Investigation of photocatalytic degradation of diazinon

using titanium dioxide (TiO2) nanoparticles doped

with iron in the presence of ultraviolet rays from the

aqueous solution

MohammadMehdiBaneshi

, Soheila Rezaei

, Abdolmohammad Sadat

, Ali Mousavizadeh

Mansour Barafrashtehpour

and Hamid Hekmatmanesh

Social Determinants of Health Research Center, Yasuj University of Medical Sciences, Yasuj Iran

Department of Biostatistics, Yasuj University of Medical Sciences, Yasuj, Iran

Department of Environment Health, Isfahan University of Medical Sciences, Isfahan, Iran

ABSTRACT

Diazinon is one of organophosphate pesticides which it is classi ed as a relatively dangerous substance (Class II by

World Health Organization). The aim of this study was to determine the ef ciency of photocatalytic degradation of

diazinon using titanium dioxide (TiO2) nanoparticles doped with iron in the presence of ultraviolet light in aqueous

solution. This cross-sectional study was conducted at the laboratory scale in a 2 L reactor. The nanoparticles were

synthesized by sol-gel method. The degradation of diazinon was evaluated in various amounts of pH, time, nanopar-

ticles dosage, and the concentration of diazinon. The obtained results were analyzed using Excel2007 and SPSS V.16

software and regression test. The results showed that the increasing pH, reducing the concentration of diazinon and

increasing contact time can lead to increase the removal ef ciency. The optimum pH was obtained to be in neutral

range and at the pH=7. In addition, the optimum amount for contact time, nanoparticle dosage and diazinon concen-

tration was found to be 60 min, 100mg/L and 50mg/L, respectively. The maximum removal ef ciency was 98.58%.

Photocatalytic processes have high capacity in removing of diazinon and can effectively mineralized this compound.

Furthermore, the TiO2 nanoparticles are not toxic and they can be used to remove the pollutants in various industries.

Thus, doped nanoparticles due to the small amount of nano-materials, low energy consumption and high ef ciency

can be used as a good alternative to the removal of diazinon.

KEY WORDS: DIAZINON, PHOTOCATALYTIC DEGRADATION, DOPING, TIO2

ARTICLE INFORMATION:

*Corresponding Author: hamidhekmat60@yahoo.com

Received 27

Nov, 2016

Accepted after revision 27

March, 2017

BBRC Print ISSN: 0974-6455

Online ISSN: 2321-4007

Thomson Reuters ISI ESC and Crossref Indexed Journal

NAAS Journal Score 2017: 4.31 Cosmos IF : 4.006

reserved.

Online Contents Available at: http//www.bbrc.in/

Biosci. Biotech. Res. Comm. Special Issue No 1:60-67 (2017)

MohammadMehdiBaneshi et al.

INTRODUCTION

A variety of methods such as degradation by ultrasonic

waves (Mahmoodi et al. 2007), biodegradation (Danesh-

var, 2007), optical degradation ( olovi et al. 2011), ozo-

nation (Wu, 2009; Yuk Sing and Chongyu, 2007), deg-

radation by gamma rays (Yuk Sing and Chongyu, 2007),

Fenton (Wang and Lemley, 2002), treatment with UV /

H2O2 (APHA and WEF, 2005) and photocatalytic degra-

dation (Li et al. 2002, Kansal et al. 2007) have been used

to remove the diazinon.

The problems of these methods are including process

complexity, high cost and high consumption of chemi-

cals. However, the nano photocatalytic method has

rarely applied. In general, common physical techniques

such as  occulation, aeration, adsorption on activated

carbon and reverse osmosis may effectively remove the

contaminants; however, these methods are not able to

destroy the pollutants and contaminants from water

and they only can transfer these pollutants to another

phase and this is led to the formation of a secondary

environmental pollution which it is casused to require

retreatment and increase total cost. Photocatalyst is an

advanced oxidation technology with bright future and

it has been utilized in Usa, Europe and Japan in order

to purify the water of pollutants (Ugurlu and Karaoglu,

2009). Advanced oxidation processes produce a strong

oxidizing agent (hydroxyl radicals) that they destroy

the pollutants in wastewater completely (Mesgari et al.

2012).

One of the chief wastewater treatment process tech-

nologies is the photocatalysts and semiconductor that

have been shown to be potentially useful for the treat-

ment of wastewater contaminants (Liu et al. 2005;

Mekprasart, 2011). Among the various semiconductor

materials (oxides, sul des ), TiO2 has gained more popu-

larity and attention due to high Photocatalytic activity,

chemical stability, resistant against optical corrosion,

economic acceptability, cost-effectiveness and lack of

toxicity (Zhou et al. 2006; Sun et al. 2009). Although

the ef ciency of TiO2 with relatively high energy band

gap (3.2eV) has limited, but various methods such as

increasing surface to volume ratio, connecting TiO2

to other semiconductor particles, splashing of various

types of TiO2 into the zeolite pores and doping the metal

and non-metal ions with TiO2 have been developed to

increase the photocatalysis activity of TiO2 particles (Zhu

et al. 2006). The conductive ion metals can lead to the

formation of doped energy level between the conduc-

tion and valence bands of TiO2 which it has identi ed

as an effective way for increasing of the Photocatalytic

activity of TiO2. Moreover, the doped ions may be act

as electrons or holes traps and they boost the catalytic

activity of TiO2 (Liu and Chen, 2009). Previous studies

have clari ed that the transition metal ions, e.g Fe+3

can be utilized to increase the Photocatalytic activity

(

Rezaei kalanteri et al. 2014; Fadaei and Sadeghi, 2013).

Metal ions Fe+3 can be easily accommodated among

TiO2 network due to half- lled electron con gurations

and with an ionic radius close to the ionic radius of Ti+4

(Sorouri Zanjani et al. 2009) and it is caused to increase

the photocatalytic activity in the visible light region. In

addition, Fe+3 ions can create a surface trap on TiO2

network for electrons and holes arising from radiation,

thereby it can increase Kvantayy ef ciency and pho-

tocatalytic activity by reducing the recombination of

generated electrons and holes. Thus, Fe+3 ions are con-

sidered as a striking doping factor (

Rezaei kalanteri et al.

2014, Samadi et al. 2010).

For many years, the mankind uses the various types of

chemicals to eliminate the pets. This material has brought

severe and irreparable damage to nature, environmental

health, balance and stability of ecosystems and living

creatures (Balschmiter et al. 1983). A part of pollutants

such as organic material are often degraded through the

biological processes but other materials such as pesti-

cides are resistant against degradation and remain in

the aquatic environment for a long time (EsmailiSari,

2001). Organophosphates, as a group of pesticides, were

replaced with organochlorine a few decades ago due

to their lesser resistant and stability (Girón-Pérez et al.

2007). These poisons are capable to create serious effect

on non-target animals such as invertebrates, mammals,

birds and  sh due to widespread distribution in the

aquatic environment (Vandergeest et al. 1997; Castano

et al. 1986). The exposure of  shes with fatal doses of

diazinon is caused to anemia (Anees et al. 1978), reduc-

tion of DNA, RNA and protein in the liver (Ansari, 1988),

effect on the nervous system, the anomaly in the gills,

increasing the amount of macrophages and the effect

on the reproductive behavior (Dutta and Maxwell,

2003). Diazinon is partially soluble in water (40 mg/L

at 25°C); non-polar and resistant against degradation

in soil (APHA and WEF, 2005) which its characteristics

are given in Table 1. Unlike to chlorinated pesticides,

they have not accumulative nature in the body and are

faster degraded in the environment (Shemer and Linden,

2006).

Diazinon is one of the Organophosphate insecticides

which are classi ed as relatively dangerous materials

(Class II by the World Health Organization). It makes

toxicity for aquatic organisms at a concentration of

350 ng/l (Li et al. 2002), and its LC50 for  sh is 4.4

ppm (Zhang and Pehkonen, 1999). More than 13 mil-

lion pounds of diazinon are annually used in the United

States (10). Thus, the releasing of this compound into

the groundwater is one of the major concerns. The toxic

effect of Diazinon, like other organic phosphorus pesti-

BIOSCIENCE BIOTECHNOLOGY RESEARCH COMMUNICATIONS INVESTIGATION OF PHOTOCATALYTIC DEGRADATION OF DIAZINON USING TITANIUM DIOXIDE 61

MohammadMehdiBaneshi et al.

FIGURE 1. Schematic of reactor used in the process

(1) Trans of lamp 150 watt, (2) glass reactor, (3) cool-

ing water, (4) Magnet (5) magnetic stirrer (6) reac-

tor doors, (7) UV lamp 150 watt medium pressure (8)

covering quartz, (9) pump, (10) the water tank (11)

pipes for water.

cides, is to stop the acetylcholinesterase (Li et al. 2002,

Zhang and Pehkonen, 1999). It was also reported that

diazinon has a negative effect on the immune system

(Immunotoxic), cells (Cytotoxic) and genes (Genotoxic)

(Mahmoodi et al. 2007).

Since the diazinon is the most widely use and danger-

ous pesticides for the environment, especially aquatic

organisms, thus, the aim of this study was to determine

the ef ciency of photocatalytic degradation of diazinon

using titanium dioxide nanoparticles doped with iron in

the presence of ultraviolet light is the aqueous medium.

The most conducted studies in Iran have revealed

that the concentration of diazinon in the water is more

than standard levels. Shaeghi et al has found that the

diazinon concentration in Gharehsou and Gorgan riv-

ers in Golestan province was 22.4ppm and 6.74ppm,

respectively which it was higher than the standard lev-

els (

Daneshvar, 2007). Khazaeii and colleagues has also

observed that the concentration of diazinon in a number

of water samples was higher than standard levels (Wu,

2009

MATERIALS AND METHODS

In this study, a reactor made of Pyrex with the overall

volume of 2.7 liters was used. The diameter and height

of this reactor was 14 cm and 18 cm, respectively. A

medium pressure Lamp UV (125 watt, length of 12 cm

and a diameter of 1 cm and coating quartz with exter-

nal diameter of 2.5cm, internal diameter of 2 cm and a

length of 12.5 cm) has been installed in the middle of the

reactor lid made of multilayer aluminum foil. There was

another hole on the reactor lid which it was for sampling

and it was covered during the process. The maximum

wavelength emitted by the UV lamps was 247.3 nm and

in UV-C range. The reactor was covered by aluminum

foil to protect against the radiation. Mixing in the reac-

tor was carried out using a magnetic stirrer and magnet.

Free height of 5.5 cm inside the reactor was intended

to move the magnet. Samples with different concentra-

tions of diazinon, which was prepared by diluting the

diazinon 60 percent, were entered into the reactor and

the samples were taken under different conditions and

at different times.

The detection of diazinon level was performed by

reverse phase method of high performance liquid chro-

matography (HPLC). Chromatographic conditions were

as following: mobile phase of methanol + water was

applied at a ratio of 70:30 and C18 was used as the col-

umns. The determination of dizazinon level was per-

formed with a UV detector at 220 nm. Diazinon was

prepared from Sigma-Aldrich CO, USA. A hanger radi-

ometer instrument (ECL-X model) which it was to meas-

ure the intensity of light in UV-C range was utilized to

determine the intensity of the lamp UV125 watt medium

pressure used in reactors radiation. Intensity of lamps

were measured and controlled in half the diameter of the

reactor (about 7 cm) at different times.

The formula for calculating the radiation intensity:

D=L ×T T: time (s) L: radiation intensity (mw/s/cm2)

The diazinon removal percentage is calculated by fol-

lowing equation:

Where C0 and C are the initial and  nal concentration of

Diazinon, respectively.

Test method and statistical analysis

Samples were taken in different states from the reac-

tor and were centrifuged at 4000 rpm for 30 minutes

and then were  ltered with a 0.23μm  lter to remove

particles of TiO2. The DX8 and SPSS V.16 software and

the ANOVA test were applied for design of experiments,

drawing graphs and statistical analysis of results and

LSD POST HOC was used to distinguish between differ-

ent modes. Also, DX8 software was used to determine

the optimal mode and model.

Nanoparticle characterization

Fig 2&3 depict the SEM images and diameter distri-

bution of TiO2 nanoparticles before doping with Fe,

respectively. The diameter measurement of nanoparticles

was performed with the Measurement software and their

average diameter was determined and it is approved that

they are nanoparaticles. In this case, the average diam-

eter of the nanoparticles was determined to be 42.4 nm.

62 INVESTIGATION OF PHOTOCATALYTIC DEGRADATION OF DIAZINON USING TITANIUM DIOXIDE BIOSCIENCE BIOTECHNOLOGY RESEARCH COMMUNICATIONS

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FIGURE 2. SEM images of nanoparticles

FIGURE 3. The diameter distribution of nanoparticle

In addition, Fig 4&5 are related to the SEM images

and diameter distribution of the doped TiO2 nanoparti-

cles with Fe, respectively. The average diameter of nano-

particle was obtained to be 37.89 nm. The comparison

of the Fig 2 and Fig 4 show that the doped nanoparti-

cle structure is smaller while it was bulky before dop-

ing. Furthermore, it was clari ed that the average size

of doped nanoparticles (Fig5) is smaller than un-doped

nanoparticles (Fig 3).

FIGURE 4. SEM images of Fe-TiO2 nanoparticles

To obtain the optimum pH, the experiments were

conducted in different pH (3, 5, 7, 9, 11) while other

parameters including time, Diazinon concentration and

nanoparticle dose were kept constant. The results are

presented in  g 7. The results clarify that the maximum

removal ef ciency was achieved to be 97.52% at pH=7

and therefore, this pH was considered as optimum pH for

next experiments. It is also observed that the removal

ef ciency was decreased at the pH<5 and pH>9.

The X-ray diffraction pattern (XRD) for doped TiO2

nanoparticles with Fe is represented in Fig 6. The

observed peaks (maximum peak at 250) in XRD pattern

indicates that TiO2 doped with Fe has Anatase structure.

Strong peaks at 27, 36 and 55 degrees are indica-

tive of TiO2 in the rutile phase. On the other hand

strong peaks at 25 and 48 degrees is represented TiO2

is in anatase. The Fig 6 shows that highest amounts are

related to anatase phase while rutile phase exists with

anatase phase, heterogeneously. Titanium dioxide can be

observed in 3 forms including Anatase, Rutile and Bru-

cite which anatase and rutile have light catalytic activ-

ity. The Anatase shows more light activity than Rutile;

thus, it is more applicable.

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MohammadMehdiBaneshi et al.

FIGURE 5. The diameter distribution of Fe-TiO2 nanoparticle

FIGURE 6. X-ray diffraction pattern for TiO2 nanoparticles doped with Fe

FIGURE 7. The effect of pH on diazinon removal ef ciency

(time= 60 min, diazinon concentration = 50 mg/L, nano-

particle dosage=100 mg/L)

To determine the optimum time, the studied param-

eter were kept constant except the time. It was varied

from 5 to 90 min. it was observed that best removal ef -

ciencies was obtained in 60, 75 and 90 min. the removal

ef ciency percentage in 60, 70 and 90 min was obtained

to be 98.57%, 98.06% and 98.66%, respectively. In

this study, 60 min was selected as optimum time. The

obtained results were presented in  g 8.

The optimum diazinon concentration was determined

by keeping constant of the pH, time and nanoparticle

dose and the varying of the diazinon concentration in

range of 1-100 mg/L. The highest removal ef ciency was

related to diazinon concentration of 50 mg/L (97.52%)

and 25mg/L (97. 40%). It is clear that the removal

ef ciency for 50 mg/L is slightly more than 25mg/L;

thus the 50 mg/L was accepted as optimum diazinon

concentration. The results of this section are shown

in Fig 9.

The optimum dose of nanoparticle was determined

by varying the nanoparticle doses between 50-300

mg/L and keeping constant of other parameters. The

best results were observed in the dosage of 100 mg/l

(97.52%), 150mg/L (98.16%) and 200 mg/L (98.58%).

Since there is no signi cance difference in diazinon

removal ef ciency in mentioned concentrations; there-

fore, there the nanoparticle dosage of 100 mg/L were

selected as optimum dose. The results are shown in

 g 10.

64 INVESTIGATION OF PHOTOCATALYTIC DEGRADATION OF DIAZINON USING TITANIUM DIOXIDE BIOSCIENCE BIOTECHNOLOGY RESEARCH COMMUNICATIONS

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FIGURE 8. The effect of time on diazinon removal ef ciency (pH=7, diazinon concentration

= 50 mg/L, nanoparticle dosage=100 mg/L)

FIGURE 9. The effect of diazinon concentration on diazinon removal ef -

ciency (time= 60, pH=7, nanoparticle dosage=100 mg/L)

FIGURE 10. The effect of nanoparticle dosage on diazinon removal

ef ciency (time = 60, pH=7, diazinon concentration = 50mg/L)

DISCUSSION AND CONCLUSION

In the present study, photocatalytic decomposition of

diazinon using TiO2 nanoparticles doped with iron in the

presence of ultraviolet rays from the aqueous medium

was studied. In addition, the effect of different param-

eters including pH, dose of TiO2 nanoparticles doped

with iron, reaction time and concentration of diazinon

was discussed.

The results indicated that the increasing of pH,

decreasing of the diazinon concentration and increas-

ing of time is resulted in higher removal ef ciencies.

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MohammadMehdiBaneshi et al.

Best pH for diazinon removal is obtained to be in neu-

tral range and t pH of 7 which it is in accordance with

Merabat study (2009); in his study, the photocatalytic

decomposition of Indole was evaluated and the optimum

ph was found to be in range of 6-7.

Daneshvar et al (2007) has investigated the photo-

catalytic decomposition of diazinon with UV-C/ZNO

and the results indicated that the 80 min is required

to remove 80% of diazinon; it shows that the results

of present work is better than their results because the

optimum time of present work is 60 min. furthermore,

the results showed that the best dosage of nanoparti-

cles to obtain the highest removal rate was 100 mg/L in

addition, 50 mg/L of diazinon was selected as optimum

concentration. Zhang et al. (2011) has neeb reported that

TiO2 is effective on photocatalytic removal process that

it is agreed with the results of present study. According

to the results, the TiO2 dosage and contact time have

positive role on diazinion removal ef ciency.

Bazrafashan et al (2007) has found that higher elec-

trical potential or contact time is needed to remove the

higher concentration of diazinon. For any speci ed time,

the removal ef ciency has signi cantly increased by

increasing the voltage. The highest Electrical potential

(40 V) was led to fastest treatment with an over 99% of

removal ef ciency of diazinon after 60 minutes which it

is consistent with present study. The removal ef ciency

was 97.52% after optimum time of 60 min.

Diazinon is one of widely used as well as most

dangerous pesticides for environment and especially

aquatic organisms. The photocatalytic processes have

high capacity in removal and effective mineralization of

diazinon. Besides, the TiO2 nanoparticles can effectively

use to remove the toxic pollutants in various industries

because they are not toxic; thus, the doped nanoparti-

cle can be used as a suitable alternative to remove the

diazinon due to small amounts of nano-materials, low

energy consumption and high ef ciency.

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