Published December 17, 2021 | Version v1

Synthesis and characterization of ternary chitosan–TiO2–ZnO over graphene for photocatalytic degradation of tetracycline from pharmaceutical wastewater

  • 1. Petroleum University of Technology

Description

Various nanocomposites of TiO2–ZnO, TiO2–ZnO/CS, and TiO2–ZnO/CS–Gr with different molar ratios were synthesized by sol–gel and ultrasound-assisted methods and utilized under UV irradiation to enhance the photocatalytic degradation of tetracycline. Characterization of prepared materials were carried out by XRD, FT-IR, FE-SEM, EDX and BET techniques. The TiO2–ZnO with the 1:1 molar ratio supported with 1:2 weight ratio CS–Gr (T1‒Z1/CS1‒Gr2 sample) appeared as the most effective material at the optimized operational conditions including the tetracycline concentration of 20 mg/L, pH = 4, catalyst dosage of 0.5 g/L, and 3 h of irradiation time. As expected, the graphene had a significant effect in improving degradation results. The detailed performances of the T1‒Z1/CS1‒Gr2 were compared with ternary nanocomposites from EDX and BET results as well as from the degradation viewpoint. This novel photocatalyst can be effective in actual pharmaceutical wastewater treatment considering the applied operational parameters.

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References

  • Magnetic NiFe2O4 nanoparticles decorated on N-doped BiOBr nanosheets for expeditious visible light photocatalytic phenol degradation and hexavalent chromium reduction via a Z-scheme heterojunction mechanism Sin J.-C. , Lam S.-M. , Zeng H. ,... Lim J.-W. , Qin Z. Applied Surface ScienceOpen source preview, 2021 DOI: 10.1016/j.apsusc.2021.149966
  • Carbonaceous-TiO2 nanomaterials for photocatalytic degradation of pollutants: a review Khalid N.R. , Majid A. , Bilal Tahir M.B. , Niaz N.A. , Khalid S. Ceramics InternationalOpen source preview, 2017 DOI: 10.1016/j.ceramint.2017.08.143
  • Photocatalytic and antimicrobial activities of chitosan-TiO2 nanocomposite Karthikeyan K.T. , Nithya A. , Jothivenkatachalam K. International Journal of Biological MacromoleculesOpen source preview, 2017 DOI: 10.1016/j.ijbiomac.2017.03.121
  • Role of precursors on the photophysical properties of carbon nitride and its application for antibiotic degradation Panneri S. , Ganguly P. , Nair B.N. ,... Warrier K.G.K. , Hareesh U.N.S. Environmental Science and Pollution ResearchOpen source preview, 2017 DOI: 10.1007/s11356-017-8538-z
  • Degradation and removal methods of antibiotics from aqueous matrices: a review Homem V. , Santos L. Journal of Environmental ManagementOpen source preview, 2011 DOI: 10.1016/j.jenvman.2011.05.023
  • Photodegradation of pharmaceuticals and personal care products in water treatment using carbonaceous-TiO2 composites: a critical review of recent literature Awfa D. , Ateia M. , Fujii M. , Johnson M.S. , Yoshimura C. Water ResearchOpen source preview, 2018 DOI: 10.1016/j.watres.2018.05.036
  • Chitosan modified N, S-doped TiO2 and N, S-doped ZnO for visible light photocatalytic degradation of tetracycline Farhadian N. , Akbarzadeh R. , Pirsaheb M. ,... Fakhri Y. , Asadi A. International Journal of Biological MacromoleculesOpen source preview, 2019 DOI: 10.1016/j.ijbiomac.2019.03.217
  • Punica granatum mediated green synthesis of cauliflower-like ZnO and decorated with bovine bone-derived hydroxyapatite for expeditious visible light photocatalytic antibacterial, antibiofilm and antioxidant activities Sin J.-C. , Quek J. , Lam S.-M. ,... Mohamed A.R. , Lim J.-W. Journal of Environmental Chemical EngineeringOpen source preview, 2021 DOI: 10.1016/j.jece.2021.105736
  • Degradation of tetracycline antibiotics: mechanisms and kinetic studies for advanced oxidation/reduction processes Jeong J. , Song W. , Cooper W.J. , Jung J. , Greaves J. ChemosphereOpen source preview, 2010 DOI: 10.1016/j.chemosphere.2009.11.024
  • Photodegradation of tetracycline antibiotics in aqueous solution by UV/ZnO Wang H. , Yao H. , Pei J. , Liu F. , Li D. Desalination and Water TreatmentOpen source preview, 2015 DOI: 10.1080/19443994.2015.1103309
  • Enhanced photocatalytic degradation of tetracycline and real pharmaceutical wastewater using MWCNT/TiO2 nano-composite Ahmadi-Moghadam M. , Ramezani Motlagh H. , Jaafarzadeh Haghighifard N. ,... Barzegar G. , Jorfi S. Journal of Environmental ManagementOpen source preview, 2017 DOI: 10.1016/j.jenvman.2016.09.088
  • Environmental applications of titania-graphene photocatalysts Faraldos M. , Bahamonde A. Catalysis TodayOpen source preview, 2017 DOI: 10.1016/j.cattod.2017.01.029
  • Enhanced photocatalytic activity of graphene–TiO2 composite under visible light irradiation Khalid N.R. , Ahmed E. , Hong Z. , Sana L. , Ahmed M. Current Applied PhysicsOpen source preview, 2013 DOI: 10.1016/j.cap.2012.11.003
  • Mix and match metal oxides and nanocarbons for new photocatalytic frontiers Melchionna M. , Prato M. , Fornasiero P. Catalysis TodayOpen source preview, 2016 DOI: 10.1016/j.cattod.2016.04.024
  • Visible light-driven photocatalytic degradation of rhodamine B and industrial dyes (texbrite BAC-L and texbrite NFW-L) by ZnO-graphene-TiO2 composite Nuengmatcha P. , Chanthai S. , Mahachai R. , Oh W.-C. Journal of Environmental Chemical EngineeringOpen source preview, 2016 DOI: 10.1016/j.jece.2016.03.045
  • Crystallinity and lowering band gap induced visible light photocatalytic activity of TiO2/CS (Chitosan) nanocomposites Rajendran R. , Aviles J. , Gracia F. , Mosquera-Vargas E. , Gupta V.K. International Journal of Biological MacromoleculesOpen source preview, 2018 DOI: 10.1016/j.ijbiomac.2017.11.125
  • Preparation of HPW-CS/TiO2/FACS photocatalysts for degradation of tetracycline hydrochloride Yang J. , Zhu M. , Chu H. , Zhou H. , Xu Y. Materials TechnologyOpen source preview, 2017 DOI: 10.1080/10667857.2017.1311399
  • Visible light photocatalytic degradation of tetracycline over TiO2 Wu S. , Hu H. , Lin Y. , Zhang J. , Hu Y.H. Chemical Engineering JournalOpen source preview, 2020 DOI: 10.1016/j.cej.2019.122842
  • Enhanced visible light photocatalytic activity of copper-doped titanium oxide-zinc oxide heterojunction for methyl orange degradation Dorraj M. , Alizadeh M. , Sairi N.A. ,... Pei Meng P.M. , Alias Y. Applied Surface ScienceOpen source preview, 2017 DOI: 10.1016/j.apsusc.2017.04.045
  • Photocatalytic degradation of tetracycline by ZnO/γ-Fe2O3 paramagnetic nanocomposite material Semeraro P. , Bettini S. , Sawalha S. ,... Valli L. , Giancane G. NanomaterialsOpen source preview, 2020 DOI: 10.3390/nano10081458
  • RGO–TiO2–ZnO composites: synthesis, characterization, and application to photocatalysis Johra F.T. , Jung W.-G. Applied Catalysis A: GeneralOpen source preview, 2015 DOI: 10.1016/j.apcata.2014.11.036
  • Sol-gel synthesis of ternary CuO/TiO2/ZnO nanocomposites for enhanced photocatalytic performance under UV and visible light irradiation Taufik A. , Albert A. , Saleh R. Journal of Photochemistry and Photobiology A: ChemistryOpen source preview, 2017 DOI: 10.1016/j.jphotochem.2017.05.012
  • Mitigation of pollutants by chitosan/metallic oxide photocatalyst: a review Mohd Adnan M.A. , Bao L.P. , Julkapli N. Journal of Cleaner ProductionOpen source preview, 2020 DOI: 10.1016/j.jclepro.2020.121190
  • Ultrasound assisted preparation, characterization and adsorption study of ternary chitosan-ZnO–TiO2 nanocomposite: advantage over conventional method Bhanvase B.A. , Veer A. , Shirsath S.R. , Sonawane S.H. Ultrasonics SonochemistryOpen source preview, 2019 DOI: 10.1016/j.ultsonch.2018.11.003
  • The influence of titanium dioxide nanofiller ratio on morphology and surface properties of TiO2/chitosan nanocomposite Al-Taweel S.S. , Radhi Saud H.R. , Kadhum A.A.H. , Takriff M.S. Results in PhysicsOpen source preview, 2019 DOI: 10.1016/j.rinp.2019.102296
  • Graphene-based nanoarchitectures. Anchoring semiconductor and metal nanoparticles on a two-dimensional carbon support Kamat P.V. Journal of Physical Chemistry LettersOpen source preview, 2010 DOI: 10.1021/jz900265j
  • C–N–S tridoped TiO2 for photocatalytic degradation of tetracycline under visible-light irradiation Wang P. , Yap P.-S. , Lim T.-T. Applied Catalysis A: GeneralOpen source preview, 2011 DOI: 10.1016/j.apcata.2011.04.008
  • Preparation of chitosan coated zinc oxide nanocomposite for enhanced antibacterial and photocatalytic activity: as a bionanocomposite Bharathi D. , Rajamani R. , Chandar Shekar B. , Bhuvaneshwari V. International Journal of Biological MacromoleculesOpen source preview, 2019 DOI: 10.1016/j.ijbiomac.2019.02.061
  • Photocatalyst of TiO2/ZnO nano composite film: preparation, characterization, and photodegradation activity of methyl orange Tian J. , Chen L. , Yin Y. ,... Liu X. , Wu P. Surface and Coatings TechnologyOpen source preview, 2009 DOI: 10.1016/j.surfcoat.2009.07.008
  • Fabrication of TiO2/ZnO nanocomposites for solar energy driven photocatalysis Prasannalakshmi P. , Shanmugam N. Materials Science in Semiconductor ProcessingOpen source preview, 2017 DOI: 10.1016/j.mssp.2017.01.008
  • Heteropolyacid–chitosan/TiO2 composites for the degradation of tetracycline hydrochloride solution Yu X. , Lu Z. , Wu D. ,... Yan Y. , Feng Y. Reaction Kinetics, Mechanisms and CatalysisOpen source preview, 2014 DOI: 10.1007/s11144-013-0631-9
  • Investigation of nitrogen doped and carbon species decorated TiO2 with enhanced visible light photocatalytic activity by using chitosan Shao Y. , Cao C. , Chen S. ,... Li X. , Li D. Applied Catalysis B: EnvironmentalOpen source preview, 2015 DOI: 10.1016/j.apcatb.2015.05.023
  • Effective photocatalytic degradation of anthropogenic dyes using graphene oxide grafting titanium dioxide nanoparticles under UV-light irradiation Atchudan R. , Edison T.N. , Suguna S. , Karthikeyan D. , Lee Y.R. Journal of Photochemistry and Photobiology A: ChemistryOpen source preview, 2017 DOI: 10.1016/j.jphotochem.2016.10.021
  • Hydrothermal synthesis of multifunctional TiO2–ZnO oxide systems with desired antibacterial and photocatalytic properties Siwińska-Ciesielczyk K. , Kubiak A. , Piasecki A. ,... Ehrlich H. , Jesionowski T. Applied Surface ScienceOpen source preview, 2019 DOI: 10.1016/j.apsusc.2018.08.256
  • Direct solvothermal synthesis of zinc oxide nanoparticle decorated graphene oxide nanocomposite for efficient photodegradation of azo-dyes Atchudan R. , Edison T.N.J.I. , Suguna S. , Shanmugam M. , Lee Y.R. Journal of Photochemistry and Photobiology A: ChemistryOpen source preview, 2017 DOI: 10.1016/j.jphotochem.2017.01.021
  • Investigations on amphoteric chitosan/TiO2 bionanocomposites for application in visible light induced photocatalytic degradation Bahal M. , Kaur N. , Sharotri N. , Sud D. Advances in Polymer TechnologyOpen source preview, 2019 DOI: 10.1155/2019/2345631
  • Highly efficient removal of As(III) from aqueous solutions using goethite/graphene oxide/chitosan nanocomposite Shan H. , Peng S. , Zhao C. , Zhan H. , Zeng C. International Journal of Biological MacromoleculesOpen source preview, 2020 DOI: 10.1016/j.ijbiomac.2020.07.108
  • Graphene oxide functionalized chitosan-magnetite nanocomposite for removal of Cu(II) and Cr(VI) from waste water Anush S.M. , Hunsur Ravikumar H.R. , Gayathri B.H. ,... Vishalakshi B. , Kalluraya B. International Journal of Biological MacromoleculesOpen source preview, 2020 DOI: 10.1016/j.ijbiomac.2020.09.059
  • Highly efficient multifunctional graphene/chitosan/magnetite nanocomposites for photocatalytic degradation of important dye molecules Maruthupandy M. , Muneeswaran T. , Anand M. , Quero F. International Journal of Biological MacromoleculesOpen source preview, 2020 DOI: 10.1016/j.ijbiomac.2020.03.045
  • Magnetic graphene/chitosan nanocomposite: a promising nanoadsorbent for the removal of 2-naphthol from aqueous solution and their kinetic studies Rebekah A. , Govindan G. , Naushad M. , Viswanathan C. , Ponpandian N. International Journal of Biological MacromoleculesOpen source preview, 2020 DOI: 10.1016/j.ijbiomac.2020.05.113
  • Mechanistic of photocatalytic decolorization and mineralization of methyl orange dye by immobilized TiO2/chitosan-montmorillonite Bahrudin N.N. , Nawi M.A. Journal of Water Process EngineeringOpen source preview, 2019 DOI: 10.1016/j.jwpe.2019.100843
  • Photocatalytic degradation of tetracycline antibiotic using new calcite/titania nanocomposites Belhouchet N. , Hamdi B. , Chenchouni H. , Bessekhouad Y. Journal of Photochemistry and Photobiology A: ChemistryOpen source preview, 2019 DOI: 10.1016/j.jphotochem.2018.12.016
  • Removal of tetracycline from aqueous solution by a Fe3O4 incorporated PAN electrospun nanofiber mat Liu Q. , Zheng Y. , Zhong L. , Cheng X. Journal of Environmental Sciences (China)Open source preview, 2015 DOI: 10.1016/j.jes.2014.04.016
  • Sonocatalytic degradation of some dyestuffs and comparison of catalytic activities of nano-sized TiO2, nano-sized ZnO and composite TiO2/ZnO powders under ultrasonic irradiation Wang J. , Jiang Z. , Zhang L. ,... Xu R. , Zhang X. Ultrasonics SonochemistryOpen source preview, 2009 DOI: 10.1016/j.ultsonch.2008.08.005
  • Photocatalytic degradation of tetracycline in aqueous solution by nanosized TiO2 Zhu X.-D. , Wang Y.-J. , Sun R.-J. , Zhou D.-M. ChemosphereOpen source preview, 2013 DOI: 10.1016/j.chemosphere.2013.02.066
  • Carbon dots anchored high-crystalline g-C3N4 as a metal-free composite photocatalyst for boosted photocatalytic degradation of tetracycline under visible light Shi W. , Yang S. , Sun H. ,... Guo F. , Shi J. Journal of Materials ScienceOpen source preview, 2020 DOI: 10.1007/s10853-020-05436-2
  • Dual enhancement of capturing photogenerated electrons by loading CoP nanoparticles on N-deficient graphitic carbon nitride for efficient photocatalytic degradation of tetracycline under visible light Shi W. , Shu K. , Sun H. ,... Chen F. , Guo F. Separation and Purification TechnologyOpen source preview, 2020 DOI: 10.1016/j.seppur.2020.116930
  • Fabrication of ternary Ag3PO4/Co3(PO4)2/g-C3N4 heterostructure with following Type II and Z-Scheme dual pathways for enhanced visible-light photocatalytic activity Shi W. , Liu C. , Li M. ,... Guo F. , Shi J. Journal of Hazardous MaterialsOpen source preview, 2020 DOI: 10.1016/j.jhazmat.2019.121907
  • Wet chemically synthesized ZnO structures for photodegradation of pre-treated palm oil mill effluent and antibacterial activity Wong K.-A. , Lam S.-M. , Sin J.-C. Ceramics InternationalOpen source preview, 2019 DOI: 10.1016/j.ceramint.2018.10.078