Colloid and Interface Science Communications 30 (2019) 100181

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Colloid and Interface Science Communications

journal homepage: www.elsevier.com/locate/colcom

Recent advancements in silica nanoparticles based technologies for removal T

of dyes from water
Sushilkumar A. Jadhava, , Harshada B. Garudb, Aravind H. Patila,c, Gajanan D. Patila,
⁎

Chetan R. Patila, Tukaram D. Dongalea, Pramod S. Patila,c

a
School of Nanoscience and Technology, Shivaji University, Kolhapur, Vidyanagar, 416004 Kolhapur, Maharashtra, India
b
Department of Chemistry, Balasaheb Desai College, Patan, affiliated to Shivaji University, Kolhapur, Vidyanagar, 416004 Kolhapur, Maharashtra, India
c
Department of Physics, Shivaji University, Kolhapur, Vidyanagar, 416004 Kolhapur, Maharashtra, India

ARTICLE INFO ABSTRACT

Keywords: Silica and silica based hybrid nanoparticles are investigated with great interest for the removal of dyes from
Silica nanoparticles water. The presence of surface silanols which can complex the dyes, ease of grafting of additional functionalities
Surface modification to improve the complexation, the possibility of photocatalyst grafting for dye degradation and good chemical
Hybrid silica nanoparticles stability are the reasons for the excellent efficiency of silica nanoparticles to remove dyes from water. In this
Dye adsorption
overview the main strategies used for the removal of dyes from water by using silica nanoparticles are discussed.
Water purification
The use of bare, core-shell and polymer-grafted silica nanoparticles for removal of dyes is explained with ex-
amples. Additionally, very latest reports about the synthesis and use of silica and hybrid silica nanoparticles for
removal of dyes from water are discussed and critically analyzed. The future challenges in the development and
use of silica nanoparticle based technologies for removal of dyes are pointed out with explanation.

1. Introduction functional groups on the material either present naturally or grafted

The traditional water treatment and purification methods such as
mechanical separation, filtration, flocculation, coagulation and che-
mical treatment or disinfection etc. are practiced since a long time.
Although some of them still retain their importance, there is need to
invent and test new water treatment technologies which can be more
efficient and fast than the conventional methods. Recently, the use of
nanotechnology for water remediation has received increased attention
due to the invention of new functional nanomaterials with high effi-
ciencies to entrap various pollutants from water [1–4]. A wide variety
of nanomaterials are reported in the literature for the removal of
harmful pollutants from water [5–8]. Nanomaterials are materials with
size in the range of 1 to 100 nm and they can be synthesized by top
down or bottom up approaches [9,10]. Due to extremely small size of
nanomaterials, their surface area is very high and that increases the
contact of polluted water and the nanomaterial contact [11]. This in-
creased contact increases the adsorption efficiency of the nanomaterial
towards various pollutants. The nanomaterials used for adsorption of
various pollutants from water are also called as nanoadsorbents
[12–15]. The adsorption of the pollutants on the nanoadsorbents results
due to some specific interactions between the pollutants and the
purposely to increase the adsorbent-pollutant interactions [16]. One of
the most commonly used nanoadsorbent for water purification include
silica and hybrid silica based nanomaterials due to their chemical sta-
bility, low cost and relatively easy surface modification [17–21].
A wide range of pollutants such as toxic heavy metals, organic
pollutants like dyes, pesticides and pharmaceuticals, degraded organic
matter etc. are found in polluted water [22–24]. Among these pollu-
tants, dyes are those pollutants which are not only toxic but they
change the color of the water [25,26]. This reduces or completely block
sunlight penetration into the stream and therefore can reduce the
photosynthetic reaction and affect the aquatic biota. This means dyes as
pollutants are harmful for human being, aquatic animals and to plants
too. Dyes are released in water mainly from textile, leather and from
synthetic color production industries [27]. Synthetic dyes are toxic and
carcinogenic hence their presence in water even in low concentrations
can cause serious health problems. Although, various materials such as
magnetic nanoparticles, metallic or metal oxide nanoparticles, compo-
site nanoparticles etc. are reported for the removal of dyes from water,
silica and silica based nanomaterials retain their importance for several
reasons [28,29]. Since last two decades, a huge number of reports in the
literature about invention of various new efficient and cost effective

⁎
Corresponding author.
E-mail address: sushil.unige@gmail.com (S.A. Jadhav).

https://doi.org/10.1016/j.colcom.2019.100181
Received 17 February 2019; Received in revised form 3 April 2019; Accepted 7 April 2019
Available online 12 April 2019
2215-0382/ © 2019 Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/BY-NC-ND/4.0/).
S.A. Jadhav, et al.
synthetic methods for silica nanoparticles and hybrid silica nano-
particles were observed [30–35]. These methods include sol-gel, hy-
drothermal, reverse microemulsion and flame synthesis of silica nano-
particles [36,37]. These methods are also adapted or suitably modified
to produce solid as well as porous and functionalized silica nano-
particles [38]. This development has provided the availability of a wide
range of different silica nanoparticles with various size, shapes and
morphologies as nanoadsorbents for pollutants. Silica is also abundant
in nature (such as in the form of sand) and it can be transformed in to
silica nanoparticles by top-down method to prepare nanomaterials
[39]. This approach in fact brings down considerably the cost asso-
ciated with synthesis of silica nanoparticles. Although, a huge number
of reports are there in the literature about use of silica or porous silica
nanoparticles for removal of dyes, most of the works are restricted to or
limited to their use in labs and none is reached in the real world ap-
plication [40]. Hence there is a need to convert laboratory scale
achievements in to scalable, low cost and highly efficient technology. In
this review, some basic points about the use of silica nanoparticles
specifically for removal dyes from water are revised. The explanation is
followed by the list of some latest reports (last 2 years only) with key
findings and critical analysis about synthesis and use of silica or hybrid
silica nanoparticles for removal of dyes from various categories. The
very recent literature is reviewed to present the readers with current
state of the art about use of silica nanoparticles for removal of dyes
from water.
2. Dyes as pollutants
‘Dye’ is a colored substance which can be natural, semi-synthetic or
totally synthetic that has an affinity to the substrate to which it is being
applied. The natural dyes because of their natural origin can be non-
toxic compared to the synthetic dyes. The main sources of synthetic
dyes pollution are textile, paper, rubber, plastics, paints, printing, and
leather industries [41]. They release various dyes containing effluents
in water. The main reason is the incomplete adhesion of the dyes to the
substrates during their coloring. The amount of unfixed dyes is more in
textile effluents compared to the effluents released by other industries
[42]. The list of most common dyes used in various industries in par-
ticular in textile industries together with their structures are shown in
Table 1. Among all dyes, the “azo” dyes are most commonly used for
coloring various substrates. They are complex in nature and are po-
tential carcinogenic substances. Due to their bigger molecular struc-
tures their degradation products are also toxic. The reductive cleavage
of azo linkages is responsible for the formation of amines, which are
classified as toxic and carcinogenic materials [43]. If azo dyes get ad-
sorbed in the soil from water, they can alter the physical and chemical
properties of the soil. This may lead to the destruction of flora in the
environment. If the toxic chemical dyes remain in the soil for a long
period they also kill useful soil microorganisms and this greatly affects
the agricultural productivity [44,45]. Due to intense coloring proper-
ties, azo dyes even in extremely low concentrations in water bodies are
visible. This reduces the light penetration through water and leads to
the decreased photosynthetic activity. This causes oxygen deficiency
and disturbs the biological cycle of aquatic biota. In addition, azo dyes
are also highly poisonous to the ecosystem and mutagens depending
upon their concentrations in the polluted water. Due to the known
toxicity of synthetic dyes the Government legislation regarding allowed
dye concentration in effluent are very strict in almost all countries
[46,47]. According to some revised polices it is expected that zero
synthetic chemicals should be released in the effluents. As we cannot
imagine a world around us without colors or colored articles such as
clothes and objects, the manufacturers will continue to use the dyes. So
new technologies must be developed to entrap almost all dye that es-
cape from the dying process and become a part of the effluent coming
out from such industries. The color concentrations limits and quantum
of water generated from industries are defined by legislation in India
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Colloid and Interface Science Communications 30 (2019) 100181
and U.S.A by USPHS: United States Public Health Services and BIS:
Bureau of Indian Standards. For textile industries the color limits for
effluents from textile industries in Hazen units are 0 to 25 in U.S.A. and
0 to 20 in India per 120 m3/Ton of fiber produced. For paper and pulp
industry the limits are 0 to 10 and 5 to 101 per 175 m3/Ton of paper
produced in U.S.A. and India respectively. Instead the limits for a
tannery the limits are 10 to 50 and 25 Hazen units per 28 m3/Ton of
raw hide [47]. Recently, the use of silica and hybrid silica nanoma-
terials as nanoadsorbents for dyes is being given considerable attention
hence a large number of reports were observed in the literature about
use of silica nanoparticles for removal of various dyes.
3. Types of silica nanoparticles for removal of dyes
3.1. Bare nanoparticles
One of the main features of silica nanoparticles (chemically silicon
dioxide SiO2) is the presence of surface hydroxyl groups. The hydroxyl
groups present on the surface of silica are termed as “silanols” as they
are attached to the silicon atom [48]. These silanols impart function-
ality to the particles as hydroxyl groups can selectively complex certain
compounds or metal ions. The interactions of various molecules with
silanols can be enhanced by varying the pH value. Further they can be
also pH sensitive. Hence bare nanoparticles of silica are also tested
directly for the removal of dyes. Recently, Rovani et al. reported the use
of bare silica particles for the removal of acid orange 8 dye from water
[49]. The silica nanoparticles used in the study were prepared from
sugarcane white ash and they were able to remove almost 100% of the
dye from the aqueous solution. The strategy of synthesis of silica na-
noparticles and percentage dye removal curves are shown in Fig. 1.
Bare porous silica nanoparticles are also tested for the removal of dyes
from water [34,50]. The mesoporous silica nanoparticles are a unique
class of porous materials with high specific surface area, large and
tunable pore volume and size between 2 and 50 nm [51]. Mesoporous
silica nanoparticles can be synthesized by various techniques [52–55].
The most common mesoporous silica nanoparticles used for removal of
dyes are MCM-41 or SBA-15 type. Recently Chen et al. have reported an
interesting method for synthesis of variously shaped porous silica na-
noparticles for dye removal application [20]. The variations in the
shapes of the nanoparticles were obtained by slight modifications of the
synthetic conditions by sol-gel process. Of the various shapes, the
spherical particles were found to possess maximum adsorption capacity
of 234.6 mg/g for rhodamine B dye. The SEM images of all the particles
prepared are shown in Fig. 2 where all the different shapes are visible.
A huge number of reports are there in literature about synthesis of
porous silica nanoparticles by various methods [56,57]. Small amphi-
philic molecules such as cetyltrimethylammonium bromide or amphi-
philic di or triblock copolymers such as Pluronics® are used as templates
to generate the porosity in silica particles [58,59]. Recently, the use of
natural materials and various other new generation materials as tem-
plates or as source of templates for porous silica synthesis has received
increased attention [60,61]. This approach substantially reduces the
cost of the synthesis of porous silica nanoparticles. Some naturally
available materials can substitute the costly chemical templates. In-
terestingly, the natural templates can give the same amount of porosity
that can be obtained with synthetic chemical templates. As an ad-
vancement in this approach, Cui et al. recently reported synthesis of
biomorphic mesoporous SiO2 with unique two-dimensional (2D) na-
nostructure fabricated by employing renewable petal cells as bioscaf-
folds [62]. The whole process is shown in Fig. 3. According to the report
the biomimetic 2D porous SiO2 showed significant adsorption capacity
for the methylene blue dye (74 mg/g), which is higher than those by
nonporous SiO2 (14 mg/g) and the traditionally hydrothermally syn-
thesized mesoporous SBA-15 (45 mg/g) type silica [62].
However, bare silica nanoparticles (both solid and porous) show
some limitations as nanoadsorbents for removal of pollutants including
S.A. Jadhav, et al. Colloid and Interface Science Communications 30 (2019) 100181

Table 1
Structures of common dyes used by industries and used in the labs for checking the efficiency of nanomaterials.
Azo dyes Congo red

Direct blue

Acidic red 337

Methyl orange

Nitro dyes Disperse yellow 14

Indigo dyes Vat blue 35

Anthraquinone dyes Reactive blue

Cationic dyes Rhodamine blue

Methylene blue

Triphenyl methyl dyes Basic violet

Malchite green

dyes. Due to high surface energy and particle-particle interactions bare
silica nanoparticles show low colloidal stability and tend to aggregate
very fast and sediment during the use [63]. This aggregation reduces
the surface area available for adsorption of pollutants and leads to the
decreased adsorption capacity of the nanoparticles. The fast aggrega-
tion also reduces the contact time between pollutant and the silica
surface which affects their adsorption capacity. The use of porous silica
particles instead of solid silica particles is preferred as even aggregated
porous silica nanoparticles retain their porosity and high total surface
area. Another problem with the use of bare silica nanoparticles for re-
moval of dyes is that when silica surface comes in direct contact with
the dye solution depending upon the acidic or basic nature of the dye it

3
S.A. Jadhav, et al.
Fig. 1. Effect of time on removal of acid orange 8 by silica nanoparticle ad-
sorbent. Conditions: 25 °C; initial concentration: 150 and 200 mg/L; adsorbent
mass: 1.0 g/L. (Figures reproduced with permission from ref. 49. Copyright ACS
publications 2018).
may lead to slow etching of the particles. Although, silica particles are
supposed to be chemically stable, slight modifications in the surface are
possible upon exposure to certain drastic environments. This can be
monitored by checking the diameter and monitoring the shape and
morphology of the particles after each reuse cycle.
3.2. Functionalized and core-shell nanoparticles
As pointed out before the pollutant-nanoadsorbent surface interac-
tions are important and they greatly influence the efficiency of the
material to remove pollutants from water. These interactions through
complexations can be further enhanced by functionalization of the
surface of the nanoparticles. As the surface of silica nanoparticles is
reactive due the presence of silanol groups, the reactivity can be used to
graft various organic functionalities on their surface by alkoxysilane
grafting chemistry [64–67]. The surface modification or grafting is a
relatively easy process. There are number of reports in the literature
about the use of functional alkoxysilane grafting on silica nanoparticles
to impart desired functionality to them [68,69]. Due to the invention
and commercialization of various new functional alkoxysilanes bearing
variety of functional groups, the process of grafting of desired func-
tionality on nanoparticles has become easy. The functionalization of
nanoparticles increases adsorption capacity of the bare silica nano-
particles [70–72]. The grafting of functional organic groups or poly-
mers on bare nanoparticles transfers them in to core-shell nanoparticles
and the shell improves the colloidal stability of the particles. The
grafted functionalities help to increase the dye molecule-nanomaterial
surface interactions, such interactions must be reversible and can be
controlled by changing conditions such as pH or temperature etc. The
4
Colloid and Interface Science Communications 30 (2019) 100181
reversible nature of the interactions is necessary because it increases
the recyclability of the nanoadsorbents. Although, the adsorption of
maximum quantity of dye or any other pollutant on the nanomaterial is
the initial priority, easy desorption of the dyes is also desirable for re-
peated use of the nanoadsorbate. Desorption of the dyes from the na-
noadsrobates to regenerate the adsorption sites increases the reusability
of the materials (cycles) and this ultimately reduces the cost of the
technology. The three main strategies adapted for the use of silica na-
noparticles for the removal of dyes from water are summarized in
Fig. 4. The main challenge is to get desorption of dyes from the surface
of the particles to generate the adsorption sites. This is a very difficult
task as the dye-silica nanoparticle (silicon dioxide) surface interactions
are very strong.
Coating silica nanoparticles with photocatalytic materials or im-
mobilization of the photocatalyst on their surface are two important
strategies that are used for adsorption followed by photocatalytic de-
gradation of dyes (refer to Fig. 4). There are many reports in the lit-
erature which use this strategy [73,74]. However, there are no con-
clusive reports about the analysis of the degradation product/s of the
dyes. The photocatalytic degradation process of the dye should be
monitored and the degradation products must be analyzed to check
their toxicity. Otherwise, it is just like conversion of one colored (dye)
toxic organic pollutants in to other toxic compounds. Hence there is a
need to monitor, isolate and analyze the dye degradation products. A
predicted or hypothesized dye degradation mechanism supported with
analytical or characterization data has been never presented.
3.3. Polymer grafted nanoparticles
Polymer-grafted silica nanoparticles have been also reported for the
removal of various pollutants from water including dyes [75,76]. Pre-
sence of functional groups on the back bone or on the branches of the
polymer chains grafted on the surface of nanoparticles increases the
complexation ability of the particles towards pollutants. Further, the
polymer shell around the nanoparticles protects direct exposure of the
silica surface to the acidic or basic dye solution in water. The polymer
grafting increases the colloidal stability of the particles and helps to
increase the contact time of the particles with the contaminated water.
One of the ways to achieve easy desorption of the dyes from the surface
of silica nanoparticle is to prepare nanomaterials (silica nanoparticles)
with switchable surface properties. This can be achieved by grafting
smart polymers on the nanoparticles. Recently, Jadhav et al. reported
the synthesis and testing of silica nanoparticles grafted with thermo-
responsive polymers bearing switchable surface properties [77]. The
surface of the silica nanoparticles can be transferred from hydrophilic at
room temperature to hydrophobic upon slight warming by virtue of the
thermoresponsive polymer, poly(N-siopropylacrylamide) grafted on the
surface of the particles. This helps in easy desorption of molecules ad-
sorbed on the particles. Such approaches need to be further developed
to assist desorption of pollutants from nanoadsorbates made from var-
ious materials. Due to increase in the density of functional groups
around the particles (present on polymer chains) it is also possible to
immobilize photocatalysts either in ionic or nanoparticle form on the
polymer grafted nanoparticles. The functional group baring polymer
chains can hold the immobilized catalyst near the surface of silica na-
noparticles. The adsorption of dye followed by its catalytic degradation
can be achieved by photocatalyst immobilized particles. Grafting of
molecularly imprinted polymers (MIP) on silica nanoparticles with
imprints of the pollutants or the dye molecule is also reported. In this
approach an imprint of the dye in the compact cross-linked polymer
shell is made which helps in selective removal or recognition of the dye
from water [78]. MIP-grafted particles can also be used to capture or
selectively separate a specific dye from combination of dyes or other
pollutants.
S.A. Jadhav, et al. Colloid and Interface Science Communications 30 (2019) 100181

Fig. 2. SEM images and size distributions of SiO2 nanoparticles (N1 − N5) obtained with different amount of NH3·H2O (a) 0.1 mL, (b) 0.2 mL, (c) 0.3 mL, (d) 0.4 mL,
(e) 0.5 mL. (Reproduced with permission from ref. 20 Copyright ACS publications 2018).

4. Recent updates about use of silica nanoparticles for removal of
dyes
The search for ideal, low cost and reusable nanomaterials as new
generation nanoadsorbents for various pollutants continues. There are
several reports in the literature about synthesis, characterization and
testing of new silica based nanomaterials for removal of dyes from
water. Recently, some significant improvements are noticed in this field
of research. The summary of the recent works reporting the improve-
ments is presented in detail in Table 2. Some important features and
drawbacks of the latest reports are summarized in Table 2 are as fol-
lows. It is worth to point out that the new generation silica based na-
nomaterials have shown excellent dye adsorption capacity and the va-
lues have reached from 70 to 230 mg per gram of the nanoadsorbent for
various dyes. This can be considered as a great achievement. Ad-
ditionally many new methods of synthesis of bare, functionalized, hy-
brid and core-shell silica nanoparticles have been reported. Some re-
ports even claim the successful synthesis and testing of fancy materials
made of combinations of iron oxide, noble metals and silica, Fe3O4@
SiO2@TiO2, magnetic materials coated with silica and various polymers

5
S.A. Jadhav, et al. Colloid and Interface Science Communications 30 (2019) 100181

Fig. 3. Illustration of the fabrication process for biomorphic porous silica nanostructures using camellia petal cells as bio-scaffolds (Reproduced with permission from
ref. 62. Copyright ACS publications 2018).

Fig. 4. Three main strategies used to develop silica or hybrid silica nanoparticle based technologies for removal of dyes from water.

such as Cobalt Ferrite@SiO2@ polyethyleneimine etc. Although, all
these are remarkable achievements, the large scale synthesis of the
reported nanomaterials with high efficiencies remains a matter of de-
bate. Another main issue is most of the materials developed recently
that appear in Table 2 were tested separately for the removal of a
specific dye. There is hardly any report which proves the selective ad-
sorption of a particular dye from the combination of dyes (or pollu-
tants). This is of great interest where a certain industry is interested in
selective capture of a specific dye and reuse it after easy desorption
from the nanoadsorbent. It is also important to point out that the ma-
terials reported were synthesized on laboratory scale and tested on
small scale model pollutant solutions prepared by dissolving target
pollutants in water. Besides the large scale synthesis of the nanoma-
terials, the main challenge is also the treatment of huge amount of ef-
fluents coming out of industries or municipal sewages with these newly
synthesized nanomaterials. If the polluted water is to be kept in contact
with the nanomaterials for adsorption of the pollutants, it will need the
development of suitable containers/reactors/beds/columns where the

6
S.A. Jadhav, et al.
Table 2
Latest reports about use of silica and hybrid silica nanoparticles for removal of dyes.
Material
Methyl functionalized silica nanoparticles (MfSNPs);
PVDF/PTFE nanocomposites
SiO2/Ag core-shell nanoparticles
Fe2O3/Au/SiO2 nanorods
SiO2@void@Ag/TiO2 yolk-porous shell nanospheres
Amino groups-grafted silica nanoparticles (porous)
Silica nanoparticles (porous)
Gallium oxide@ silica /polyvinyl pyrrolidone hybrid
(SNF) nanofluids
Fe3O4@SiO2@TiO2 and Ag/Fe3O4@SiO2@TiO2
Nanocomposites
Cobalt Ferrite@SiO2@ polyethyleneimine magnetic
nanoparticles, (Co-Fe2O4@PEI)
Fe/SiO2, Zn4Fe2/SiO2 nanoparticles
Fe3O4@silica nanoparticles functionalized with amino
groups
Fe3O4@SiO2@chitosan
Boron doped-TiO2-SiO2 cobalt ferrite nanocomposite
SiO2 nanoparticles
Fe3O4@SiO2-CR nanoparticles
Colloid and Interface Science Communications 30 (2019) 100181
Dye Note with observation Ref.
Congo red In this work, membranes from the hybrid material MfSNPs/PVDF/ [79]
PTFE were prepared and found to be highly efficient in removing
Congo red dye from water with 99% removal efficiency.
Rhodamine B This work involves sonocatalytic degradation of Rhodamine B dye on [80]
the surface of the core-shell nanoparticles prepared. Influence factors
such as pH, O2 saturation of solution and the concentration of H2O2
added were studied and the conditions at which the catalyst show
maximum efficiency were found.
Methyl orange This work reports a novel heterogeneous Fenton-like catalyst, hollow- [81]
structured Fe2O3/Au/SiO2 nanorods was synthesized and tested for
the degradation of methyl orange under visible light irradiation. It was
found to degrade the dye with 100% removal efficiency within very
short time of 20 min.
Methylene blue Yolk-porous shell nanospheres showed 99.5% of dye removal [82]
efficiency in 3 h with visible light irradiation, higher than pristine
TiO2 and Ag/TiO2 nanoparticles, due to the synergy effect of robust
adsorption capacity and photocatalysis effect.
Direct blue This report is the first example of very fast removal and recycle of high [83]
amounts of DB with adsorbent materials. Very high adsorption and
desorption capacities up to 300 mg/g for each adsorption cycle was
achieved.
Methylene blue In this work, a low cost mesoporous silica nanomaterial that can be [84]
used for 5 times for effective removal of methylene blue was
developed. The maximum adsorption amount of MB onto mesoporous
silica achieved was 347.2 mg/ g.
Malecite green In this work, nanofluids based on Gallium oxide@ silica /polyvinyl [85]
pyrrolidone were prepared and tested for their photocatalytic activity
to degrade MG dye. The conditions at which the nanofluids show
maximum efficiency were optimized.
Methyl orange The photocatalytic degradation capacity of the newly synthesized [86]
nanocomposite material Fe3O4@SiO2@TiO2 to degrade MO dye was
found to be 74%. This was further enhanced by loading silver
nanoparticles on the surface of the nanocomposites through the photo
deposition method. The efficiency of degradation of the deposited
material under visible and UV irradiation was improved to 84% and
98%, respectively.
Tetrazine In this work, a facile synthesis route for the synthesis of magnetic [87]
nanoparticles (Co-Fe2O4@PEI) was developed. This new sorbent was
used in the service of ultrasound assisted dispersive micro-solid phase
extraction (UA-DMSPME) for influential clean-up, pre-concentration,
and determination of tartrazine (TA). Excellent recoveries up to 99.5%
of TA in samples including saffron spray, cotton candy and water
samples were achieved.
Methyl orange This work reports, Hybrid material, iron catalyst supported silica [88]
nanoparticles synthesis and testing for dye degradation. The catalysts
were able to degrade methyl orange efficiently in 180 min. Fe/SiO2
furnished the higher reaction rates, followed by Zn4Fe2/SiO2, which
presented the higher iron content as well as the smallest nanoparticles.
Sudan dyes In this work, amine group functionalized magnetic silica [89]
nanocomposite as a solid-phase extraction adsorbent were prepared.
The results showed excellent efficiency of target analyates (Sudan
dyes) in the range of 90–102%.
Malchite green This work reports synthesis and testing of magnetic adsorbent with [90]
chitosan-modified Fe3O4@SiO2 nanoparticles for the removal of
malachite green in aqueous solution. The Fe3O4@SiO2@chitosan
sample showed higher efficiency on the adsorption of malachite green
compared with Fe3O4@SiO2 and Fe3O4@SiO2-NH2. The removal
efficiency of malachite green was 92% by Fe3O4@SiO2@chitosan,
while that of Fe3O4@SiO2 and Fe3O4@SiO2-NH2 were 60% and 85%,
respectively.
Natural dyes, diazinon, paraquat A new magnetic photocatalyst, boron doped-TiO2-SiO2 cobalt ferrite [91]
dichloride and biologically treated was synthesized. After being reused for three times, the reduction of
POME COD removal efficiency of the natural dyes, diazinon, and paraquat
dichloride and biologically treated POME was found to be 1, 1, 3 and
4%, respectively that confirmed the photocatalytic stability of the
nanocomposite.
Methylene blue The efficiency of the nanosized semiconductors SiO2 as photocatalyst [92]
was tested to remove and degrade MO dye using an ultraviolet light
source. Different parameters affecting the process have been studied.
Complete degradation was achieved in 90 s, using 10 g/L SiO2
nanoparticles. A possible molecular mechanism for photocatalytic
degradation of MB by SiO2 nanoparticles is discussed.
Methylene blue In this work, core-shell congo red composite nanoparticles (Fe3O4@ [93]
SiO2-CR) were synthesized and completely characterized. The
(continued on next page)
7
S.A. Jadhav, et al.
Table 2 (continued)
Material
Fe3O4@SiO2-COOH NPs
Polymer-functionalized Fe3O4@SiO2-MPSg- AA-AMPS
(FSMAA) nanoparticles
Mesoporous silica supported TiO2 and mesoporous silica
supported ZnO and ZnO- and TiO2-silica composites
Nanofibrous sandwich structured adsorbent of silica
nanofiber/magnetite nanoparticles/porous silica
(SNF/MNP/PS)
γ-Fe2O3/silica (SiO2)/titania (TiO2)
Magnetic nanocomposites (NP-SiO2).
Magnetic amino functionalized nanoparticles Fe3O4@
SiO2-NH2
Chitosan/PVA/SiO2 nanocomposite
Spherical and rod shaped porous silica nanoparticles
Titania-coated silica nanostructures on polymers
TiO2-SiO2 mixed oxides
Gold/carbon co-doped TiO2 photocatalysts immobilized
on fused silica
Silica colloid with immobilized iron oxide nanoparticles
β-cyclodextrin coated silica nanoparticles SiO2@β-CD
Colloid and Interface Science Communications 30 (2019) 100181
Dye Note with observation Ref.
parameters at which the adsorbent shows maximum efficiency were
optimized. The methylene blue composite material interactions were
studied and a hypothetical mechanism is proposed.
Malachite green This work reports carboxylic group functionalized magnetic silica iron [94]
oxide nanoparticles (Fe3O4@SiO2-COOH NPs) were synthesized. The
particles then applied as a nano-adsorbent for removal of malachite
green (MG). It was found that 97.5% of MG could be removed from
aqueous solutions using an adsorbent amount of 0.5 g/L at pH = 9 in
120 min.
Methylene blue This work reports synthesis of poly acrylic acid (PAA) and Poly 2-acryl [95]
amido-2-methyl-1-propanesulfonic acid (PAMPS)-grafted Fe3O4@SiO2
(FSMAA) nanoparticles. The maximum adsorption capacity of FSMAA
for methylene blue was found to be 421.9 mg/g.
Reactive Blue 19 Mesoporous silica supported TiO2 and ZnO photocatalysts were [96]
prepared, tested and comparatively analyzed. The reactive blue
adsorption on silica supported ZnO nanoparticles was found to be
higher than on silica supported TiO2 nanoparticles. The highest dye
adsorption (50%) and the fastest dye degradation (kapp = 0.0544
/min at 25 °C) was observed on disordered ZnO/silica with Zn:Si
molar ratio 1:1.
Methylene blue In this study, a novel nanofibrous sandwich structured adsorbent of [97]
silica nanofiber coated with magnetite nanoparticles and porous silica
(SNF/MNP/PS) was synthesized. The adsorbent showed good
adsorption capacity for both methylene blue and Pb (II) ions. The
maximum adsorption capacity of 103.1 mg/g for MB separately and
74.5 mg/g for MB + Pb (II) mixture was achieved. The nanomaterial
can be easily magnetically separated and adsorption sites can be
regenerated by a simple process.
Methylene blue This work reports preparation of core–shell magnetic photocatalyst γ- [98]
Fe2O3/silica (SiO2)/titania (TiO2) with varying amounts of TiO2 has
need synthesized and tested. A adsorption capacity of 74 mg/ g for MB
dye was achieved. The nanomaterial can be easily magnetically
separated and adsorption sites can be regenerated by via non-
radiation driven H2O2 activation.
Toluidine blue A magnetic nanocomposite electrode material (NP-SiO2) is prepared [99]
and fully characterized. The removal efficiency of magnetic
nanoparticles (MNPs) and magnetic nanocomposites (NP-SiO2) for
TBO was investigated. Good electrocatalytic effect towards nitrite
oxidation was observed for both electrodes.
Acid red 114 The synthesized magnetic amino-coated silica iron oxide nanoparticles [98]
were applied as nano-adsorbents for removal of acid red 114 dye from
aqueous solutions. The optimum condition at which the
nanoadsrobent shows maximum efficiency are reported. The
maximum absorption capacity of 84.75 mg/g was achieved in just
2 min of time. The nanomaterial can be easily magnetically separated
and reused several times.
Direct red 23 This work reports preparation of chitosan/poly (vinyl alcohol) (PVA)/ [100]
SiO2 nanocomposite ENMs. The major finding was that the
incorporation of 1.0% of SiO2 increased both water permeability and
Direct Red 23 (DR 23) rejection. The optimized nanocomposite
membrane provided 98% DR 23 rejection.
Hoechst 33342 and rhodamine The material was effectively used for the removal of two fluorescent [101]
dyes named Hoechst 33342 and rhodamine from aqueous solution.
Methylene blue This study indicate that the titania-coated silica can be easily adhered [102]
to the polymer systems and can show a higher photocatalytic activity
towards the degradation of organic pollutants such as MB under UV
irradiation.
Methylene blue The synthesized TiO2-SiO2 mixed oxide system showed significantly [103]
higher MB removal and degradation efficiency in comparison with
that of the commercial TiO2 Degussa, P25 material.
Methyl orange and bisphenol In this work, gold/carbon co-doped TiO2 photocatalysts with different [104]
contents of gold were prepared and were immobilized on fused silica
to test their photocatalytic activity using methyl orange under visible
light. It was found that the co-doping significantly red shifted the
absorption edge of the photocatalysts. A high photocatalytic activity
towards methyl orange were achieved. The photodegradation of
combined MO and bisphenol was tested but showed reduced
efficiency.
Methylene blue Methyl orange The silica colloid with immobilized iron oxide nanoparticles was [105]
prepared and fully characterized. It was tested to check removal of MB
and MO. The nanocomposite with more branched structure with low
charge showed better pollutant dye removal capability.
Bromophenol blue, Crystal violet This work reports the synthesis of β-cyclodextrin coated silica [106]
nanoparticles SiO2@β-CD. The material was tested as adsorbent to
remove bromophenol blue (BPB) and crystal violet (CV) in water
(continued on next page)
8
S.A. Jadhav, et al.
Table 2 (continued)
Material
Silica nanoparticles
SiO2 and TiO2 capped Ag2S nanocomposites
Mesoporous silica nanoparticles (MSNs)
Silica superparamagnetic iron supraparticles
Silica nanoparticles
Carboxymethyl cellulose coated Fe3O4@SiO2 core–shell
magnetic nanoparticles
Silver nanoparticle immobilized amino-functionalized
silica nanoparticles
Silver nanoparticles loaded silica nanoparticles
Fe3O4@SiO2@KIT-6-SO3H nanoparticles
Cobalt impregnated silica nanoparticles (Co-SiO2)
Silica nanoparticles
Silica nanoparticles
Nickel nanoparticle loaded mesoporous SiO2-Al2O3
Colloid and Interface Science Communications 30 (2019) 100181
Dye Note with observation Ref.
solution. The sorption kinetics was studied in detail and the removal
of dyes was achieved at room temperature.
Methylene blue In this work, silica nanoparticles were prepared from rice husk by [107]
microwave process. The nanoparticle are tested to remove methylene
blue dye from aqueous media. The particles attained a adsorption
capacity of 679.9 mg/g with removal percentage of 80%.
Eosin Y, Safranin O In this work, SiO2 and TiO2 capped Ag2S nanocomposites (NCs) by a [108]
simple one-pot hydrothermal method with photocatalytic properties
are reported. The prepared samples were tested for the degradation of
Eosin Y (EY) and Safranin O (SO) dyes under sunlight. The results
showed that TiO2 capped Ag2S nanocomposites exhibited an excellent
photocatalytic activity in the degradation of EY (96.41%) and SO
(91.38%) dyes than the bare Ag2S nanoparticles.
Rhodamine B, methylene blue, This work reports synthesis of monodispersed mesoporous silica [109]
methyl violet, malachite green, and nanoparticles (MSNs) as efficient adsorbents for removal of various
basic fuchsin dyes. The conditions at which the adsorbate show maximum efficiency
were optimized and the adsorption capacities were in the range of
14.70 mg/g to 34.23 mg/g, which could be achieved within very short
time. The role for surface silanols and their interactions with cationic
dyes is predicted as possible mechanism of adsorption of the dyes on
the porous silica.
Methylene blue Raspberry-like micron sized supraparticles, capable of methylene blue [110]
removal from water within a few seconds is reported. Supraparticles
built from 10 nm silica nanoparticles combined with 10 nm
superparamagnetic iron oxide nanoparticles showed clearance of
methylene blue from water in 60 s.
Methylene blue, Methyl red In this study silica nanoparticles were synthesized and impregnated in [111]
fly ash to synthesize the cubic shaped nano Faujasite materials This
material was tested to remove the heavy metals (Lead, Chromium, and
Cobalt) and adsorption and degradation of dyes (Methylene blue and
Methyl red).
Methylene blue This work reports preparation and testing of core–shell Fe3O4@SiO2 [112]
magnetic nanoparticles (MNPs) and its use for removal of methylene
blue from aqueous solutions. The optimum conditions at which the
material shows maximum efficiency are reported.
Indigo carmine The work reports, green biosynthesis synthesis of silver nanoparticle [113]
immobilized amino-functionalized silica nanoparticles and their use
for the removal of indigo carmine (IC) dye from aqueous solution. The
maximum adsorption capacity for the IC dye achieved was 73.05 mg/g
Methylene blue Silica nanoparticles loaded with silver nanoparticles on its surface [114]
were prepared. The adsorption performance and catalytic activity of
the Ag/SiO2 for methylene blue (MB) removal was investigated. The
maximum adsorption capacity achieved was 55 mg/g and 99%
catalytic degradation of MB. The nanoadsrobate can be used for eight
and four successive cycles for adsorption and catalytic degradation,
respectively.
Methyl green This work reports preparation of KIT-6 magnetite mesoporous silica [115]
nanoparticles (Fe3O4@SiO2@KIT-6-SO3H NPs) as adsorbents for
methyl green dye from aqueous solutions. The removal efficiency of
the material was 96.4% in acidic pH in only 10 min. The maximum
adsorption capacity for methyl green achieved was 196 mg/g.
Methylene blue and Trinitrotoluene The Co-SiO2 nanoparticles were used for removal of methylene blue [116]
(MB), trinitrotoluene (TNT), and mercury ions. The maximum
adsorption capacities achieved were 250, 20.49 and 40.24 mg/g for
methylene blue, trinitrotoulene and Hg ions respectively.
Acid orange 8 In this work silica nanoparticles were prepared from sugarcane waste [49]
ash and tested for the removal of acid orange dye. The maximum
adsorption capacity achieved was 230 mg/g with reusability of the
material up to five cycles.
Methylene blue This study reports, synthesis of silica nanoparticles (NSBFS) from [117]
commercial blast furnace slag (BFS). The synthesized nanoparticles
were tested to remove methylene blue (MB) from water. The
maximum adsorption capacity achieved in basic pH conditions for MB
from water was 80.8 mg/g.
Methyl orange This work reports the synthesis of Ni loaded mesoporous SiO2-Al2O3 [118]
for selective removal and photocatalytic degradation of methyl orange
dye. About 86% of dye removal and degradation was achieved after an
irradiation time of 180 min using the catalyst at a dose of 3 g/L.
9
S.A. Jadhav, et al.
adsorption will carried out. The design and testing of such structures is
necessary. Another important missing investigation in almost all the
reports is about the stability of various silica based hybrid materials
developed and the exact role of silica in some hybrid materials made of
three to four different materials. The hydrothermal stability of silica or
hybrid silica nanomaterials is important as during their use as na-
noadsorbents and also during their repetitive use (cycles) for removal of
dyes these materials will be kept in contact with water for prolonged
period. So it is important to test the stability of the siloxane network in
the silica particles at different pH or at different concentrations of
acidic or basic dyes. Although, the list of new silica based hybrid na-
noadsorbents with high dye removal efficiencies is increasing none of
them have reached the final stages of the technology development.
5. Conclusions and future challenges
Most of the recent reports in the literature use bottom up ap-
proaches for the synthesis of silica based nanomaterials used for ad-
sorption of pollutants. Although, bottom up methods produce mono-
dispersed nanomaterials with high adsorption efficiencies there scale up
is challenging. To obtain monodispered nanoparticles in large scale
production can be a difficult task. The increased polydispersity of the
nanomaterials affect the efficiencies of the material. Hence, together
with synthesis of new efficient materials the focus of research should be
also on the development of large scale production of the nanomaterials.
As silica is available naturally from various sources, top down ap-
proaches to prepare silica nanomaterials may provide an alternative for
the costly bottom up approaches. The research in future must be also
focused on the transformation of nanoadsorbents in to usable tech-
nology. The laboratory scale models will not work in real application to
purify huge quantity of water. Also while developing the alternative
pollutant removal technology scientists should also bear in mind the
present water purification technologies used by various industries and
perform a comparative analysis with the newly developed or proposed
technology. As we know water pollution is one of the biggest challenge
in front of the human being in coming time, the research on develop-
ment of various technologies to remove pollutants from water will
continue with great interest. Silica and hybrid silica based nanoma-
terials have shown their potential to be one of the most effective na-
noadsorbents for removal pollutants especially dyes from water.
Conflicts of interest
The authors confirm that there are no conflicts to declare.
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