PHOTOCATALYTIC DEGRADATION OF METRONIDAZOLE USING BIOI–MWCNT COMPOSITES: SYNTHESIS, CHARACTERIZATION, AND OPERATIONAL PARAMETERS

Davoud Balarak; Chinenye Adaobi Igwegbe; Pius Chukwukelue Onyechı

PHOTOCATALYTIC DEGRADATION OF METRONIDAZOLE USING BIOI–MWCNT COMPOSITES: SYNTHESIS, CHARACTERIZATION, AND OPERATIONAL PARAMETERS

Abstract

This study centers on the application of photocatalytic process using supported bismuth (III) oxyiodide–multi-walled carbon nanotube (BiOI–MWCNT) composites for the elimination of Metronidazole (MNZ) from its solution. The characteristics of BiOI and synthesized BiOI–MWCNTs composites were analyzed via the scanning electronic microscopy (SEM), X-ray diffraction (XRD), and transmission electron microscopy (TEM). The photocatalytic study was performed to evaluate the effect of UV (8, 15, 30, and 125 W), irradiation time (10–90 min), pH (5-9), initial MNZ concentration (10-100 mg/L) and BiOI–MWCNTs dosage (0.3–1.2 g/L) on MNZ removal at fixed neutral pH of 7. MNZ concentration was examined via the HPLC by measuring at 348 nm. Higher MNZ degradation was achieved using both BiOI–MWCNTs and UV light than using each separately. Maximum MNZ degradation efficiency of 99.95 % was obtained at pH 7, BiOI–MWCNTs dosage of 0.6g/L, MNZ concentration of 10mg/L, and irradiation time of 90min. MNZ removal was increased by increasing irradiation time and decreasing initial MNZ concentration. Pseudo-first-order rate of reaction (K) based on the Langmuir-Hinshelwood (L-H) model and adsorption equilibrium constant of 1.629 mg/L.min and 0.044 L/mg, respectively were obtained. Also, the adsorption kinetic study fitted the pseudo-first-order reaction. The electrical energy consumption per order of magnitude (E) for MNZ degradation was lower for the UV/BiOI–MWCNTs process than the BiOI–MWCNTs- alone and UV- alone processes. The photocatalytic degradation process using BiOI–MWCNTs can be applied efficiently for the removal of MNZ from aqueous solutions.

Keywords

References

[1] Balarak D., Azarpira H., (2016) Photocatalytic degradation of Sulfamethoxazole in water: investigation of the effect of operational parameters, International J. ChemTech Res. 9, 731-8.
[2] Ahmadi S., Banach A., Kord Mostafapour F., (2017) Study survey of cupric oxide nanoparticles in removal efficiency of ciprofloxacin antibiotic from aqueous solution: Adsorption isotherm study, Desal. Water Treat. 89, 297-303.
[3] Balarak D., Azarpira H., Mostafapour F.K., (2016) Study of the Adsorption Mechanisms of Cephalexin on to Azolla Filiculoides, Der Pharma Chemica 8, 114-121.
[4] Liu Z., Xie H., Zhang J., Zhang C., (2012) Sorption removal of cephalexin by HNO3 and H2O2 oxidized activated carbons, Sci. China Chem. 55, 1959–67.
[5] Liu H., Liu W., Zhang J., Zhang C., Ren L., Li Y., (2011) Removal of cephalexin from aqueous solution by original and Cu (II)/Fe (III) impregnated activated carbons developed from lotus stalks kinetics and equilibrium studies, J. Hazard Mater. 185, 1528–35.
[6] Yu F., Li Y., Han S., Jie Ma J., (2016) Adsorptive removal of antibiotics from aqueous solution using carbon Materials, Chemosphere 153, 365–385.
[7] Mohammadi A.S., Yazdanbakhsh A.R., Sardar M., (2013) Chemical oxygen demand removal from synthetic wastewater containing non-beta lactam antibiotics using advanced oxidation processes: A comparative study, Arch. Hyg. Sci. 2, 23-30.
[8] Rahdar S., Rahdar A., Igwegbe C.A., Moghaddam F., Ahmadi S., (2019) Synthesis and physical characterization of nickel oxide nanoparticles and its application study in the removal of ciprofloxacin from contaminated water by adsorption: Equilibrium and kinetic studies, Desal. Water Treat. 141, 386–393.

[9] Balarak D., Azarpira H., (2016) Rice husk as a biosorbent for antibiotic metronidazole removal: isotherm studies and model validation, International Journal of ChemTech Research 9, 566-573.
[10] Azarpira H., Mahdavi Y., Khaleghi O., (2016) Thermodynamic studies on the removal of metronidazole antibiotic by multi-walled carbon nanotubes, Der Pharmacia Lettre 8, 107-13.
[11] Shemer H., Kunukcu Y.K., Linden K.G., (2006) Degradation of the pharmaceutical Metronidazole via UV, Fenton and photo-Fenton processes, Chemosphere 63, 269-276.
[12] Farzadkia M., Esrafili A., Yang J.K., Siboni M.S., (2015) Photocatalytic degradation of Metronidazole with illuminated TiO2 nanoparticles, Journal of Environmental Health Science and Engineering 13, 35-44.
[13] Zhang W., He G., Gao P., Chen G., (2003) Development and characterization of composite nanofiltration membranes and their application in concentration of antibiotic, Sep. Purif. Technol. 30, 27–35.
[14] Gao J., Pedersen J.A., (2005) Adsorption of sulfonamide antimicrobial agents to clay minerals, Environ. Sci. Technol. 39, 9509-16.
[15] Peterson J.W., Petrasky L.J., Seymourc M.D., Burkharta R.S., Schuilinga A.B., (2012) Adsorption and breakdown of penicillin antibiotic in the presence of titanium oxide nanoparticles in water, Chemosphere 87, 911–7.
[16] Rahdar S., Igwegbe C.A., Rahdar A., Ahmadi S., (2018) Efficiency of sono-nano-catalytic process of magnesium oxide nanoparticle in removal of penicillin G from aqueous solution, Desalin. Wat. Treat. 106, 330–335.
[17] Homem V., Santos L., (2011) Degradation and removal methods of antibiotics from aqueous matrices-A review, J. Environ. Manage. 92, 2304-2347.
[18] Yoosefian M., Ahmadzadeh S., Aghasi M., Dolatabadi M., (2017) Optimization of electrocoagulation process for efficient removal of ciprofloxacin antibiotic using iron electrode; kinetic and isotherm studies of adsorption, J. Mole. Liq. 225, 544-553.
[19] Ghauch A., Tuqan A., Abou A.H., (2009) Antibiotic removal from water: Elimination of amoxicillin and ampicillin by microscale and nanoscale iron particles. Environ Pollut. 157, 1626–1635.
[20] Alexy R., Kumpel T., Kummerer K., (2004) Assessment of degradation of 18 antibiotics in the closed bottle test, Chemosphere 57, 505–512.
[21] Carabineiro A., Thavorn-Amornsri T., Pereira F., Figueiredo L., (2011) Adsorption of ciprofloxacin on surface modified carbon materials, Water Res. 45, 4583-91.
[22] Peng X., Hu F., Dai H., Xiong Q., (2016) Study of the adsorption mechanism of ciprofloxacin antibiotics onto graphitic ordered mesoporous carbons, Journal of the Taiwan Institute of Chemical Engineers 8, 1–10.
[23] Balarak D., Azarpira H., Mostafapour F.K., (2016) Adsorption isotherm studies of tetracycline antibiotics from aqueous solutions by maize stalks as a cheap biosorbent, International Journal of Pharmacy & Technology 8, 16664-75.
[24] Mahvi A.H., Mostafapour F.K., (2018) Biosorption of tetracycline from aqueous solution by Azolla filiculoides: equilibrium, kinetic and thermodynamics studies, Fresenius Environmental Bulletin 27, 5759-5767.
[25] Balarak D., Mostafapour F., Bazrafshan E., Saleh T.A., (2017) Studies on the adsorption of amoxicillin on multi-wall carbon nanotubes, Water Science and Technology 75, 1599-1606.
[26] An T., Yang H., Li G., Song W., Nie X., (2010) Kinetics and mechanism of advanced oxidation processes (AOPs) in degradation of ciprofloxacin in water, Applied Catalysis B: Environmental 94, 288–94.
[27] Fairooz N.Y., (2016) Evaluation of new couple Nb2O5/Sb2O3 oxide for photocatalytic degradation of Orange G dye, International Journal of ChemTech Research 9, 456-61.
[28] Hayat K., Gondal M.A., Khaled M.M., Ahmed S., Shemsi A.M., (2011) Nano ZnO synthesis by modified sol gel method and its application in heterogeneous photocatalytic removal of phenol from water, Applied Catalysis A: General 393, 122–29.
[29] Fan J., Hu X., Xie Z., Zhang K., Wang J., (2012) Photocatalytic degradation of azo dye by novel Bi-based photocatalyst Bi4TaO8I under visible-light irradiation, Chem. Eng. J. 179, 44–51.
[30] Ahmadi S., Igwegbe C.A., Rahdar S., (2009) The application of thermally activated persulfate for degradation of Acid Blue 92 in aqueous solution, Int. J. Ind. Chem.
[31] Asahi R., Morikawa T., Ohwaki T., Aoki K., Taga Y., (2011) Visible-light Photocatalysis in nitrogen-doped titanium oxides. Science 293, 269–71.
[32] Karuppuchamy S., Kumar R. D., (2015) Synthesis and characterization of visible light active titanium dioxide nanomaterials for photocatalytic applications, International Journal of ChemTech Research 8, 287-83.
[33] Su M., He C., Zhua L., Sun Z., Shan C., Zhang Q., (2012) Enhanced adsorption and photocatalytic activity of BiOI–MWCNT composites towards organic pollutants in aqueous solution, J. Hazard. Mater. 229–230, 72– 82.
[34] Xia J., Yin S., Li H., Xu H., Yan Y., Zhang Q., (2010) Self-assembly and enhanced photocatalytic properties of BiOI hollow microspheres via a reactable ionic liquid, Langmuir 27, 1200-1206.
[35] Tettey K.E., Yee M.Q., Lee D., (2010) Photocatalytic and conductive MWCNT/TiO2 nanocomposite thin films, ACS Appl. Mater. Interfaces 2, 2646–2652.
[36] Li S., Hu S., Xu K., Jiang W., Liu J., Wang Z., (2017) A novel heterostructure of BiOI nanosheets anchored onto MWCNTs with excellent visible-light photocatalytic activity, Nanomaterials (Basel) 7, 22.
[37] Zhang X., Ai Z.H., Jia F.L., Zhang L.Z., (2008) Generalized one-pot synthesis, characterization, and photocatalytic activity of hierarchical BiOX nanoplate microspheres, J. Phys. Chem., C 112, 747–753.
[38] Igwegbe C. A., Ahmadi S., Rahdar S., Ramazani A., Mollazehi A.R., (2020) Efficiency comparison of advanced oxidation processes for ciprofloxacin removal from aqueous solutions: Sonochemical, sono-nano-chemical and sono-nano-chemical/persulfate processes, Environ. Eng. Res. 25(2), 178-185.
[39] Guettai N., Amar H., (2005) Photocatalytic oxidation of methyl orange in presence of titanium dioxide in aqueous suspension. Part II. Kinetics study, Desalination 185, 439-448.
[40] Seidmohammadi G.A., Torabi L., (2016) Removal of metronidazole using ozone activated persulfate from aqua solutions in presence of ultrasound, J. Mazandaran Univ. Med. Sci. 26, 160-173.
[41] Rivera-Utrilla J., Prados-Joya G., Sánchez- Polo M., Ferro-García M.A., Bautista-Toledo I., (2009) Removal of nitroimidazole antibiotics from aqueous solution by adsorption/bio-adsorption on activated carbon, J. Hazard. Mater. 170, 298-305.
[42] Wang W.-L., Wu Q.-Y., Wang Z.-M., Hu H.-Y., Negishi N., Torimura M., (2015) Photocatalytic degradation of the antiviral drug Tamiflu by UV-A/TiO2: Kinetics and mechanisms, Chemosphere 131, 41-47.
[43] Pino N.J., Palominos R.A., Mansilla H.D., (2010) Degradation of the antibiotic oxolinic acid by photocatalysis with TiO2 in suspension, Water Res. 44, 5158-5167.
[44] Liu Y., Gan X., (2009) Photoelectrocatalytic degradation of tetracycline by highly effective TiO2 nanopore arrays electrode, J. Hazard. Mater. 171, 678-683.
[45] Rodrigo A., Palominos A., (2009) Photocatalytic oxidation of the antibiotic tetracycline on TiO2 and ZnO suspensions, J. Catalysis Today 114, 100–105.
[46] Bu Q., Wang B., Huang J., Deng S., Yu G., (2013) Pharmaceuticals and personal care products in the aquatic environment in China: A review, J. Hazard. Mater. 262, 189-211.
[47] Yang L., Yu L.E., Ray M.B., (2008) Degradation of paracetamol in aqueous solutions by TiO2 photocatalysis, Water Res. 42, 3480-3488.
[48] Xekoukoulotakis N.P., Xinidis N., Chroni M., Mantzavinos D., Venieri D., Hapeshi E., (2010) UV-A/TiO2 photocatalytic decomposition of erythromycin in water: Factors affecting mineralization and antibiotic activity, Catalysis Today 151, 29-33.
[49] Anandan S., Kathiravan K., Murugesan V., Ikuma Y., (2009) Anionic (IO3) non-metal doped TiO2 nanoparticles for the photocatalytic degradation of hazardous pollutant in water, Catalysis Communications 10, 1014–19.
[50] Karthikeyan N., Narayanan V., Stephen A., (2015) Degradation of textile effluent using nanocomposite TiO2/SnO2 semiconductor photocatalysts, International Journal of ChemTech Research 8, 443-49.
[51] Muruganaadham M., Swaminathan M., (2004) Solar photocatalytic degradation of a reactive azo dye in TiO2-suspension, Solar Energy Mater. Solar Cells 81, 439–57.
[52] Hequet V., Gonzalez C., Cloirec P.L., (2001) Photochemical processes for atrazine degradation: methodological approach, Water Res. 35, 4253–60.
[53] Galindo C., Jacques P., Kalt A., (2000) Photodegradation of the aminoazobenzene acid orange 52 by three advanced oxidation processes: UV/H2O2, UV/TiO2 and VIS/TiO2, Journal of Photochemistry and Photobiology A: Chemistry 130, 35-47.
[54] Vaiano V., Sacco O., Sannino D., Ciambelli P., (2014) Photocatalytic removal of spiramycin from wastewater under visible light with N-doped TiO2 photocatalysts, Chem. Eng. J. 39, 42–50.
[55] Behnajady M.A., Modirshahla N., Hamzavi R., (2006) Kinetic study on photocatalytic degradation of C.I. Acid yellow 23 by ZnO photocatalyst, J. Hazard. Mater., 133, 226–232.
[56] Bansal P., Singh D., Sud D., (2010) Photocatalytic degradation of azo dye in aqueous TiO2 suspension: reaction pathway and identification of intermediates products by LC/MS, Sep. Purif. Technol. 72, 357–365.
[57] Chang X.F., Huang J., Tan Q.Y., Wang M., Ji G.B., Deng S.B., Yu G., (2009) Photocatalytic degradation of PCP-Na over BiOI nanosheets under simulated sunlight irradiation, Catal. Commun., 10, 1957–1961.
[58] Balarak D., Mostafapour F.K., (2019) Photocatalytic degradation of amoxicillin using UV/Synthesized NiO from pharmaceutical wastewater, Indonesian Journal of Chemistry 19, 211-218.
[59] El-Sayed G.O., Dessouki H.A., Jahin H.S., Ibrahiem S.S., (2014) Photocatalytic degradation of metronidazole in aqueous solutions by copper oxide nanoparticles, Journal of Basic and Environmental Sciences 1, 102–110.
[60] Hamzehzadeh A., Fazlzadeh M., Rahmani K., (2017) Efficiency of nano/persulfate process (NZVI/PS) in removing metronidazole from aqueous solution, J. Environ. Health Eng. 4, 307-320.

Details

Primary Language

English

Subjects

-

Journal Section

Research Article

Authors

Davoud Balarak This is me
0000-0003-3679-9726
Iran

Chinenye Adaobi Igwegbe This is me
0000-0002-5766-7047
Nigeria

Pius Chukwukelue Onyechı This is me
0000-0002-9612-4272
Nigeria

Publication Date

December 1, 2019

Submission Date

October 2, 2019

Acceptance Date

November 6, 2019

Published in Issue

Year 2019 Volume: 37 Number: 4

IZ

https://izlik.org/JA69MP53NC

Cite

RIS / Bibtex

APA

Balarak, D., Igwegbe, C. A., & Onyechı, P. C. (2019). PHOTOCATALYTIC DEGRADATION OF METRONIDAZOLE USING BIOI–MWCNT COMPOSITES: SYNTHESIS, CHARACTERIZATION, AND OPERATIONAL PARAMETERS. Sigma Journal of Engineering and Natural Sciences, 37(4), 1235-1249. https://izlik.org/JA69MP53NC

AMA

1.Balarak D, Igwegbe CA, Onyechı PC. PHOTOCATALYTIC DEGRADATION OF METRONIDAZOLE USING BIOI–MWCNT COMPOSITES: SYNTHESIS, CHARACTERIZATION, AND OPERATIONAL PARAMETERS. SIGMA. 2019;37(4):1235-1249. https://izlik.org/JA69MP53NC

Chicago

Balarak, Davoud, Chinenye Adaobi Igwegbe, and Pius Chukwukelue Onyechı. 2019. “PHOTOCATALYTIC DEGRADATION OF METRONIDAZOLE USING BIOI–MWCNT COMPOSITES: SYNTHESIS, CHARACTERIZATION, AND OPERATIONAL PARAMETERS”. Sigma Journal of Engineering and Natural Sciences 37 (4): 1235-49. https://izlik.org/JA69MP53NC.

EndNote

Balarak D, Igwegbe CA, Onyechı PC (December 1, 2019) PHOTOCATALYTIC DEGRADATION OF METRONIDAZOLE USING BIOI–MWCNT COMPOSITES: SYNTHESIS, CHARACTERIZATION, AND OPERATIONAL PARAMETERS. Sigma Journal of Engineering and Natural Sciences 37 4 1235–1249.

IEEE

[1]D. Balarak, C. A. Igwegbe, and P. C. Onyechı, “PHOTOCATALYTIC DEGRADATION OF METRONIDAZOLE USING BIOI–MWCNT COMPOSITES: SYNTHESIS, CHARACTERIZATION, AND OPERATIONAL PARAMETERS”, SIGMA, vol. 37, no. 4, pp. 1235–1249, Dec. 2019, [Online]. Available: https://izlik.org/JA69MP53NC

ISNAD

Balarak, Davoud - Igwegbe, Chinenye Adaobi - Onyechı, Pius Chukwukelue. “PHOTOCATALYTIC DEGRADATION OF METRONIDAZOLE USING BIOI–MWCNT COMPOSITES: SYNTHESIS, CHARACTERIZATION, AND OPERATIONAL PARAMETERS”. Sigma Journal of Engineering and Natural Sciences 37/4 (December 1, 2019): 1235-1249. https://izlik.org/JA69MP53NC.

JAMA

1.Balarak D, Igwegbe CA, Onyechı PC. PHOTOCATALYTIC DEGRADATION OF METRONIDAZOLE USING BIOI–MWCNT COMPOSITES: SYNTHESIS, CHARACTERIZATION, AND OPERATIONAL PARAMETERS. SIGMA. 2019;37:1235–1249.

MLA

Balarak, Davoud, et al. “PHOTOCATALYTIC DEGRADATION OF METRONIDAZOLE USING BIOI–MWCNT COMPOSITES: SYNTHESIS, CHARACTERIZATION, AND OPERATIONAL PARAMETERS”. Sigma Journal of Engineering and Natural Sciences, vol. 37, no. 4, Dec. 2019, pp. 1235-49, https://izlik.org/JA69MP53NC.

Vancouver

1.Davoud Balarak, Chinenye Adaobi Igwegbe, Pius Chukwukelue Onyechı. PHOTOCATALYTIC DEGRADATION OF METRONIDAZOLE USING BIOI–MWCNT COMPOSITES: SYNTHESIS, CHARACTERIZATION, AND OPERATIONAL PARAMETERS. SIGMA [Internet]. 2019 Dec. 1;37(4):1235-49. Available from: https://izlik.org/JA69MP53NC