al2 O3 , 150°C for 48 h ZSM-5 Zeolite consumption, good crystal (Sari et al., 2015)
tetra propylammonium quality
hydroxide
H2 O, NaOH, 100°C for 48 h Zeolite T (Bohra et al., 2013)
tetramethyl
ammonium hydroxide,
KOH
Waste & glass HNO3 , NaOH, NaAlO2 96°C for 48 h Zeolite A (Tsujiguchi et al.,
materials 2014)
Paper sludge Diatomite, NaOH, H2 O 90°C for 12 h Zeolite NaP (Wajima et al., 2006)
Kaolin/ NaOH, H2 O, Na2 SiO3 , 80°C for 24 h Zeolite P (Atta et al., 2012)
metakaolin SiO2
H2 O, NaOH 90°C for 8 h Zeolite X (Ma et al., 2014)
Na2 SiO3 , SiO2 , NaOH 180°C for 14 h ZSM-5 Zeolite (Kovo et al., 2009)
Coal fly ash KOH, Deionized water 160°C for 24 h Zeolite K (Lakiss et al., 2020)
Lithium slag NaOH, H2 O 95°C for 8 h Zeolite NaX (Chen et al., 2012)
Windshield NaOH, H2 O. Ethanol, 90°C for 24 h Zeolite A (Kim et al., 2015)
waste NaAlO2
Halloysite NH4 Cl, NaCl, NaOH, 400°C for 2 h Zeolite NaA (Zhao et al., 2010)
mineral HCl
K-feldspar KOH, NaOH, H2 SO4 90°C for 12 h Zeolite A (Su et al., 2016)
Alkali fusion BFS NaOH, EDTA 600°C for 6 h Zeolite X, Use of low-grade raw High energy (Wajima, 2014)
method zeolite A materials & production of consumption and costs
Waste stone NaOH, H2 O, HCl 800°C for 1 h Zeolite X high-quality anhydrous (Wajima et al., 2008)
cake zeolite
Kaolin/ NaOH 850°C for 3 h Zeolite Y (Htay and Oo, 2008)
metakaolin NaOH 100°C for 24 h Faujasite (Atta et al., 2007)
Zeolite
Coal fly ash NaOH/Fly ash ratio of 550°C for 24 h Zeolite NaX (Fukasawa et al., 2017)
1:3
Porcelain NaOH, H2 O 80°C for 12h Zeolite 13X (Wajima and
wastes Ikegami, 2009)
Waste of iron Na2 SiO3, NaAlO2, 450°C for 1 h Zeolite A (Kim et al., 2015)
mine tailings NaOH, H2 O
SiO2 sinter and NaOH 90°C for 120 h Zeolite Y, P (Petkowicz et al.,
perlite 2008)

Environmental Advances 2 (2020) 100019

Alkaline Paper sludge HCl, NaOH 90°C for 4/8 h Zeolite A - - (Rojas-Valencia et al.,
hydrothermal 2014, Wajima and
method Ikegami, 2007)
BFS NaOH, NaAlO2, water 56-75 0 C Zeolite A (Sugano et al., 2005)
Alkali-leaching Rice husk ash NaOH, NaAlO2, water 100-300°C for Sodalite Allows impure raw Multistep, expensive (Shoppert et al., 2017)
method 2h Zeolite materials and which offers and time consuming
Fly ash NaOH, NaAlO2, water 90°C for 8 h A-X zeolite very efficient products (El-Naggar et al., 2008)
(continued on next page)
 A. Khaleque, M.M. Alam, M. Hoque et al.
Table 2 (continued)

Synthesis Raw materials Auxiliary materials Reaction Type of zeolite Advantages Limitations Ref.
method condition

Sol-gel method Rice husk ash HCl, H2 O, NaOH, 90°C for 24 h Zeolite NaY A versatile method, less Cost of precursors, (Wittayakun et al.,
KOH, NaAlO2 energy consumption, no difficult to avoid 2008)
Alumina disk Na2 SiO3 , methanol, 200°C for 172 ZSM-5 zeolite need special and residual porosity and (Tsujiguchi et al.,
cilica sol h expensive equipment. OH groups, 2014)
Silatrane TPAOH, ethylene - MFI zeolite precipitation of a (Phiriyawirut et al.,
glycol, NaOH, NaCl, particular oxide during 2003)
CH3 CN sol-formation
TEOS as TEOS, HCl, NaOH, H2 O 90 °C for 4 h MCM-22 (Wu et al., 2009)
precursor & 550 °C for 5 zeolite
h
Microwave - HCl, H2 O, NaOH, - Zeolite NaA Faster reaction, selective Difficulty in heat force (Sapawe et al., 2013)
synthesis NaAlO2 heating, higher control, water
- TEAOH, NH4F, NaAlO2 150°C for 4 h Zeolite beta temperature evaporation (Kim et al., 2004)
Coal fly ash NaP1 zeolite (Querol et al., 1997)
Coal fly ash H2 O, NaOH, 75 °C for 24 h, Na-A zeolite (Tanaka et al., 2008)
NaAlO2
Iono-thermal Metakaolin H2 O, NaOH, - NaY zeolite Production of large crystal High operating time (Wang and Yan, 2010)
synthesis NaAlO2 and easy to control crystal and production of
- 1-ethyl-3-methyl 180°C for 10 h SAPO-LTA composition toxic chemicals. (Lin et al., 2019)
imidazolium bromide, zeolite
Al [OCH(CH3 )2 ]3 ,
H3 PO4 , H2 O, HF, TEOS
and TPAOH
Solvothermal - Aluminum sulfate octa 180°C for 12 h. ZSM-22 (TON) Easy control over the size, Need for expensive (Kulkarni, 2007,
method decahydrate, DAH, zeolite shape distribution, autoclave and organic Smart and
KOH, DI crystalline product solvent. Moore, 2012,
Jamil et al., 2016)
Metakaolin and NaOH, RCI, C2 H5 OH, 120°C for 6 h Faujasite and (Setthaya et al., 2016)
rice husk ash CH3 OH, and DI P1 zeolite
Ultrasound Sodium Sodium silicate, 50°C and 60°C, Zeolite A simple, rapid reaction, and (Andaç et al., 2005)
energy method aluminosilicate sodium aluminate, DI, 2-15 h do not need any complex
solutions NaOH facilities, high crystal
Coal Fly Ash NaOH, HCl, Distilled Zeolite X growth rate, uniform (Kuwahara et al., 2010)
water particle size distribution
Metakaolin NaOH 550°C for 4 h LTA Zeolite and morphology and (Gordina et al., 2017)

Environmental Advances 2 (2020) 100019

DI provides control on the
Na2 Si2 O3 NaAlO2 180°C for 48 h ZSM-5 Zeolite nucleation process (Huang et al., 2016)
TPABr
NH4 NO3
TPAOH: Tetra propyl ammonium hydroxide, TEAOH: Tetra ethyl ammonium hydroxide TEOS: Tetraethyl orthosilicate, RCI: Ranong China clay, DAH: 1,6-diaminohexane, DI: Deionized water.
 A. Khaleque, M.M. Alam, M. Hoque et al.
Table 3
Properties of synthetic zeolites produced by different approaches.

Synthesis SiO2 /Al2 O3 Ion exchange BET surface area Microspore

method Structure ratio capacity (mg/g) (m2 /g) Crystal size Crystallinity (%) volume (cm3 /g) Ref.

Hydrothermal zeolite X 571 0.19 (Qiang et al., 2019)

zeolite X 2.93 560 1 to2 𝜇m 83 0.441 [933]
Zeolite X 1.13 248 453 0.2838 (Yao et al., 2018)
Zeolite Y 15 830 0.33 (Borel et al., 2017)
Solvothermal Faujasite and 4 487 100-1500 nm (Setthaya et al., 2016)
P1 zeolite
zeolite omega 14 282 (Cui et al., 2014)
ZSM-22 91.4 <100 nm 100 (Jamil et al., 2016)
Ionothermal SAPO-LTA 802.7 0.26 (Lin et al., 2019)
zeotype
NaY zeolite 17 655 150– 250 nm 0.34 (Wang and Yan, 2010)
Alkali-fusion NaY zeolite 2.5 1.0 𝜇m (Lee et al., 2018)
Zeolite A 0.5-3.2 302 500 (Ma et al., 2010)
zeolite X. 3.43 3.42meq /g 293 0.1169 (Mezni et al., 2011)
zeolite X 1.68–1.98 383 5.69 𝜇m 125.93 (Ojha et al., 2004)
Alkali leaching ZSM-5 zeolite 160 0.13 (Abello et al., 2009)
A-X zeolite 2.1 4.624 meq/g 593.64 96 (El-Naggar et al., 2008)
blend
Fe-ZSM-5 336 0.12 (Melian-Cabrera et al., 2006)
Sol-gel MCM-22zeolite 26 548 5 × 1 𝜇m 98 (Wu et al., 2009)
MCM-22 36 525 4 × 0.5𝜇m 100 (Wu et al., 2009)
MCM-22 16 531 9 × 3𝜇m 97 (Wu et al., 2009)
Microwave Zeolite Y 645 6–19 𝜇m 0.322 (Le et al., 2019)
NaY zeolite 10 474 44.4 nm 0.35 (Bunmai et al., 2018)
Zeolite beta 25 676 0.09 μm 95(sample-I) 0.22 (Kim et al., 2004)
Ultrasound Zeolite A 5 96 (60°C, (Andaç et al., 2005)
energy method approx. 6 h)
LTA type 83 2 μm 4.47 (Gordina et al., 2017)
Zeolite
Zeolite X 540.09 0.191 (Kuwahara et al., 2010)

Environmental Advances 2 (2020) 100019

(AFM-X) (AFM-X)
A. Khaleque, M.M. Alam, M. Hoque et al.
Fig. 3. General schematic of all solvothermal method (including hydrothermal and ionothermal) for the synthesis of zeolite.
solvothermal where water is used as a solvent, and a base is used as
a mineralizer at different temperatures and pressures (Fig. 3). Conven-
tionally, hydrothermal synthesis needs to use a sealed vessel usually
made of polypropylene and teflon-lined (PTFE) steel autoclave (Fig. 2)
(Sangeetha and Baskar, 2016). In this method, a lower temperature is
required. That is why, this method is very straight forward and cheaper
in comparing to other methods.
Zeolites are habitually synthesized via hydrothermal approach
(Cundy and Cox, 2003) due to some advantages agreed by differ-
ent researchers (Byrappa and Yoshimura, 2012; Julbe et al., 2000;
Rabenau, 1985), which includes low energy consumption, the high re-
activity of reactants, easy maintenance over the solution, lower air pol-
lution, formation of metastable phases and unique condensed phases
(Byrappa and Haber, 2001; Wu et al., 2006). There are many factors
which can affect the performance of any hydrothermal method for exam-
ple temperature and pressure, batch composition, silica and aluminum
ratio, reactant materials, overall alkalinity, aging time, template con-
Environmental Advances 2 (2020) 100019
dition, and seeding (Johnson and Arshad, 2014). To date, there have
been multiple previous attempts to synthesis zeolites via conventional
hydrothermal method. For example, Wang et al. (2007) illustrated the
preparation of synthetic zeolite (i.e., ZSM-5) from expanded perlite
(or kaolin) via the hydrothermal method. Another research group de-
veloped different hierarchical structured zeolites (BEA, LTA, FAU) via
conventional hydrothermal approach (Chen et al., 2011). However, re-
cently, many improvements have been put forward on this method. For
example, Yao et al. (2018) synthesized Zeolite X powder from diatomite
(i.e., a high silica content raw material with alumina) via a green and
the straightforward hydrothermal method. This zeolite X has great po-
tential for industrial, catalytic and adsorption technology applications.
Tsujiguchi et al. (2014) reported the synthesis of zeolite A from an alu-
minoborosilicate glass via hydrothermal approach. They conducted acid
treatment before hydrothermal treatment which was useful to produce
a single phase of zeolite A with high crystallinity. Municipal waste has
also been used to produce zeolite A as they are very cheap and had
A. Khaleque, M.M. Alam, M. Hoque et al.
higher alumina content (Terzano et al., 2015). Zeolite K–F was synthe-
sized from waste amber container glass by the utilization of a one-pot
hydrothermal method (Taylor et al., 2020). The advantages of this pro-
cess are that it does not require the pre-treatment for the activation
or the removal of hazardous components. However, the conventional
hydrothermal method does not satisfy the severe terms of sustainability
(Lee et al., 2003; Meng and Xiao, 2014). Meng and Xiao (2014) reported,
using structural directing agents, they assemble and fill the pore volume
of synthesized zeolites directly which constantly needs high tempera-
ture combustion to be removed. Therefore, there has a great chance of
hazardous and greenhouse gases production due to high temperature
combustion. Moreover, generation of high autogenous pressure in the
(PTFE-) lined steel autoclave because of heating the reaction mixture,
can develop a severe thread for the equipment. Also, the conventional
hydrothermal synthesis approach is often viewed as a high energy con-
sumption method because of taking a long period of times (1–20 days)
for final production. In addition, in conventional hydrothermal method
controlling of nucleation is difficult due to slow mixing hence uncon-
trollable nucleation leads to form larger crystal size (Li et al., 2006).
Although, an agitator is used to overcome such problem but it pro-
motes only the motion of macroscopic layers so mixing inside the lay-
ers depends on the slow diffusion of reactants molecule. To overcome
the above-mentioned limitations of conventional hydrothermal strategy
for zeolite synthesis, researcher have developed diverse means of sus-
tainable ways for synthesizing strategies such as microwave-assisted hy-
drothermal method (Rao et al., 1999), alkali fused hydrothermal method
(Bukhari et al., 2015), microwave digested-alkali fusion assisted hy-
drothermal method (Chen et al., 2020), and ultrasound-assisted hy-
drothermal method (Jusoh et al., 2017).
Microwave-assisted synthesis has characteristic ‘‘microwave effects”.
Katsuki et al. (2005) highlighted the zeolite synthesis through mi-
crowave heating which offered lower time requirement for the zeo-
lite production over the conventional hydrothermal method. After that,
they perceived, utilization of microwave heating throughout the syn-
thesis can be efficient to reduce synthesis reaction period. For example,
Chon et al. (1996) prepared NaY zeolites via microwave heating of 10–
15 min with high crystallinity and purity. Meng and Xiao (2014) stated
that excessive precaution is required during microwave heating other-
wise there may develop high pressure which can lead another reaction
especially in case of using low-boiling solvents. There also have been
reported about sonochemical-assisted hydrothermal for the synthesis
of zeolites. For example, Jusoh et al. (2017) reported sonochemical-
assisted hydrothermal growth of zeolite T. However, zeolite synthe-
sis, especially from waste raw materials, often have a chance to form
multiphase products and need long time (Li et al., 2018). Therefore,
alkali fusion prior to the hydrothermal treatment can shorten synthe-
sis time and prevent all the inert multiphase (Bukhari et al., 2015).
To date, there have been several attempts to synthesize zeolite via al-
kali assisted hydrothermal method. For example, the synthesis of zeo-
lite X has also been carried out from a low-grade bauxite raw material
by the utilization of a two-step synthesis method. They are alkali fu-
sion activation and hydrothermal reactions (Wang et al., 2013). On the
other hand, Belviso et al. (2017) used clay minerals to produce syn-
thetic zeolites (i.e., sodalite, faujasite and A-type zeolite). They used
alkaline hydrothermal route and pre-alkali fusion with or without the
addition of alumina (Wang et al., 2013). Industrial waste bauxite tail-
ings have also been used for zeolite X synthesis (Qiang et al., 2019).
Other raw materials such as waste perlite dust, fly ash and steel slag
have also been used for the synthesis of faujasite zeolite, Zeolite Y and
X via hydrothermal methods (Ojha et al., 2004; Belviso et al., 2017;
Wajima and Onishi, 2019; Kuwahara et al., 2008). Hence, the alkali fu-
sion method needs a higher temperature above 800°C and continuing for
2 h (Cui et al., 2012). However, to reach a higher temperature within a
very short period, researchers have imparted microwave heating system
into the alkali fusion hydrothermal method. For instance, Li et al. (2018)
proposed the synthesis of zeolite by the utilization of both microwave
Environmental Advances 2 (2020) 100019
digestion and alkali fusion assisted hydrothermal method. They used
coal fly ash as a raw material. Furthermore, Chen et al., (Mason and Pe-
ters, 2002) reported a fusion-pretreated microwave-assisted hydrother-
mal method for fabrication of zeolite from municipal solid waste incin-
eration (MSWI) fly ash. Fusion pretreatment transformed the quartz into
an amorphous form that’s why they dissolved easily into a hydrothermal
solution and after that zeolite fabrication was accelerated.
Having some disadvantages hydrothermal method still found
promising for producing faujasite, X, Y and ZSM-5 type zeolites suit-
able for particular applications. In summary, the synthesis of zeolites
by the utilization of the hydrothermal method has great potential with
huge advantages (Chandrasekhar and Pramada, 1999).
3.1.2. Ionothermal method
Ionothermal synthesis refers to the use of ionic liquids and they
are mainly based on the low vapor pressures compounds (Fig. 3)
(Barrer, 1982). Hence, ionic liquids act as both the solvent and potential
template or structure directing agent simultaneously in the formation of
solids. Generally, hydrothermal, solvothermal and ionothermal meth-
ods are similar, except for the use of different solvents (Parnham and
Morris, 2007). Hence, these three methods have similar factors for the
synthesis of zeolites (Abdullahi et al., 2017). The ground-breaking of
this area reported by Cooper and his coworkers in 2004, they used
deep eutectic solvents (e.g.,1-ethyl-3-methylimidazolium bromide and
urea/choline chloride) to prepare several distinct materials depending
on the conditions (Cooper et al., 2004). The crucial advantage of this
method is that the solvent can act as template or structure-directing
agent and after getting products it is relatively easy to remove them since
both solvent and template are the same species (Cooper et al., 2004).
In addition, the ion thermal method produces a large size of crystals
and the ability to create a crystalline phase. It is also easy to control
the composition of growing crystals (Meligrana et al., 2006; Yoldi et al.,
2019). But the drawbacks are the production of toxic chemicals and high
operating time (Table 2). Several studies have also been reported to syn-
thesize zeolites. For example, the first time, in 2004, Cooper et al. (2004)
reported the use of an ionic liquid or eutectic mixture as the solvent to
produce synthetic zeolite. Recently, this method has received a growing
interest among zeolite scientific community. There are many reports on
the preparation of synthetic zeolites using this method. For instance,
Wang and Yan (2010) reported the synthesis of nano-sized NaY zeolite
from metakaolin by ionothermal method together with the microwave-
assisted method. In a different study, Wang et al. (2019) reported the
successful ionothermal synthesis of germanosilicate zeolites. However,
the more depth study is required to get a full judgement of this synthesis
technology.
3.2. Alkali-fusion and leaching method
In zeolite synthesis, alkali fusion method describes a general ap-
proach to decompose the material rich with silica or alumina in the
presence of alkali which acts as an activator for the formation of soluble
aluminate and silicate salts. Solvothermal methods also use alkali (e.g.,
NaOH) but there have some differences between solvothermal and alkali
fused method. In alkali fusion method alkali is used to prevent multi-
phase and fused in solid-state with raw materials before going to any sol-
vent while in solvothermal method, alkali is used in terms of solution
state and they act as mineralizer of the reaction medium. Generally,
in the alkali-fusion method, the raw material is first fused with alkali
(e.g., NaOH) before a hydrothermal treatment (Fig. 4) (Belviso et al.,
2017; Ayele et al., 2016). At the hydrothermal treatment, the fused
product mixed with water and treat with the proper conditions like heat-
ing with appropriate temperature for the crystallization to form zeolite
(Christidis and Papantoni, 2008).
Factors affecting the alkali-fusion methods are: (i) silicon aluminum
ratio of the raw material, (ii) concentrating the reacting alkali medium,
A. Khaleque, M.M. Alam, M. Hoque et al. Environmental Advances 2 (2020) 100019

Fig. 4. A schematic representation of zeolite synthesis via alkali-

fusion method.

(iii) temperature, and (iv) crystallization rate (Ma et al., 2010). Previ-
ously, many works were carried out to synthesis zeolite via this method.
For example, Ojha et al. (2004) reported the synthesis of X-type zeo-
lite by alkali fusion (e.g., sodium carbonate as an activator) followed
by hydrothermal treatment by using coal fly ash as a raw material. It
was found that alkali activator has a significant influence on the synthe-
sis of synthetic zeolite (Ma et al., 2010). In addition, Takaaki Wajima
illustrated the alkali fusion method to synthesize zeolite-A, zeolite-X
and hydroxysodalite from the BFS (Wajima, 2014). In a previous study,
Chen et al. (2012) reported the synthesis of zeolite X from the lithium
slag by hydrothermal reaction with alkali fusion. They mentioned excel-
lent properties the zeolite. Moreover, in most of the processes, the alkali
fusion technique is followed by a hydrothermal method of synthetic ze-
olite. Both methods require high temperatures, time, and pressures. The
main sources for zeolite synthesis are commercial chemicals, which are
very rich in alumina silicate, mineral resources in the earth’s crust and Fig. 5. Alkali leaching method for synthesis of zeolite.
industrial by-products (Belviso, 2008; Kuwahara et al., 2010). By vary-
ing the experimental conditions different types of zeolite products can
be obtained, such as zeolite-X, zeolite- P, hydroxy sodalite, tobermorite,
and nepheline. This method allows low-grade raw materials without pu-
rification, and it offers the anhydrous zeolite with high purity, which is
considered as the advantages of this method (Yoldi et al., 2019). While
it still has the problems of high energy consumption and the associated
cost (Lei et al., 2009).
Alkali leaching is another approach where the leaching maintains
the silica-alumina ratio out of the leachates such as NaOH solution
(Wang et al., 2012). The schematic representation of this method is
shown in Fig. 5. The factors that affect the alkali leaching method are:
(i) desalination rate, (ii) silica-alumina ratio of leachate free solid prod-
uct, (iii) fusion temperature, (iv) concentration of leaching agent and (v)
crystallization rate (Melián-Cabrera et al., 2006). Several investigators
Fig. 6. Sol-gel method for synthesis of zeolite.
have reported different zeolites synthesis via alkali leaching approach.
For instance, El-Naggar et al. (2008) synthesized the pure zeolites by al-
kaline leaching method from the silica extract which was obtained from 3.3. Sol-gel method
the fly ash. Their synthesized A-X zeolite blends had the greatest po-
tential for the sorption of cesium ion. Another group of researchers has It is a physicochemical process that involves the formation of an in-
reported the preparation of mesoporous ZSM-5 zeolite catalysts using organic colloidal suspension (sol), and the gelation of the sol in a contin-
organic hydroxides by using alkali leaching and desalination methods uous liquid phase (gel) to form a three-dimensional network structure
(Abello et al., 2009). According to their finding’s, the silicon dissolu- (Fig. 6) (ul Haq and Akhtar, 1997). The sol-gel process encompasses
tion in tetraalkylammonium hydroxides was much slower than in NaOH the transition of a solution system from a liquid “sol” into a solid “gel”
making the demetallation process highly controllable hence producing phase. This method provides better control of the technique which ulti-
different quality of zeolite. The main benefit of this route is to get a very mately provides higher porosity and definite particle size (Brinker and
efficient product (Table 2). However, this method often suffers from the Scherer, 2013).
need of multistepa, require a significant amount of time and expensive, There are several factors which can influence the performance of this
which need to overcome in future (Melián-Cabrera et al., 2006). method. They are: (i) hydrolysis rate, (ii) temperature, (iii) heating rate
A. Khaleque, M.M. Alam, M. Hoque et al.
and (iv) pH (Serrano et al., 1995; Han et al., 2007). There are many
reports on this method. For example, Han et al. (2007) prepared the hi-
erarchical porous zeolite materials by the utilization of a template-free
method. This method involved with hydrothermal recrystallization of
the Xerogel to form ZSM-5. Wu et al. (2009) reported a two-step sol–gel
route for the synthesis of MCM-22 zeolite under static hydrothermal con-
ditions using tetraethyl orthosilicate as a silica source. Phiriyawirut et al.
(2003) synthesized the MFI zeolite directly from the silatrane. The reac-
tion temperature was varied by the utilization of the microwave heating
technique. They reported that a long ageing time is more important to
achieve high crystallinity. Sathupunya et al. (2002) illustrated the syn-
thesis of analcium (ANA) and gismondine-type (GIS) zeolites directly
from the precursor of alumatrane and silatrane this technique together
with microwave-assisted method.
The major advantage of this method is that this method does not
require the specialized and expensive equipment’s. Steps of the sol-gel
method is represented in Fig. 6 (Wittayakun et al., 2008). This method
offers a high-quality product with homogeneity due to mixing at the
molecular level (Hench and West, 1990). Besides various advantages,
there are some limitations such as the cost of precursors which need to
overcome in the future (Table 2) (Hench and West, 1990).
3.4. Microwave method
Microwave heating is a fast and energy-efficient technique in where
microwave radiation is applied for the synthesis of zeolites (Rao et al.,
1999). In this method, microwaves act as high-frequency electric fields
which eventually produce heat to carry out the reaction (Li and
Yang, 2008). Hence, the energy transfer from the microwave to the
reactant material occurs either through the resonance or relaxation
(Rao et al., 1999; Xu et al., 2000; Arafat et al., 1993). There are many
advantages of using microwave methods. For example, it gives concise
time, which leads to small particle size and high purity zeolite can be
obtained (Fig. 7) (Xu et al., 2000).
Factors that affect for the microwave method are (i) SiO2 /Al2 O3 mo-
lar ratio (Si/Al), (ii) alkalinity, (iii) wavelength produced from the mag-
netron, (iv) zeolization time and temperature, (v) crystallization time
and temperature (Shon et al., 2004). In most of the cases, microwave-
assisted synthesis of zeolite is applied in combination with other meth-
ods such as hydrothermal, solvothermal and ionothermal (Le et al.,
2019; Xu et al., 2001; Hwang et al., 2004; Somani et al., 2003; Ou et al.,
2017; Khalil and Muraza, 2016). For example, Kim et al. (2004) uti-
lized microwave the irradiation for synthesis of synthetic zeolite beta
in fluoride media. In their experiment, they showed the role of fluoride
mineralization under microwave and seeding to reduce the particle size
due to higher nucleation. Recently, Le et al. (2019) proposed a rapid
microwave heating method for the liquid phase synthesis of Y-type zeo-
lite under high-temperature conditions. The effect of microwave heating
temperatures, crystallization time and silica to alumina ratio on the syn-
Environmental Advances 2 (2020) 100019
Fig. 7. Microwave methods for synthesis of zeolite.
thesis of Y-type zeolite is systematically investigated. From 1990 to on-
wards, the major attempts on zeolitization of fly ash have been made by
Mondragon et al. (1990). Thereafter, several research works have been
reported on the synthesis of zeolites from fly ash (Amoni et al., 2019;
Ramírez et al., 2019; Joseph et al., 2020). For example, Querol and his
coworkers reported conventional and microwave-assisted hydrothermal
alkaline activation experiments to synthesis zeolite (Querol et al., 1997).
Different zeolitic materials (e.g., NaP1, hydroxy sodalite, hydroxycan-
crinite, analcime, tobermorite, and nepheline hydrate) with varying de-
gree of properties were synthesized from the same fly ash by changing
the synthesis parameters by using NaOH as an activation agent.
3.5. Ultra-sound energy method
The ultrasound with frequency 20 kHz to 2 MHz is the branch
of termed sonochemistry which is widely used in synthetic chemistry
(Mason and Peters, 2002). Ultrasound has significant influences in dif-
ferent types of synthesis cases such as various amorphous or crystalline
materials synthesis and polymerization reactions (Amara et al., 2001).
Because of high influences on crystallization, application of ultrasound
has been received much more attention in the field of zeolite synthe-
sis. The advantages of this method are very simple, rapid reaction, and
do not need any complex facilities, high crystal growth rate, suitable
particle size distribution and morphology and provide control on nu-
cleation process (Table 2) (Andaç et al., 2005; Gora et al., 1997). Ultra-
sound develops cavitation, and this cavitation is the result of the growth
and explosive collapse of microscopic bubbles (Boels et al., 2010). The
cavitation can also raise the secondary nucleation rates and the crys-
tal purity in the time of cooling crystallization (Suslick et al., 1990;
McCausland et al., 2001). Owing to the various traditional and emerg-
ing applications of synthetic zeolites, ultrasound energy method offers
zeolite synthesis with tunable properties (Table 3). Temperature, time,
and the molar ratio of reactants are considered as the main parameters
to determine the type and characteristics of the zeolite formed. Ultra-
sound energy method have been used extensively to synthesis zeolites.
For example, Pal et al. (2013) illustrated the synthesis of NaP zeolite
nanocrystals at ambient temperature within short crystallization time
via the ultrasound method. Herein, sonication energy enables to form
of active radicals which lead to rapid crystallization of zeolite phase.
Synthesis of hierarchical structured ZSM-5 zeolites with a long-life cat-
alytic activity was also reported via the ultrasound-assisted method
(Huang et al., 2016). However, the ultrasound method is also imple-
mented with other conventional methods to develop zeolite materials
more efficiently. For instance, SSZ-13 zeolite identified as effective cat-
alysts activity for long but needed the long crystallization period which
was the main difficulty for the industry application. In this purpose,
Mu et al. (2017) reported pre-treatment prior to hydrothermal crys-
tallization with a sonochemical-assisted method to synthesis of SSZ-13
zeolite which reduced the time requiring for zeolite synthesis. It was
A. Khaleque, M.M. Alam, M. Hoque et al.
proposed that the possibility of using ultrasound irradiation of pristine
zeolite Y were intensified by the alkaline treatment step (Zhang et al.,
2020). However, ultrasound energy-assisted method are being attract-
ing to researchers due to their great influence in zeolite synthesis.
4. Comparison among different raw materials for zeolite synthesis
Synthetic zeolite is also known as molecular sieves, and until now
there are more than 200 species have been reported (Zhao, 2010;
Sillanpää and Bhatnagar, 2015). Among them zeolite A, zeolite Y, ZSM-
5, Aluminophosphate (AlPO-5) (Jhung et al., 2004), silicoaluminophos-
phate (SAPO-5/SAPO-34) (Jhung et al., 2003), SBA-15 (Kruk et al.,
1997; Luan et al., 1999), SBA-16 (Dong et al., 2011), and Lynde (LTA)
(Luan et al., 1999) type zeolites are mentionable. Synthetic zeolites have
versatile applications ranging from the environmental to medicinal ap-
plications. Hence, more emphasis is given on the basic understanding of
the chemistry of zeolite structures and different routes of preparations
(Moshoeshoe et al., 2017). Apart from this, many attempts have also
been given on the use of different sources of raw materials in order to
get a suitable zeolite having versatile properties. But, the main parame-
ter is the proper content of the alumina and silica in the raw materials.
There are many natural sources of aluminosilicate such as clay mate-
rials. For example, obsidian is a natural raw material which is originated
from volcanic ejecta. It has a similar range of silica and alumina compo-
sition as like as perlite composition (Belviso, 2016). In contrast to per-
lite, obsidian has lower amount of water content. Due to the availability
of volcanic glass (i.e., ilicic, alkalic, mafic), several attempts have been
reported for the synthesis of zeolite from natural obsidian (Kawano and
Katsutoshi, 1997; Mamedova, 2014; Mamedova, 2016). However, most
of the studies were focused on the hydrothermal synthesis method. For
example, Belviso (2016) synthesized hexagonal polytype of cubic fau-
jasite (FAU) type zeolite using low temperature (∼30°C) hydrothermal
incubation. Mamedova (2014; 2016) investigated zeolite crystallization
at a varied temperature range of temperature (150–250°C). Only a few
experiments have found which described its potential use as zeolite.
Therefore, more investigation is required to examine the behavior of
these volcanic glass material as a potential source of raw material.
Coal fly ash, a by-product of coal combustion, is one of the most
abundant industrial solid wastes which is used for the zeolite synthe-
sis. The main components of coal fly ash are Si- and Al-containing
compounds. However, when toxic metallic elements are present, they
may restrict the full application of such materials to synthesize zeolites
(Amoni et al., 2019; Inada et al., 2005). On the other hand, the RHA is
a residue rich in amorphous silica, and it is very active in the synthesis
of zeolite. The chemical analysis reveals that RHA contains 90%–99%
of silica (Table 4). RHA is very cheap which can be used in several in-
dustrial sectors (Kamseu et al., 2017; Alam et al., 2020). The synthesis
of crystalline aluminosilicate zeolites can be carried out from the clay
minerals such as kaolinite. The improvement of the properties of kaoli-
nite by the chemical method is difficult due to its low reactivity. Thus
clay mineral is not significantly affected by acid or alkaline treatments
even under strong conditions. Previous work has also been shown that
kaolin is not stable under highly alkaline condition, and different ze-
olitic materials can form (Abbott et al., 2003; Tavasoli et al., 2014). Af-
ter dehydration, kaolin is transformed into amorphous metakaolin. Raw
kaolin and metakaolin have been used as the Al and Si sources for syn-
thesis of zeolite Linde Type A, X, Y, P, 4A, NaA, KI, cancrinite, sodalite,
hydroxysodalite, faujasite, phillipsite, chabazite and several other types
of zeolites (Abbott et al., 2003; Tavasoli et al., 2014). However, the
synthesized products are contained quartz phases as impurities coming
from the natural kaolin samples. Similarly, perlite is a naturally occur-
ring volcanic rock and it is characterized by an amorphous structure
(Wajima and Onishi, 2019). Expanded perlite has a very high bulk den-
sity and vesicular structure, which results in a multitude of applications.
However, expanded perlite waste sub-grain is formed in the production
process, which is due to the high volatility and the difficulty in storing
Environmental Advances 2 (2020) 100019
(da Silva Filho et al., 2018). Waste perlite is a source of reactive silica,
and therefore it can be used for the synthesis of zeolites.
Glass and aluminum are recycled through a process where high tem-
perature is used (Taylor et al., 2020). Hence, the waste glass can be
converted into high value-added materials like zeolite. Since waste glass
has a high proportion of SiO2 , it is proposed as a suitable precursor for
the zeolite synthesis via a hydrothermal process (Taylor et al., 2020).
Unlike other glass type industrials silicate containing materials, amber
container contains a smaller number of hazardous elements. Therefore,
in most of the cases, there is no requirement of pretreatment. However,
phase pure zeolite is hardly produced without any pretreatment par-
ticularly for the application in the biomedical and chemical separation
process and any particular industrial, agricultural application. For ex-
ample, pretreatment such as treatment with acid or alkali was used to
produce single-phase zeolite (Kim et al., 2015; Kamitani et al., 2014). On
the other hand, some studies reported without pretreatment (Kim et al.,
2015; Kamitani et al., 2014; Majdinasab et al., 2019). However, when
it is not the major concern to get single phase zeolite, pretreatment pro-
cess can be avoided to simplify and make feasible the synthetic process
(Majdinasab et al., 2019).
Another potential source of raw materials for zeolite synthesis is the
BFS. BFS mainly consist of CaO, SiO2 , Al2 O3 and MgO as well as slight
amounts of Fe, Ti and Mn as metallic elements (Sugano et al., 2005;
Kuwahara et al., 2010). Previously, zeolite synthesis from BFS reported
by several groups, but previously attempted to use BFS as a chemical
source of zeolite were limited by the compositional complexity, more
accurately and presence of significant Ca content (Sugano et al., 2005).
Consequently, recently, a novel synthetic method of a hydroxyapatite-
zeolite micro composite from BFS reported. This process only required
cheap chemical reagents, H3 PO4 and NaOH, and convenient prepara-
tion procedures. This conversion process offers novel solutions to waste
(Kuwahara et al., 2009). Still, more research is required for produc-
ing diverse types of zeolites for potential applications such as catalysts,
biotechnology, and gas separation.
In contrast to natural zeolite, the use of industrial waste as a raw ma-
terial for zeolite synthesis has huge environmental significance. Some
industrial wastes such as BFS, iron ore tailing, rice husk ash, coal fly
ash, lithium slag, paper sludge ash and so many can be used as raw
materials for the zeolite synthesis as they have a significant amount of
silica/alumina content in their composition. The main benefit of using
different industrial wastes is that it can reduce environmental pollution.
However, not from all sources discussed above have excellent zeolitic
properties, but zeolites synthesis from clay (kaolin), waste pearlite, coal
fly ash, rice husk ash, and glass type materials were found to be most
promising materials. Many synthetic approaches have adopted for pre-
viously and recently for effective resolution of synthetic zeolites and im-
prove the efficacies. Till now, zeolites from clay materials (e.g., kaolin,
metakaolins) and coal fly ash found very potential for versatile applica-
tions.
5. Environmental applications of synthetic zeolite
Zeolites are widely used in various technological applications such
as environmental engineering (e.g., water treatment and water soften-
ing), as a catalyst and molecular sieves materials, for the removal of ra-
dioactive contaminants, biotechnology and biomedical applications and
petrochemical application. These applications of zeolites were typically
related to their specific properties. Although zeolite has many types of
applications, we keep our discussion mainly on environmental engineer-
ing sections such as water and wastewater treatments, and gas adsorp-
tion only.
5.1. Synthetic zeolites for contaminants removal
Zeolite is well-known materials for the treatment of water and
wastewater contaminants. Recently, zeolites are used for water soften-
 A. Khaleque, M.M. Alam, M. Hoque et al.
Table 4
Advantages and disadvantages of different industrial waste for producing synthetic zeolites.

Raw Materials Chemical composition % Advantages Disadvantages Synthesis route Zeolite Ref.

Natural 80.04% Si02 , 12.27% Higher silica content, Still limited study Hydrothermal Organic (Belviso, 2016,
obsidian Al2 03 , 0.16% availability found not mentioned template-free Kawano and
Ti02 , 0.84% any specific EMT-type, Katsu-
FeO, 0.18% MgO, application. Due to natrolite, toshi, 1997,
1.10% CaO, 3.14% Na2 O wide range of behavior Za-gmelinite Mamedova, 2014,
and 3.04% K2 0 change with respect to Mamedova, 2016)
synthetic condition.
BFS CaO (40.1), SiO2 Availability, low cost, Higher CaO content Hydrothermal A (Sugano et al.,
(34.58), A12 O3 (14.78), convenient preparation 2005)
MgO (5.29) steps (Kuwahara et al.,
2010)
RHA 80% silica, Al2 O3 , iron Low cost, ultrafine Pre-treatment of RHA Hydrothermal ZSM5, T, NaY (Kamseu et al.,
oxide, CaO, MgO, size, highly porous and and waste glasses 2017)
sodium and potassium chemically reactive. increase the cost (Zhang et al.,
oxides, and others 2019) [1912]
Waste glass SiO2 (63%), Al2 O3 Excellent mechanical Problem in handling, Hydrothermal A
materials (18%), B2 O3 (10%), and and thermal need a substrate or (Tsujiguchi et al.,
alkaline earth oxides properties, free of base material for 2014)
harmful elements commercial use. (Taylor et al.,
2020)
Paper sludge SiO2 35.9 Al2 O3 22.8 Amorphous and Low abundance of Si Hydrothermal Na-P1 (Mun and
ash CaO 33.2 Na2 O 0.6 crystalline phases and significant Ca Ahn, 2001)
MgO 4.5 Fe2 O3 0.9 formed by content.
TiO2 2.2 incineration, low
temperature required
Waste stone SiO2 38.9 Al2 O3 12.2 Specific pore sizes and Most of SiO2 and Hydrothermal, zeolite-A, P, X (Barrer, 1978)
cake CaO 6.9 Na2 O 1.4 K2 O large surface areas, Al2 O3 are in crystalline Alkali fusion and ZSM-5 (Wajima et al.,
1.8 MgO 2.7 Fe2 O3 3.1 high silica content phases, it is difficult to 2008)
CO2 32.6 SO3 0.1 P2 O5 dissolve into alkali
0.1 solution, contains
impurities
Clay materials SiO2 46.5, Al2 O3 41.18, Availability, convenient High energy Hydrothermal, NaA, (Abbott et al.,
(kaolin, Fe2 O3 0.19, TiO2 0.13, source for producing consumption processes Alkali fusion mordenite, 2003,
smectite) MgO 0.04, K2 O 0.13, low silica zeolites like like grinding, faujasites, and, Tavasoli et al.,
Na2 O 0.18, ZrO2 0.01, Y, use of kaolin waste calcination, fusion NaP 2014)

Environmental Advances 2 (2020) 100019

SO3 0.15, P2 O5 0.03, for zeolite synthesis required. Raw
LOI 16.25 reduce the cost of materials mining
reagents destroys the natural
landscape.
(continued on next page)
 A. Khaleque, M.M. Alam, M. Hoque et al.
Table 4 (continued)

Raw Materials Chemical composition % Advantages Disadvantages Synthesis route Zeolite Ref.

Coal fly ash SiO2 38.3, Al2 O3 34.8, Main constituents are Effect of the impeller Hydrothermal, X, Na‐P1, A, Y (Inada et al.,
CaO 11.0, Fe2 O3 8.1, silica and alumina, type and agitation microwave- 2005)
Others 7.8 which offer the during the assisted (Amoni et al.,
potential of converting hydrothermal hydrothermal 2019)
it to zeolite, Produce treatment stage of the method and
low price zeolite with process. fusion
high purity, no methods.
harmful effect.
Lithium slag SiO2 70.67, Al2 O3 High silicon aluminum Very few experiments Hydrothermal X, FAU/LTA (Lin et al.,
27.24, Fe2 O3 0.52, ratio have been addressed 2015)
SO3 0.45, CaO 0.29, in this field.
K2 O 0.22, MgO 0.16,
Na2 O 0.13, P2 O5 0.12,
Others<0.1
Waste of iron SiO2 -67.58, Al2 O3 Have economic and Very few experiments Hydrothermal A, ZSM-5 (Zhang and
mine tailings/ -8.70, Fe2 O3 -7.42, environmental aspects. have been addressed Li, 2018)
iron ore tailing CaO-5.78, MgO -4.37, on this field, contains
K2 O-2.32, Na2 O-2.15, hazardous impurities
Cl -0.69, TiO2 -0.33, which decrease the
P2 O5 -0.26, SO3 -0.23, quality of zeolites
MnO -0.10,
SrO -0.06
waste pearlite SiO2 – 75.39%, Al2 O3 – Good source of High volatility, Hydrothermal X, Na-P1 (Wajima and
13.36%, Na2 O – 4.61%, reactive silica > 70 % impurities such as Onishi, 2019)
K2 O – 4.11%, Fe2 O3 – and therefore can be CaO, K2 O, Fe2 O3 and (da Silva Filho
1.22%, CaO – 0.97%, used in the synthesis Cl, are present in et al., 2018)
MgO – 0.11%, and of zeolites perlite dust which
others – 0.23% disrupts the zeolite
synthesis.

Environmental Advances 2 (2020) 100019

A. Khaleque, M.M. Alam, M. Hoque et al.
ing purposes. Zeolites are hygroscopic compounds with ion-exchanging
properties. Hence, zeolites can soften hard water by exchanging Ca2+
ion and Mg2+ ion for Na+ ion. Also can prevent the precipitation of sur-
factants. Usually, they are used as a pure powder which does not contain
additive or clay binder. Various applications of synthetic zeolite are pre-
sented below.
5.1.1. Heavy metal, cation and anion removal
Zeolite exhibit great potential to remove cationic heavy metals
(HMs) species from industrial wastewater. It is well known that HMs
have many adverse effects on the environments and biological systems.
Various adsorbents or ion exchange materials are used to treat HM con-
taminated water and wastewater. As a part of this, both naturally oc-
curring zeolites and synthetic zeolites are successfully applied to adsorb
a wide range of HM cations such as Cu2+ , Cd2+ , Cr6+ , Zn2+ , Pb2+ and
Hg2+ from various contaminated water streams. Among the different ze-
olite as sorbents, fly ash-based zeolites, particularly, are gaining popu-
larity amidst researchers. Due to low-cost and bulk availability, presence
of well-defined molecular and porous structure, high thermal stability,
ion selectivity, ion exchange capacity and high surface area (Petrus and
Warchoł, 2005; Nascimento et al., 2009). The HM removal efficiency of
fly ash zeolites was much higher compared to raw fly ash, which was
mainly attributed to their mineralogical alteration (Kolay et al., 2001;
Kolay and Singh, 2000). For example, only raw fly ash removed less
than 8% of Pb2+ , while its zeolitized counterpart showed up to 98%
removal of Pb2+ (Lee et al., 2000). Another study reported that zeolite
synthesized from coal fly ash had high adsorption capacity for different
HM cation adsorption in an artificially polluted medium (Ji et al., 2015).
The calculated maximum adsorption capacities of zeolite for Cu2+ , Cd2+ ,
Cr6+ , Zn2+ and Pb2+ in seawater were 3.057, 1.123, 0.325, 13.101 and
6.116 mg g−1 , respectively. In two particular experiments, zeolite from
fly ash collected from thermal power plants was used. It was found that
the removal efficacies of Fe, Mn, Cu, Zn, Pb, Cd and Ni were 99 %, 100
%, 90 %, 100 %, 100 %, 100 %, and 100 %, respectively (Prasad and
Kumar, 2016). In addition, zeolite produced from Indian fly ashes and
raw fly ash were used to treat two British acidic mine waters. The re-
sult demonstrated that fly ash- zeolites were more effective than raw fly
ash. Fly ash has been found effective for the removal of Pb (Prasad and
Mortimer, 2011).
Table 5 summarizes the results of some studies on removing toxic
HMs with different synthetic zeolites. Adsorption properties of chi-
tosan/zeolite conjugate films were evaluated for removing Cr4+ ions
and excellent adsorption capacity was observed (Jain and K, 2000). The
positive effect of zeolitic materials on adsorption of other HM cations
has been studied thoroughly. For instance, the remediation of Cu2+ tox-
icity in Jawa tilapia by using a faujasite zeolite was reported (James and
Sampath, 2003; Chaurasia and Jain, 2006). Moreover, many HMs have
successfully been removed from water and wastewater streams which
indicates the capability as well as the selectivity of zeolite materials
toward HMs (Yuna, 2016). In summary, synthetic zeolites have higher
potentials in the removal of HMs from water and wastewater.
The use of cation and anion exchangers in waste-water treatment to
remove inorganic contaminants is practiced widely. Synthetic zeolites
have great potential for the capture of cations from waste-water selec-
tively. Synthetic zeolites such as mordenite and faujasites can act as a
cation exchanger (Dyer et al., 1993). Zeolites prepared from the coal
fly ash was found the most promising materials for the cation removal
(Table 6). It was also found that zeolites 4A and Na–P1 had higher cation
exchange capacities for calcium ion and ammonium ion exchange (i.e.,
zeolites 4A: 4.5 meq Ca2+ g−1 and zeolites Na–P1: 2.6–2.8 meq NH4 +
g−1 ) (Cardoso et al., 2015). Additionally, zeolite prepared from kaolinite
can work as a cation exchanger (Barrer and Munday, 1971). High con-
centrations of Na+ are undesirable in water, which can be absorbed by
soil, and eventually may cause soil aggregation and reduce permeability.
Therefore, sodium concentration is an important parameter when eval-
uating the suitability of wastewater for irrigation (Gibb et al., 2017).
Environmental Advances 2 (2020) 100019
The use of zeolite in Na+ reduction process is opposite to that in the
water softening process as other cations such as Ca2+ or NH4 + in ze-
olites replaces Na+ in the saline and sodic water. The removal of salt
from wastewater much depends on three closely-correlated processes:
ion exchange, adsorption, and salt storage (Wen et al., 2018).
Zeolite has a net negative structural charge like clay materials which
can substitute cations from the crystal lattice. Due to this negative
charge, zeolites have little or no affinity for anionic species. Ion ex-
change of a quaternary amine and an extra structural cation (i.e., Na, Ca,
K) on the zeolite’s external surface may neutralize the negative charge
but should not reverse it. Therefore, little or no sorption affinity has
been reported for anions exchange by zeolites. However, in the previ-
ous report it was found that the quaternary amine hexadecyltrimethy-
lammonium zeolite showed the strong sorption of inorganic oxyanions
(e.g., chromateand sulfate) from aqueous solution (Haggerty and Bow-
man, 1994). Modified zeolite and Al-modified zeolites (Hermassi et al.,
2016), and surfactant modified zeolites (Sun et al., 2011) were devel-
oped to remove anionic phosphates and organic pollutants. Although
many studies have been carried out in the removal of cations, but still
need more study in order to dig more information about the mechanism
of action and need to prepare more suitable synthetic zeolite with higher
ion exchange capability.
5.1.2. Removal of organic contaminant
Natural and synthetic zeolites have been attracting great attention
for removing organic and inorganic pollutants, contaminants (e.g., ani-
line, cationic surfactants, phenol, and sulfonamide antibiotics) because
of their high sorption capacity, larger specific surface area, and high se-
lectivity (Table 7) (Amin et al., 2010; Peng et al., 2015). Recently, nano-
crystalline zeolites have been synthesized with favorable properties for
adsorption processes. In a recent study, Fe-nano zeolite (Fe-NZ) for the
treatment of phenolic compounds in wastewaters have been prepared.
The maximum adsorption capacities of phenol (Ph), 2-chlorophenol (2-
CP) and 2-nitrophenol (2-NP) using Fe-NZ were found to be 138.7, 158.9
and 171.2 mg/g, respectively (Tri et al., 2020). Maximum removal effi-
ciencies of 4-nitrophenol were 90% and 80% using synthetic zeolite and
kaolin clay, respectively (Ahmedzeki et al., 2013). On the other hand,
surfactant modified fly ash zeolite Na-P1 had the adsorption capacity for
phenol, p-chlorophenol, bisphenol A 37.7 mg/g, 52.4 mg/g, 90.9 mg/g,
respectively (Xie et al., 2012).
Surface modification of zeolites using different surfactant can signif-
icantly increase the adsorption properties of zeolites. Previous studies
showed that the surfactant modified zeolite was widely used for ex-
traction of phenol and 4-chlorophenol (Chen et al., 2007), chromate
(Zeng et al., 2010; Cordoves et al., 2008), acid dye (Mirzaei et al.,
2016), nitrate (Schick et al., 2010), aromatic hydrocarbons (Vidal et al.,
2011), volatile organic compounds (Altare et al., 2007), and BTEX (Ben-
zene, Toluene, Ethylene, o-Xylene, m-Xylene, p-Xylene) (Chestnut and
Mills, 2005) from aqueous solution. However, it illustrated that hex-
adecyltrimethyl ammonium bromide (CTAB) surfactant was the most
suitable surfactant for the modification of zeolites to remove organic
contaminants of wastewater (Chestnut and Mills, 2005). Structurally,
this surfactant has a small positive hydrophilic head and it has also a
long hydrophobic hydrocarbon (C16 ) tail, which can help to adsorb or-
ganic molecules in aqueous solution (Salim and Malek, 2016). Recently,
modified zeolite Y was synthesized from bentonite by CTAB surfactant,
and tested for the removal of organic contaminants from wastewater of
the olefin plant. The results indicated that it could remove 89% of or-
ganic contents from the industrial wastewater (Hosseini Hashemi et al.,
2019).
5.1.3. Removal of radioactive substances
Zeolite is one of the well-known inorganic ionic exchanger for de-
contaminating radioactive wastewater due to its unique characteristics
such as high exchange capacity, thermal and mechanical stability and
high resistance to radiation. In the process of nuclear power accidents
 A. Khaleque, M.M. Alam, M. Hoque et al.
Table 5
Adsorption of HM by synthetic zeolite (Yuna, 2016).

Metal ion Zeolite Zeolite origin Temperature (°C) Time (h) Initial concentration (mg/L) S/L ratios (g/mL) pH Adsorption capacity, q(mg/g)

Cr3+ and NaA Blend of NaX From mordenite 25 24 500 1/200 71.1
Cr3+ and NaP Blend of NaY From mordenite 25 24 500 1/200 83.2
Cr3+ NaP From mordenite 25 24 500 1/200 52
Cr3+ te Hydroxysodali From kaolin 25 24 500 1/200 34.7
Cr3+ Zeolite 4A From CFA 25 1 50–100 1/1000 3–4 38.7–56.4
Cr3+ NaP1 From CFA 22 6 100 1/100 4 43.6
Cd2+ Zeolite X From kaolin 25 0.5 20 1/125 7.5 92
Cu2+ Zeolite A From kaolin 25 0.5 20 1/125 7.5 41.6
Cu2+ Zeolite X From kaolin 25 0.5 20 1/125 7.5 44.16
Cu2+ Zeolite 4A From CFA 25 1 50–100 1/1000 3–4 39.8–72.0
Cu2+ NaP1 From CFA 22 6 100 1/100 5 50.5
Cu2+ NaX +-activated carbon From CFA 25 24 500 1/500 7 101.7
Cd2+ NaX +; activated carbon From CFA 25 24 500 1/500 129
Cd2+ Zeolite A From kaolin 25 0.5 20 1/125 7.5 71
Cd2+ NaP1 From CFA 22 1 100 1/100 6 50.8
Pb2+ NaX +-activated carbon From CFA 25 24 1000 1/500 228
Pb2+ Zeolite From kaolin 25 0.5 20 1/250 7.5 213
Pb2+ Zeolite X From kaolin 25 0.5 20 1/125 7.5 187
Zn2+ Zeolite A From kaolin 25 0.5 20 1/125 7.5 28.6
Zn2+ Zeolite X From kaolin 25 0.5 20 1/125 7.5 41
Zn2+ Zeolite 4A from CFA 25 2 50–100 1/1000 3–4 19.6–40.4
Zn2+ NaP1 From CFA 22 1 100 1/100 6 32.6
Ni2+ Zeolite A From kaolin 25 1 20 1/125 7.5 24.65
Ni2+ Zeolite X From kaolin 25 1 20 1/125 7.5 24.89
Ni2+ NaP1 From CFA 22 1 100 1/100 6 20.1
Ni2+ Zeolite 4A from CFA 25 1 50–100 1/1000 3–4 11.5–6.1
Ni2+ NaX +-; activated carbon From CFA 25 24 500 1/500 132.1
Co2+ Zeolite 4A from coal flash 25 1 50–100 1/1000 3–4 5.5–16.8
Co2+ Modified zeolite (MCP-GLU) From Iran 25 6 600 1/100 6 29.38
Co2+ (NCP) Modified zeolite From Iran 25 6 600 1/100 6 19.05
Co2+ Modified zeolite (NCP-GLU) From Iran 25 6 600 1/100 6 41.47

Environmental Advances 2 (2020) 100019

 A. Khaleque, M.M. Alam, M. Hoque et al.
Table 6
Removal of anion and cation by synthetic zeolites.

Anion/ Zeolite SiO2 /Al2 O3 SSA (m2 /g) CEC Efficiency, (%) Adsorption Operation Conditions Ref.
Cation (meq/100g) capacity, q
pH Time, (min) Temperature Initial Dosage (g/mL)
(mg/g)
(°C) concentration,
(mg/L)

Ca2+ 4A 450 82 5 30 25 (Cardoso et al., 2015)

NH4 + Na-P1 280 57–61 31–4 5 30 25 (Cardoso et al., 2015)
NH4 + Na-P1, Faujasite, 1.49 283.3 19.57 1 485 0.01 (Prasad and Mortimer, 2011)
Chabazite
Gismondine 2.62 45.511 69 4.8 8 25 7.3 0.04 (Elmolla and Chaudhuri, 2012)
NH4 + Na-P1 290 52 30 10 g/l (Cardoso et al., 2015)
Cl− Na-P1 290 48.38 3.3 30 12.4 0.01 (Cardoso et al., 2015)
F− Na-P1 290 75 3.3 30 1.2 0.01
NO− 3 Na-P1 290 52.63 3.3 30 3.8 0.01
PO4 3− Na-P1, Ancalime, 91 5.24 30 25000 0.03 (Otal et al., 2005)
Chabazite
Na-P1, Sodalite 3.57 35.38 188 57.14 24h 15000 0.01 (Pengthamkeerati et al., 2008)
SO4 2− Na-P1 290 84.97 3.3 30 406 0.01 (Cardoso et al., 2015)

Table 7
Removal organic compounds by synthetic zeolite.

Compound Zeolite Specific Surface Area Adsorption capacity, % of removal pH Time (hr) Temperature (°C) Dosage (mg/L) Ref.
(m2 /g) q (mol/g)

phenol (Ph), Fe-nano zeolite (Fe-NZ) 692 138.7, 158.9 and 10 to 300 min. 425, 327-2, 368- (Tri et al., 2020)
2-chlorophenol (2-CP) and 171.2
2-nitrophenol (2-NP)
4-Nitro-phenol Na-Y 156.876 90 % 20 min 40 (Ahmedzeki et al., 2013)
Total organic carbon surfactant modified zeolite Y 527.26 89% 10 (Hashemi et al., 2019)

Environmental Advances 2 (2020) 100019

Trichloroethylene (TCE) ZSM-5 (silicalite) 97% 0.1 (Anderson, 2000)
Alizarin sulfonate Analcime (HS) 7.4 0.713 4 0.01 (Woolard et al., 2002)
Methylene Blue A 25.98 30 50 (Wang et al., 2009)
X 35.42 30 50 (Wang et al., 2009)
Methylene Blue Na-P1 25.7 15.99 6.2 72h 30 (Wang et al., 2006)
Safranine Na-P1, Y, X, Sodalite 27.4 7.015 6.34 1d 45 10 (Atun et al.,
Thionine Na-P1, Y, X, Sodalite 27.4 9.702 6.39 1d 45 10 2011)
A. Khaleque, M.M. Alam, M. Hoque et al. Environmental Advances 2 (2020) 100019

and nuclear waste disposal, more attention has been paid to the treat-

(Sharma and Tomar, 2011)

(Mustafa and Zaiter, 2011)
ment and disposal of radionuclides. The study showed that the zeolite
and mordenite had good adsorption capacity for 137 Cs, 90 Sr, and 60 Co

(Merceille et al., 2012)

(Falyouna et al., 2020)

(Ibrahim et al., 2008)

(Huang et al., 2020)
(Munthali et al., 2015; Long et al., 2013). Recently, magnetic zeolite

(Liang et al., 2020)

(El-Kamash, 2008)
(El-Kamash, 2008)
composite (Ze/FeO) was selected as the ideal adsorbent for treating ce-
sium contaminated water in a lab-scale continuous treatment system. It
was found that cesium removal capacity was 100% and generated clean
effluents that were safely discharged to the environment without posing

Ref.
any environmental and health risks (Falyouna et al., 2020). Recently, Y
type nano zeolite NFA-Y was used for the adsorption of Cs+ from aque-
ous solution. The adsorption capacity of the NFA-Y was 167.12 mg g−1

90-120
90-120
(Huang et al., 2020). Very recently, an aluminosilicate with CHA-type

(min)
Time

24h
120
zeolite framework was synthesized and investigated for the adsorption

3h
80

60
of Sr2+ ions which removed 100% of these ions at very high concen-
tration (Liang et al., 2020). Synthetic zeolite A was an efficient ion

Temperature,
exchange material for the removal of 137 Cs and 90 Sr ions from waste
aqueous. The maximum sorption capacities (qm) were in the range of

25–55.

25-55.
27-60
2.51–2.54 and 4.90–5.51 mmol/g for Cs+ and Sr+2 ions, respectively

(°C)

25

25
25

50
(Table 8) (El-Kamash, 2008). Zeolite NaA–X was tested as a sorbent ma-
terial for the sorption of cesium ions from chloride waste solutions. The
maximum Cs ion sorption capacities of Zeolite NaA–X (qm) were in the

6.0 to 8.0
range of 2445.9–2550.9 mmol/kg (Ibrahim et al., 2008). Hence, it is

5.5 to 6
clear about the significance of synthetic zeolite in this field. However,

3-11

8–9
6.0

6.0
6.0
pH
some future studies should have been carried out regarding the applica-

5
tions such as adsorption mechanisms, surface modification of synthetic
zeolites, safe handling of the adsorption process.

77,730 Bq L−1
concentration,
5.2. Synthetic zeolite for gas adsorption

50-100

50-100
50-100
(mg/L)
Initial

0.001
Zeolites have tunable channels with a very rigid framework. This

5
imparts zeolites with excellent shape selectivity and capabilities to-
wards gas molecules (Ennaert et al., 2016). Natural and synthetic ze-
olites are found potential for removing SOx, NOx, COx, H2 S, and stor-
% of adsorption

ing H2 gas. Recently, several numbers of reports have published on the

adsorptive removal of CO2 using synthetic zeolites (Table 9). Zeolites
100 %

and metal−organic frameworks are one of the most widely applicable

classes of solid-porous adsorbents for CO2 capture (Guo et al., 2015; 100%

Yaghi et al., 2003; Khandaker et al., 2020). However, narrow pore open-
ings limit CO2 capture dynamics. Hierarchically porous zeolites have
been attracted great consideration since they have exhibit additional
3400 Bq L−1
Adsorption

porosity on the larger length scales (mesopores and/or macropores) re-

capacity, q

0.408 and
sulting in shorter pathways to the zeolitic microspores. This can be sig-
167.12
(mg/g)

0.337
0.455
0.339

0.455
140

nificantly improved the CO2 diffusion and consequently faster adsorp-

Overview of the removal of radioactive substance-using synthetic zeolites.

tion kinetics (Schwieger et al., 2016; Khan et al., 2019). To enhance

CO2 separation selectivity and adsorption capacity for carbon capture
and sequestration applications, recently a core-shell Zn/Co zeolitic imi-
Specific surface

dazolate framework (ZIF) was synthesized which showed the maximum

area(m2 /g)

7.82 × 104

CO2 uptake (3.22 mmol/g at 273 K and 1 bar). This was 2.13 times
593.64

cm2 /g
508.2

446.6

higher than that of the raw core-shell Zn/Co ZIF. Nowadays, nitrogen-
470

doped carbons derived from core-shell Zn/Co ZIF was found the promis-
ing materials for solid CO2 separation from industrial power plant flue
gas (Cheng et al., 2020).
Y type nano zeolite

(MOR) type zeolite

composite (Ze/Fe0 )

The modification of zeolite substrates with catalytic nanoparticles

CHA-type zeolite
Magnetic zeolite

is a suitable method for the removal of similar pollutants such as hy-

framework

drogen sulfide. In a study, the effect of adding magnetite nanoparti-

Zeolite A
Zeolite A

Zeolite A
(NFA-Y)

cles to zeolite ZSM-5 and Y substrates was investigated. Hydrogen sul-

NaA–X
Zeolite

Na-A

fide removal at high temperatures by the two substrates was compared

(Jafari et al., 2020). Some of the volatile organic compounds have also
been captured by different zeolites (Maiti et al., 2018; Karthikeya and
Saravanan, 2013). Some recent studies suggest that understanding the
Th(IV) and Eu(III)

flexibility of other zeolites and metal organic frameworks will lead

to applications in selective separation and storage of small molecules
Radioactive

(Kumar et al., 2020; Bezverkhyy et al., 2020). Still, the performance

substance
Table 8

of these materials is quite limited because of their small pore size and
Cs

Cs

Cs

Cs
90Sr

Co
Sr

Sr
137

137

137

137

restricted surface area. However, this could be improved by physico-

90

90
60

chemical modification of zeolite. There are still lots of challenges on

A. Khaleque, M.M. Alam, M. Hoque et al. Environmental Advances 2 (2020) 100019

Table 9
Overview of gas adsorption using synthetic zeolites.

Temperature Sorption
Adsorbate Adsorbent BET(m2 /g) (°C) Pressure Capacity Ref.

CO2 Zeolite Ti-Beta 758 25 1bar 5 mmol/g (Mazaj et al., 2020)

nanocrsytal-
lites
CO2 ZeY@CS 795 25 36.712 ccg−1 (Kumar et al., 2020)
composite
CO2 ZSM-5@CS 444 25 53.610 ccg−1 (Kumar et al., 2020)
composite
CO2 Zn/Co zeolitic 356 0 1 bar 3.22 mmol/g (Cheng et al., 2020)
imidazolate
framework
(ZIF)
CO2 Modified 179.44 0 30 bar 5.2 mmol/g (Wahono et al., 2020)
Indonesian
calcite-rich
mordenite-
clinoptilolite
zeolites
CO2 Na-X 112 3 bar 0.778 mol (Ferella et al., 2020)
CO2 /kg
CO2 ZIF-67 1478 27, 0/ 25 50bar 51.4 (49.2)wt% (Ethiraj et al., 2020)
CO2 zeolite-like 1 atm (27.6/19.4 wt % (Lin et al., 2012)
metal azolate
framework
MAF-66
CO2 Zeolite A 25 145mg/g (Soe et al., 2016)
CO2 Zeolite X 800 25 220 mg/g (Soe et al., 2016)
CO2 Zeolite X 643 25 225 mg/g (Zhang et al., 2017)
D2 /H2 CHA zeolites 40K 530–650 hPa 12 mmol/g (Bezverkhyy et al., 2020)
SO2 Pearlite 102.4 Room 46 mg/g (Pedrolo et al., 2017)
temperature
SO2 Zeolite X, 25 1.68mmolg−1 (Czuma et al., 2016)
Zeolite A
N2 O Na-P1 64.77% (Maiti et al., 2018)
NOx Zeolite X-Ag 292 65% (Karthikeya and
Saravanan, 2013)
VOCs (Benzene, Na-P1, quartz, 94.49 45 1.44 𝜇g g−1 ,
Toluene, mullite 10.52 𝜇g g−1 ,
o-Xylene, 26.22 𝜇g g−1 ,
m-Xylene, 25.96 𝜇g g−1 ,
p-Xylene 20.50 𝜇g g−1
H2 ZeY@CS 795 1bar 113.61 ccg−1 (Kumar et al., 2020)
composite
−1
H2 ZSM-5@CS 444 1bar 110.75 ccg (Kumar et al., 2020)
composite
H2 S ZSM-5 and Y 365.40,550.08 300°C Weight 3% and (Jafari et al., 2020)
5%-Y/Fe3 O4
CH4 Zeolite 4A 25.131 45 12 mmol/g (Wang et al., 2020)

the applications of natural zeolites due to their limitation of synthesis,
small pore size, no uniform crystallinity, presence of foreign materials.
Comparatively synthetic zeolites and their frameworks have vastly ex-
perimented for gas adsorption.
6. Future recommendations
Different forms of synthetic zeolites facilitate their applications into
various fields. However, challenges associated with the synthesis and
application of zeolite to need to overcome in future.
• Need to find out alternative synthetic routes to synthesize high sur-
face area, controllable molecular dimensions and high adsorption ca-
pacity of zeolite materials from different raw materials. Especially,
more study requires to find out inexpensive raw materials for the
zeolite synthesis.
• Need to study more about on how the nucleation growth during syn-
thesis process of zeolite with the relevant kinetics study and energy
calculation.
• Need to develop easy synthetic routes in order to reduce the cost of
production.
• Synthetic zeolites need to apply for many new applications including
electronic wearable materials development.
Need to study on the performance of the regeneration of the synthetic
zeolite for environmental applications.
7. Conclusion
Different aspects of the effective synthesis of synthetic zeolites from
various raw materials have been critically reviewed. Besides this, the
potential advantages and disadvantages of the different synthetic routes
and different raw materials have been summarized. It was found that
zeolites have versatile applications, although our discussion was lim-
ited in environmental applications only. This review results show that
the readily available, cheap raw materials have been proven to pro-
duce good quality zeolites compared to the use of relatively expensive
raw materials. These raw materials can maintain a uniform structure
together with lowering the ageing time as well as the cost. However,
different methods have some limitations which need to control properly
in future. Furthermore, environmental applications of synthetic zeolites
have great potential as they have a wide range of applications. Still now,
A. Khaleque, M.M. Alam, M. Hoque et al.
there are a few observations which need to address in the future for the
full application of synthetic zeolites in a commercial scale.
Declaration of Competing Interest
The authors declare no conflict of interest.
Authors contribution
First four authors are equally contributed to collect data, write the
draft and revise the manuscript. Authors J.B.H., B.X., A.K.K., J.L.Z.,
M.A.H.J., have designed the manuscript, edit and write the manuscript.
M.B.A., has supervised, planed, monitored, revised, and re-written the
manuscript.
Funding
This research received no external funding.
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