Materials Today: Proceedings xxx (xxxx) xxx

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Materials Today: Proceedings

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

Development of super-hydrophobic surface using Tio2 to reduce adverse

effects of environmental pollutants on buildings
Malathy Ramalingam a, Dhivya Kamaraj a, S.R.R. Senthil Kumar b, R. Raghavi a,
Dharmaraj Rajalinggam c
a
Department of Civil Engineering, Sona College of Technology, Salem 636005, Tamil Nadu, India
b
Sona College of Technology, Salem 636005, Tamil Nadu, India
c
KPR Institute of Technology, Coimbatore, Tamilnadu, India

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

Keywords: The development of self-cleaning surfaces in recent years has been significant in preserving buildings from
Nanoparticles environmental contaminants and improving visual durability. Titanium dioxide (or titania), a photocatalyst, is
Photocatalyst used with cement to improve aesthetic durability and de-pollution properties. Super hydrophilic materials were
Environmental contaminants
developed by covering glass, ceramic tiles, or polymers with the semiconducting photocatalyst titanium dioxide
TiO2 self-cleaning surface
(TiO2). Grease, grime, and organic pollutants disintegrate when TiO2 is exposed to light and are simply swept
away by water (rain). Ink and vehicle smoke are utilised to evaluate the self-cleaning properties of TiO2-con­
taining concretes, and the oxidation of carbons (COx), gaseous atmospheric pollutants responsible for acid rain
and photochemical smog, is explored using nano titanium dioxide. The research allowed for the identification of
photo-oxidation mechanisms of stain and COx on TiO2-containing cement, as well as parallels and differences
with pure unsupported TiO2. Engineering TiO2 particles with certain crystallite sizes and modifying the pho­
tocatalyst electrokinetic properties by changing the overall pKa of the TiO2 surface have both been shown to be
efficient approaches for controlling the attractive features of ion-ion correlation forces. The effects on applica­
tions in a concrete building, specifically on the exterior surface, to improve overall photocatalytic activity are
reviewed. The experimental data on photocatalytic performances measured for regular and nano-coated samples
are examined regarding photocatalyst qualities and the effect of cement’s chemical environment on titania
particles. The research allowed for the identification of photo-oxidation mechanisms of stain and COx on TiO2-
containing cement, as well as parallels and differences with pure unsupported TiO2.

1. Introduction solar energy chemical conversion and storage. In recent years, TiO2
semiconductor photocatalysis has been employed to address key envi­
The super-hydrophilic or super-hydrophobic feature of TiO2 is ronmental issues such as water and air purification.
employed to create a self-cleaning material surface in the concrete. The
microstructure of selected plant surfaces was translated into practical 2. Need for Tio2 in concrete
materials such as cement, tiles, and facade paints to create super-
hydrophobic surfaces (Lotus effect) [1]. Super hydrophilic materials Because of the different causes of pollution in large cities, the air
were developed by coating glass, ceramic tiles, or polymers with the inside buildings can be more polluted than the air outside. The air
semiconducting photocatalyst titanium dioxide (TiO2). Grease, dirt, and cleaning agents such as Titanium dioxide (TiO2) in the technology of
organic pollutants dissolve when TiO2 is exposed to light and are simply making concrete composite panels for tackling the problem of carbon
wiped away by water (rain) [2]. The interaction of TiO2 with common dioxide (CO2) in buildings are reported in this paper. TiO2′s anti-
building materials including concrete, cement, and plaster will be the fogging, anti-bacterial, anti-corrosion, and semiconducting quali­
focus of our future research [3]. In 1972, Fujishima and Honda used ties led to its usage in concrete surfaces [4]. The porosity of the panel,
TiO2 electrodes to find photocatalytic water splitting. In heterogeneous different types of materials, and varying percentages of TiO2 utilized in
photocatalysis, this marked the beginning of a new age. Even though the mix design were all evaluated as factors that would affect the per­
TiO2 absorbs only approximately 5% of the solar light that reaches the formance of the panel. The degradation processes under normal sunlight
earth’s surface, it is the most studied semiconductor in the subject of conditions are investigated to assess the efficacy of photocatalytic active

https://doi.org/10.1016/j.matpr.2023.07.331
Received 19 March 2023; Accepted 28 July 2023
2214-7853/Copyright © 2023 Elsevier Ltd. All rights reserved. Selection and peer-review under responsibility of the scientific committee of the 2023 International
Conference on Advanced Technologies in Chemical, Construction and Mechanical Sciences.

Please cite this article as: Malathy Ramalingam et al., Materials Today: Proceedings, https://doi.org/10.1016/j.matpr.2023.07.331
M. Ramalingam et al. Materials Today: Proceedings xxx (xxxx) xxx

concrete products [5]. greater than 3,2 eV (λ= 388 nm). (See Figs 5.1-5.3 Figs 6.1 and 6.2).

3. Materials and methodology 3.1.3. Cement

By mixing pozzolanic materials with gypsum and OPC clinker, either
3.1. Materials used simultaneously or separately ground, Portland Pozzolana Cement (PPC)
is created. PPC withstands intense water attacks and prevents the
Depending on the application, the catalyst can be used with either development of calcium hydroxide during the setting and hydration of
white cement or standard cement. White cement is preferred for the cement. PPC is utilised in heavy-duty infrastructure and construction,
aesthetic appeal of the building’s exterior surface. The titanium dioxide including marine structures, mass concreting, plastering, masonry
catalyst utilized for the photocatalytic effect is detailed further below. mortars, and any other applications where regular Portland cement is
used. PPC is very well-liked in India, and as more cement plants
3.1.1. Titanium dioxide construct jetties for shipping, initial costs will eventually go down as
In India, the titanium dioxide element is prevalent. Sulfate and well. PPC is more resistant to the attack of aggressive fluids than Ordi­
chloride procedures are used to extract titanium dioxide predominantly nary Portland Cement and creates less heat during hydration. Addi­
from slag. Sulfuric acid is used to cure the slag, and the resulting titanyl tionally, when employed in hydraulic structures, it lessens the leaching
sulphate is then hydrolyzed to generate a hydrate, which is then calcined of calcium hydroxide. It is very effective in a mass concrete building,
at 1000 ◦ C to produce Titanium dioxide. Both the sulfate and chloride including maritime and hydraulic construction. Wherever ordinary
processes yield rutile crystalline forms, however, only the sulfate pro­ Portland cement may be used, Portland Pozzolana Cement can generally
cedure yields anatase Titanium Dioxide, which is the preferred form for be utilised as well.
food, medicine, and cosmetic applications. Titanium dioxide absorbs
moisture from the environment [6]. As a result, it produces unstable 3.1.4. Fine aggregate
radicals that react with pollutants such as carbon dioxide and Sulphur For concrete work, the aggregate should be tough, enduring, and
dioxide, breaking them down and preventing them from clinging to the clean. There should be no trace of organic or vegetative materials, fine
building’s surface [7]. In addition to rutile, anatase, and brookite, tita­ dust, or lumps of clay in the aggregate. All of these obstructions hinder
nium dioxide can be produced into three metastable phases (monoclinic, aggregate from adhering, lowering the concrete’s strength. A fine
tetragonal, and orthorhombic), as well as five high-pressure forms aggregate is defined as material that can pass through a sieve with a
(-PbO2-like, baddeleyite-like, cotunnite-like, orthorhombic OI, and 4.75 mm opening. Natural river sand is typically used as fine aggregate.
cubic phases). Fine aggregate is composed of angular grains that are clean, and free of
organic materials, dust, and grime. It is forbidden to utilise sea sand.
3.1.2. Photo catalytic effect of Tio2 Sand is a crucial component of paver blocks. Small silica grains make up
Titanium dioxide is a semiconducting material that is chemically the sand particles. Due to a variety of weather-related factors, sand­
activated when exposed to light as shown the Figure 1. The photo­ stones decompose to create them. Based on the natural resources used to
activity of TiO2, which has been known for over 60 years, is currently produce the sand. Pit sand, River sand, and Sea sand are the three
being studied in depth [8]. There was a serious barrier for a long time, different forms of sand. In that, river sand is frequently on hand and in
particularly in terms of its use as a pigment. When exposed to light, pristine form. It is extensively used for various objectives. We are only
organic materials tend to deteriorate. As a result of photocatalytic ac­ allowed to use zone III sand.
tivities, the organic components of the paint dissolve, resulting in the
well-known phenomenon of “paint chalking.” When compared to rutile 3.1.5. Water
and brookite, anatase has the highest photoactivity. As a result, rutile Concrete was mixed and the specimen was also cured using potable
TiO2 is virtually exclusively used in industrial applications [9,15]. TiO2 tap water that was on hand in the lab and that had a pH value of 7–1 and
is a semiconductor with an Eg = 3,2 eV band gap energy. The band gap is complied with IS 456–2000.
exceeded and an electron is promoted from the valence to the conduc­
tion band when this material is bombarded with photons with energies 3.2. Properties of materials

3.2.1. Cement

3.2.1.1. Specific gravity. The empty dry-density bottle was initially

weighed and designated as M1. Cement was added to the bottle after
which it was weighed as M2. After being dry, the density bottle was
partially filled with cement and kerosene, and it was weighed as M3.
Kerosene was added to the density container until it reached the top, and
it was then weighed as M4.

Fig. 1. Photocatalysis Process. Fig. 5.1. Normal Coating (Left), Nano Coating (Right).

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M. Ramalingam et al. Materials Today: Proceedings xxx (xxxx) xxx

Fig 5.2. Stain removed in Nano TiO2 Coated Surface.

Fig 6.2. Carbon Removed on the Surface in 10 h.

block’s surface. It was permitted access to the test block. The test block
was initially entirely penetrated by the needle. The needle could only go
down 33 to 35 mm from the top once the paste started to lose its flexi­
bility. The first setting time was calculated as the interval between
adding water to the cement and when the needle had pierced the test
block 33–35 mm or more from the top.

3.2.1.3. Consistency. The purpose of this test is to determine how much

water has to be added to the cement to produce a paste with a typical
consistency. For the first trial, 500 grammes of cement were obtained
and formed into a paste using a measured amount of water (per cent by
Fig 5.3. Stain in Normal Concrete Surface. weight of cement). Vicat mould plunger with a 10 mm diameter and
50 mm length was attached, lowered down to meet the paste’s surface in
the test block, and then quickly released to sink into the paste by its
weight. The paste was made according to the usual procedure. The
plunger’s depth of penetration was noted. Similar to this, tests were
carried out with increased water-cement ratios until the plunger pene­
trated 33–35 mm below the top. The amount of water needed to create
cement paste with a specified consistency is that specific percentage,
which only permits the plunger to penetrate 33–35 mm below the
surface.

3.2.2. Fine aggregate

3.2.2.1. Specific gravity. Dry off and clean the pycnometer. Find the
mass of the brass cap and washer-equipped empty pycnometer (M1) in
kilogrammes. 200 to 400 g of dry soil sample retained at 4.75 mm should
be added to the pycnometer to fine-tune the mass (M2). Red glass and
the soil sample should be well combined. Stir in additional water. To fill
the pycnometer flush with the hole in the conical cap, replace the screw
top. Dry the pycnometer outside, then calculate its mass (M3). Clean the
pycnometer thoroughly, then fill it up to the opening in the conical top
with clean water to determine its mass (M4).
Specific gravity of cement (G) = (M2-M1)/[(M2-M1)-(M3-M4)].
M1= Mass of the empty pycnometer.
M2= Mass of the bottle & sand.
M3= Mass of the bottle, sand & water.
M4= Mass of the bottle filled with water.
Fig 6.1. Initial Stage when smoke is applied on the Tio2 Surface.
3.2.2.2. Water absorption test. The weight of 100 g of nominal coarse
Specific gravity of cement (G) = (M2-M1)/[(M2-M1)-(M3-M4)]. aggregate, or W1, was calculated. After then, the sample spent 24 h
M1= Mass of empty density bottle. submerged in water. It was then removed, drained, and its weight, say
M2= Mass of the bottle & cement. W2, was determined using the expression given below. The sample’s
M3= Mass of the bottle, cement & kerosene. water absorption is determined by the difference between W1 and W2.
M4= Mass of the bottle filled with kerosene.
W = [(W 2 − W 1 )/W 1 ]X100

3.2.1.2. Initial setting time. The Vicat apparatus needle was swiftly
3.2.2.3. Surface moisture. The amount of sand was measured as M1 and
released after being gently lowered and coming into touch with the test

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placed in the little pan. The pan was then left in the oven for a whole day. photodegradation of TiO2 distributed in cementitious materials [21]. To
It was removed, and M2 is the estimated dry weight. The sample’s evenly mix the mixture put within, an ultrasonic vibrator creates ul­
surface moisture is determined by the difference between M1 and M2. trasonic vibration. The catalytic process is carried out by ultrasonic vi­
bration in the absence of a catalyst. For the entire catalytic process, we
3.2.2.4. Fineness modulus (by sieve analysis). The sample was dried at can place the mixture for 180 s. We can apply surface coating because
room temperature to achieve an air-dry condition. The necessary the combination we can obtain is uniform.
amount of the sample was collected (Kg). In a mechanical sieve shaker,
the sieves were arranged in size order, with the largest sieve on top. Ten 4.3. Tests on samples
minutes were spent sieving. The fraction of aggregate that is coarser
than the sieve under consideration and finer than the sieve above is The various test to determine the smog-eating effect of mortar cube is
represented by the material that was retained on each sieve after listed below [30].
shaking. A total sample was created by weighing the material that was
retained in each filter. The ratio of the cumulative percentage of weight • Stain removal test
retained (F) to 100 was used to calculate the fineness modulus. • Carbon emission test
• Sorpitivity test
3.2.2.5. Bulk density. The weight of a substance in a specific volume is
known as bulk density. Kg/m3 is used to express it. With 25 S of thor­
oughly mixed sand, the cylindrical measure was filled approximately 1/ 4.3.1. Stain removal test
3 at a time. Using a rod as a straight edge, the measure was carefully We have placed a few stains on the surface of the nano titanium
knocked off level. It was calculated how much fine aggregate weighed in dioxide mortar cube as part of the stain removal test. By using a pho­
net terms. tocatalytic reaction, the nano titanium dioxide reacts with stains and
Bulk Density= M/V. clears them from the coated surface. Here, two samples were used to
M= Mass of aggregate. compare how well nano TiO2 and regular cement both removed stains.
V= Volume of cylinder = πr2. To examine the effect, the ink is applied to the sample. While the stain is
still there in regular cement, it has been erased using nano titanium
4. Testing results using titanium dioxide dioxide.

4.1. General 4.3.2. Carbon emission test

This nanoparticle-coated material is put through a test for carbon
The feasibility of photocatalytic reaction of reducing air pollutants in dioxide emissions. The specimen is mounted on the car, and the smoke is
the micro-working environment was determined through experimental left in the open area with its surface exposed. The discolouration on the
investigation of the self-cleaning and smog-eating environment prop­ surface material has been eliminated after 10 h. Below is a photo that
erties by using nano titanium dioxide in a commercial building, depicts the outcome. Whereas in regular cement, the modifications have
educational institution, industrial building, etc [10]. The impact of not occurred, the nano TiO2 has changed as a result of the photocatalytic
operating factors like exposure time, catalyst coating and UV radiation effect [13]. It can be utilised in industries with substantial carbon di­
on the photocatalytic reaction’s ability to reduce co-pollutants in the air oxide output to avoid sticking and lessen the pollution effect.
was also discovered [16]. The results of the co-evaluation are explained
below. 4.3.3. Reaction of stain and carbon on Tio2
TiO2 + Moisture.
UV ↓.
4.2. Optimised proportion of titanium dioxide with cement OH– + H+ (Radicals).
↓.
In the earth’s crust, the element titanium is typically found with iron Toxic gases + OH– + H+ (Radicals + stain).
in the mineral oxide ilmenite (FeTi03) and the less frequent ore rutile. ↓.
For this white pigment, these are the typical starting components. Iron is Changes the toxic gases into a non-toxic and eliminates them into a
extracted from iron ores with a high titanium content, and the leftover free atmosphere.
slag is then treated and put to use. By utilizing the photocatalytic ac­ According to reports, moisture significantly influences how well this
tivity of the catalyst, we can combine cement with 5 to 20 per cent of nanomaterial performs. This study looked into the effects of moisture on
nano titanium dioxide to produce an effective self-cleaning character­ stain reemission and removal as well as the relevant mechanisms.
istic [11]. Paints, cosmetics, and other ageing industries can employ Adsorption was discovered to be minimal without UV irradiation [14].
roughly 5% of the nano titanium dioxide. We employed between 10% As per the findings, UV irradiation can be used effectively to reduce
and 20% of nano titanium dioxide with cement in this case to counteract harmful gas emissions and reemission.
the smog-eating effect of the concrete on the surface [12]. The following
tools were used to combine titanium dioxide with cement for experi­ 4.3.4. Sorptivity test
mental purposes: While there won’t be any seepage of water through the concrete,
there is less water absorption of the titanium dioxide. The water ab­
• Microbalance sorption test took this away. A mortar cube with nano-TiO2 coating and
• Magnetic stirrer a standard mortar is used to collect the two samples. Both are weighed,
• Ultrasonic vibrator submerged for 24 h, and removed. The sample should be weighed once
again. Table 1 displays their outcomes.
Here, a magnetic stirrer is used in which a magnetic pellet is placed
with fully and uniformly mix material utilizing magnetic wave action. 5. Recommendations
The magnetic pellet is first placed into the sample and over the machine;
after that, the RPM speed can be adjusted based on the sample’s mag­ TiO2 has applications in latex paint decorative architectural coatings
netic wave motion. 360 RPM was utilized here for mixing. Strini et al. and powder coatings/paints [17]. They can be employed in solar panel
used the Mixed flow reactor to investigate the gas phase coatings with low VOC/high solids compositions [18]. The self-cleaning

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