Self-cleansing of rigid pavements by using flyash and titanium dioxide.

doi:10.21203/rs.3.rs-4876639/v1

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Self-cleansing of rigid pavements by using flyash and titanium dioxide.

https://doi.org/10.21203/rs.3.rs-4876639/v1

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This study innovatively investigates the use of TiO₂ particles and flyash with cement to reduce pollution. The study was conducted by replacing OPC with photocatalytic concrete, prepared by partial replacement of cement with TiO₂ and flyash. As it is a chemically stable and versatile semiconductor, TiO₂, when incorporated into concrete mixes as a photocatalyst, degrades organic pollutants like NOx, SOx etc. in the presence of UV light radiation. For the best efficiency of TiO₂, flyash was added, which not only adds to the durability of concrete but also increases the porosity of concrete, and thus increases the number of active sites for the photocatalytic reactions to take place. The M30 concrete mix ratio was used for the casting of nominal and photocatalytic concrete. Cement was partially replaced by 10%, 15% and 20% flyash. TiO₂ was used as 1.6%, 2.2%, and 2.6% by the weight of M30-grade concrete. Concrete cubes were made based on combinations of varying percentages of flyash and TiO₂ for the slump cone test and compressive strength test. The early compressive strength, though decreased due to addition of flyash but attained the peak value of 42.65 N/mm² at 15% flyash which further increased to 52.60 N/mm² for the combination of 15% flyash and 2.6% TiO₂. The photocatalytic activity of TiO₂ and degradation of pollutants was investigated by exposing the cubes sprayed with methylene blue dye as a model pollutant and structurally by the Fourier transform infrared spectroscopy test, where the graphs obtained were compared with the reference graphs.

Titania

Photocatalysis

Nanoparticles

Methylene blue dye

FTIR

In urban areas and metropolitan cities, one of the major issues- air pollution is caused by industries and transportations. Local traffic and industrial flue gases produce the vast majority of pollutants

(Ms.C.Sakthipriya et al. 2020). From coal-fired thermal stations, thermal power electricity is produced. Coal based thermal power plants produce large amount of coal ash which causes major environmental issues as well as other connected difficulties. Flyash- a byproduct of coal combustion, made up of fine particles which are expelled from the boilers along with flue gases. Because flyash is difficult to decompose, it was formerly released into the atmosphere but the current air pollution control rules mandate that the flyash needs to be collected by installing pollution control devices (Rishabh Joshi 2017). In the near future, these air pollutants will continue to be the major problem despite stricter emission control regulations and more installations of emission reduction devices. Though several initiatives like redesigning automobiles, promoting carpooling and public transit etc. have been taken for reduction of emission, these emissions are still major cause of air pollution (Ms.C.Sakthipriya et al. 2020).

Cement production contributes to greenhouse gas emissions (Prof. Rakesh Kumar et al 2023). Cement production accounts for about 5% of all carbon emissions released into the atmosphere. Roughly half of the CO₂ is released by the calcinations process to produces CaO out of CaCO₃. The remaining carbon is a result of energy used during the production process (M. Ondova et al. 2012). According to the International Energy Agency’s (IEA) Greenhouse Gas R&D Program (D.N. Huntzinger 2009), cement production generates an average world carbon emission of 0.81 Kg CO₂ per Kg cement produced.

This study aims to reduce emission by employing air cleaner sources like phoyocatalyst, which is a method of eliminating pollutants from atmosphere (Shen. et al. 2015) alongwith, the partial substitution of flyash into cement paste because it has pozzolanic activity, which helps the concrete to set and provides additional protection to concrete from moisture and chemicals (Rishabh Joshi 2017). CO₂ emissions associated with cement productions can be lowered by the addition of flyash as an additional cementitious ingredient to concrete to increase its sustainability (P. Nath et al 2011). Flyash is amorphous aluminosilicate material that, although not cementitious in its pure state, become cementitious compound when it react with water and calcium hydroxide, establishing them as a far more superior than traditional Portland cement concrete in terms of environmental friendliness, as it provide numerous benefits such as improved cold resistance, decreased heat of hydration (P. R. de Matos et al, 2019) and even energy reduction (S. Zhang et al, 2022), constraining CO₂ emission, utilizing fewer natural resources, and handling hazardous waste oversight (M. Czop et al 2022). Besides improving workability, pumpability, durability and flexural strength, flyash concrete also improves concrete finishing. Additionally, it lessens alkali silica corrosion (Ketan et al 2012).

The last three decades have seen a steady influx of smart devices into the market, based on the discovery of photocatalytic capabilities of conductor materials (O. Carp et al 2004). Currently, the self cleaning surfaces that rely on photocatalytic reactions are used in a variety of settings including buildings, roads, side view mirrors, lamps and even textiles (K. Hashimoto 2005). Due to their effective ability to transform solar energy into chemical energy, heterogeneous photocatalyst have gained substantial attention, primarily in applications related to field of environmental cleanup. A number of studies produced good and promising outcomes in terms of deterioration of various pollutants released by fossil fuels used in vehicles. Because photocatalytic road pavements have large surface area, they are cited as potentially useful surfaces for reduction of SO₂, NOx, Cox and VOCs that are found in atmosphere (Iran Rocha 2019).

Photocatalytic materials have the ability to degrade organic pollutants like oils and greases,that have been adsorbed to the surface when exposed to light radiation. This property makes photocatalytic materials self- cleaning, which is crucial for road engineering applications as it can significantly reduce the number of car accidents (Iran Rocha 2019). TiO₂ harness the energy from light striking the concrete surface to breakdown the dirt into molecules like water and O₂. Liquid and solid remain on the surface to be carried away by rain whereas gases drift away (Ms.C.Sakthipriya et al. 2020).

TiO₂ has drawn greatest attention among oxide based semi conductors which include ZnO and WO₃. In 1960s, Fujishima conducted research on photocatalysis of water using TiO₂ electrode. His studies revealed novel techniques for producing hydrogen using TiO₂ material in the wake of this major shift in photoelectrochemistry and in response to the oil crises of 1970s. However, because UV light radiation is necessary (merely making upto 3% of the solar spectrum) to initiate photocatalysis, the generation of H₂ by employing TiO₂ seemed unappealing. Afterwards, studies have indicated use of TiO₂ to the photo degradation of air and water pollutants (K. Hashimoto 2005). Photocatalytic concrete with TiO₂ additives was produced by Husken et al, (2009) and as a result of experiments, they reported that they separated NO and NO₂ compounds under UV light. Bertrand Rout et al (2009) studied the photocatalytic activity of cement paste and mortar through the addition of varying amounts of TiO₂. In cement paste as compared to mortar, it was observed that TiO₂ concentrations of upto 5% and more than 1% have good photocatalytic qualities. Chen et al (2011) investigated the self cleaning performance. Rhodamine B was used as a model pollutant. Products containing TiO₂ showed the color shift. In non- TiO₂ products, no color shift was seen. Wang et al (2015) investigated the degradation of organic pollutants on TiO₂ – coated road surfaces. The studies reveal that TiO₂ is effective in degrading VOCs and nitrogen oxides under UV light radiations. The high photocatalytic activity is observed because of its large surface area, high crystallinity and generation of reactive oxygen species. Li et al (2019) conducted a study regarding the parameters influencing the photocatalytic activity of TiO₂ and ZnO. Degradation efficiency was found to be highly dependent on a number of variables including catalyst loading, exposure duration, surface shape and radiation intensity. Liu et al (2020) studied the efficiency of TiO-ZnO composite coatings in self cleaning road applications. He prepared TiO-ZnO composites were created and applied to concrete road samples. When compared to pure TiO₂ or ZnO coatings, the composite coatings showed increased photocatalytic activity. It has been observed from literature review that various researchers investigated the photocatalytic activity of TiO₂ on pavements and various factors that influence it. However, the present study deals with the combined effect of TiO₂ and flyash. TiO₂ was incorporated into concrete mix for its self cleaning ability. Flyash is also added to enhance the self cleaning ability as it increases the porosity of concrete and hence active sites for photocatalytic reactions.

Materials

In the present study, cement of grade 43, having specific gravity 3.15 was used. Locally available sand (zone 3) passing through 4.75mm IS sieve size having specific gravity of 2.71 was used as fine aggregate. The coarse aggregate of nominal size 20mm was used. Titanium dioxide or titania was used as a phoyocatalytic material to degrade the organic pollutants in the presence of UV light radiations. C type flyash which is obtained from lignite or sub-bituminous coal was used. Cement was partially replaced with different percentages of flyash (10%, 15% and 20%).

Sample preparation

The M30 concrete cube specimens of 150mm x 150mm x 150 mm were casted as per IRC 44: 2017 and IS 10626:2009 (wherever necessary). 6 conventional cubes were casted and the rest by using the combination of varying percentages of flyash (10%, 15% and 20%) and TiO₂ (1.6%, 2.2% and 2.6%). Flow diagram 1 shows the combinations of varying percentages of flyash and TiO₂.

Methodology

The Workability of fresh cement paste was determined by the slump cone test to study the effect of TiO₂ and flyash inclusion in cement. Compressive strength test was conducted on the prepared cube specimens. The 7-day and 28-day compressive strengths were recorded by means of a universal testing machine (UTM) with a loading rate of 30kN/min. The average of test results from the three specimens was taken as the compressive strength of a particular mix sample.

The self-cleaning performance of TiO2-modified fly ash was examined by analyzing the photodecomposition of Methylene Blue Dye (MB Dye), acting as a model pollutant, on specimen surface under artificial UV exposure. MB [7-(dimethylamino)phenothiazin-3-ylidene] dimethylazanium chloride (C₁₆H₁₈ClN₃S). Methylthioninium chloride- also called Swiss Blue is an organic dye of dark blue color. Photocatalytic decomposition of MB dye would be given by the fading of dark blue color. Methylene Blue solution was prepared by adding each 20mg and 30 mg of MB dye in 1lt of distilled water at room temperature.

FTIR test of specimens was done to examine, chemically, the degradation of pollutants (MB dye). Samples for this test were prepared by taking the small pellets of cubes and removing coarse aggregates from them. These pellets were grinded into fine powder and sieved.

Slump cone test results

The slump value for the conventional concrete was found to be 100mm. The slump value was found to be decreased with the addition of flyash and TiO₂. As the percentages of flyash and TiO₂ are increased, the slump value goes on decreasing and thus the workability increased due to the addition of flyash. Table 1 shows the decrease in slump value with the addition of flyash and TiO₂.

Table-1 Slump value due to addition of flyash and TiO₂

Flyash	TiO₂	Slump value
10%	1.6	90
15%	2.2	85
20%	2.6	80

Compressive strength test

To evaluate the impact of flyash replacement on concrete strength, a series of tests were conducted by using UTM. Concrete cubes, made with varying flyash replacement levels (0%, 10%, 15% and 20%), were tested after 7 and 28 days of curing. The control group, consisting of regular concrete without flyash, exhibited standard compressive strengths of 21.41N/mm² and 32.11N/mm² after 7 and 28 days, respectively. The compressive strength of M30 grade of concrete for varying proportions of flyash after 7 and 28 days are listed in table 2 and 3.

Table-2 Compressive strength of M30 grade concrete for varying proportions of flyash at the age of 7 days.

7 days compressive strength test
Mix	Load (KN)	Compressive strength N/mm²	Average Compressive strength N/mm²
0% flyash	454.1	20.18	21.41N/mm²
	491.5	21.82
	455.3	22.23
10% flyash	338.7	15.05	15.16N/mm²
	344.9	15.32
	341.2	15.16
15% flyash	328.4	14.5	14.71N/mm²
	342.9	15.24
	325.8	14.4
20% flyash	320.6	14.22	14.24N/mm²
	341.2	15.18
	322.8	14.34

Table-3 Compressive strength of M30 grade concrete for varying proportions of flyash at the age of 28 days.

28 days compressive strength test
Mix	Load (KN)	Compressive strength N/mm²	Average compressive strength N/mm²
0% flyash	697.05	30.98	32.11 N/mm²
	712.35	31.66
	758.47	33.71
10% flyash	784.57	34.87	35.34 N/mm²
	792	35.20
	808.87	35.95
15% flyash	965.25	42.9	42.65 N/mm²
	976.5	43.4
	937.12	41.65
20% flyash	841.95	37.42	38.59 N/mm²
	893.47	39.71
	869.40	38.64

The effect of fly ash and TiO₂ on compressive strength at the age of 7 and 28 days of age is shown in the table 3 and 4.

Table-4 Compressive strength of M30 grade concrete for varying proportions of flyash and TiO₂ at the age of 7 days.

7 days compressive strength test
Flyash (%)	Titanium dioxide (%)	Compressive strength (N/mm²)
10	1.6	18.22
	2.2	22.48
	2.6	25.74
15	1.6	19.61
	2.2	23.54
	2.6	27.13
20	1.6	17.54
	2.2	20.48
	2.6	24.74

Table-5 Compressive strength of M30 grade concrete for varying proportions of flyash and TiO₂ at the age of 28 days.

28 days compressive strength test
Flyash (%)	Titanium dioxide (%)	Compressive strength (N/mm²)
10	1.6	38.60
	2.2	41.40
	2.6	43.96
15	1.6	46.45
	2.2	49.34
	2.6	52.60
20	1.6	36.43
	2.2	38.01
	2.6	41.78

Methylene blue dye test result

Decolourization of methylene blue dye was observed when concrete cubes sprayed with 20mg/l and 30mg/l were exposed to light.

Discoloration of MB dye on TiO₂ in cement involves not only a proper photocatalytic mechanism (TiO₂ sensitized photoreaction) but also a dye sensitised pathway. In the first mechanism, light activates TiO₂ through the promotion of electrons from the valence band to the conductance band. Adsorbed water and oxygen react with valence band positive holes (left after promotion) and conductance band electrons respectively to generate hydroxyl radicals, HO, which ultimately degrade the adsorbed dye. In the second mechanism, electrons in the HOMO level of the dye undergo transitions to the LUMO level and are subsequently injected into the conductance band of TiO₂. These electrons are therefore used by oxygen to generate oxidative species which degrade the already partially reacted dye.

FTIR test results

The specimen’s FTIR (Fourier Transform infrared Spectroscopy) data displays distinctive peaks that match the functional groups found in the material utilized, including titanium dioxide, cement, flyash and dye molecules.

Identification of titanium dioxide

Because of it’s lattice vibrations, titanium dioxide displays an absorption bands in the 400–800 cm^–1 range. The peaks in graph that correspond to hydroxyl groups, aliphatic compounds, and aromatic compounds are extremely recognizable and suggestive of certain chemical interactions.

When concrete cubes, partially replaced with fly ash and titanium dioxide, are exposed to sunlight to degrade MB dye, the FTIR results reveal alterations in the spectra that reflect the breakdown products and potential structural alterations. The degradation of dye molecules is indicated by shifting or disappearing peaks and the creation of additional peaks represents the byproducts or intermediates of that degradation.

Observations from absorption spectra

Figure 6 shows the FTIR spectrum of the test sample. Following are the FTIR results concluded from the graph:

Interactions of the Matrix:- Changes in the concrete matrix during degredation reveal interactions between the photocatalytic materials ( flyash and titanium dioxide). These interactions are evident in the changes observed in the infrared spectra of concrete.
Existence of Fly Ash:- Presence of flyash was indicated by specific peaks including (Al-O-Si) stretching vibrations at (800-900 cm^-1) and (Si-O-Si) stretching vibrations between 1000-1200 cm^-1.
Titanium Dioxide Peaks:- Peaks observed in the region of 400-800cm^-1 revealed the presence of titanium dioxide bonds.
Dye Degradation:- The breakdown of dye molecules was evident by the disappearance of peaks associated with aromatic C-H stretching vibrations (around 2900-3100cm^-1) and C=C stretching vibrations (approximately 1600-1700cm^-1) suggested that the dye molecules are breaking down.
Formation of Byproducts:- The emengence of new peaks in the spectrum indicated the formation of degradation intermediates or byproducts. These peaks line up with functional groups like carboxyl or hydroxyl groups, found in the breakdown products.

The study aims the self cleaning application of flyash and titanium dioxide as they provide an efficient strategy to obtain self cleansing effect of roads. The results of the experimental tests were leaded the following conclusions:-

Comparing with the conventional concrete, workability of TiO₂ and fly ash concrete goes on increasing with increase in TiO₂ and fly ash percentages.

It was observed that the compressive strength decreases with addition of fly ash. The compressive strength was found to be maximum in nominal concrete which started decreasing with increasing percentages of fly ash.

For constant fly ash percentage, the compressive strength was found to be increased by the addition of varying percentages of titanium dioxide.

For a constant titanium dioxide percentage, the compressive strength Increases for 10% and 15% fly ash and then decreases at 20% fly ash.

The Si-O-Si vibrations around 1000–1200 cm^-1 and Al-O-Si stretching vibrations around 800–900 cm^-1 indicated the incorporation of fly ash into the concrete matrix.

New peaks started forming in the spectra corresponding to the Intermediates formed during the photocatalytic process. These products corresponds to the functional group of degraded products.

Appearing of small peaks corresponding to the C = C stretching vibrations Showed the degradation of dye.

FTIR shows high impact on the fly ash and TiO₂ containing samples and little impact on the conventional concrete.

Funding

This research received no specific grant from any funding agency in the public, commercial, or not-for-profit sectors.

Author Contribution

Study conception and design: Author Miss Sofian Farooq, Author Miss Mehreena Manzoor, Author Mr. Tajamul Islam Zargar; Material collection: Author Miss Sofian Farooq, Author Miss Mehreena Manzoor; Analysis and interpretation of result: Author Miss Sofian Farooq, Author Miss Mehreena Manzoor, Author Mr. Tajamul Islam Zargar; Draft manuscript preparation: Author Miss Sofian Farooq, Author Miss Mehreena Manzoor. All authors reviewed the results and approved the final version of the manuscript.

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No competing interests reported.

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You are reading this latest preprint version

Self-cleansing of rigid pavements by using flyash and titanium dioxide.

Status:

Version 1

Abstract

Figures

Introduction

Materials and methodology

Materials

Sample preparation

Methodology

Result and discussion

Slump cone test results

Compressive strength test

Methylene blue dye test result

FTIR test results

Identification of titanium dioxide

Observations from absorption spectra

Conclusions

Declarations

Funding

Author Contribution

References

Additional Declarations

Status:

Version 1