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Enhanced dye-removal performance of Cu-TiO2-fly ash composite by optimized adsorption and photocatalytic activity under visible light irradiation

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Abstract

The performance of Cu/TiO2/FA composite, a hybrid adsorbent-photocatalyst consisting of copper-doped titania particles supported on fly ash, was optimized, under visible light irradiation, for the removal of the model dye pollutant methyl orange (MO) by using a response surface methodology and Box-Behnken experimental design. Three independent variables were considered for the optimization study: catalyst/solvent dosage (0.5 – 2.0 g/L), irradiation time (30–120 min), and the initial concentration (5– 25 ppm) of the dye. A 99.91% rate of removal was achieved using 2 g/L dosage, 5 ppm initial concentration, and 100 min of irradiation time as the optimal operating conditions. The recorded trends support the hypothesis of a combined and synergic adsorption-photocatalytic degradation process which fully exploits the “capture and destroy” approach for pollutant removal.

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References

  • Abidi M, Assadi AA, Bouzaza A, Hajjaji A, Bessais B, Rtimi S (2019) Photocatalytic indoor/outdoor air treatment and bacterial inactivation on CuxO/TiO2 prepared by HiPIMS on polyester cloth under low intensity visible light. Appl Catal B Environ 259:118074

    Article  CAS  Google Scholar 

  • Adriana Z (2008) Doped-TiO2: A Review. Recent Pat Eng 2:157–164

    Article  Google Scholar 

  • Aguilar T, Navas J, Alcántara R, Fernández-Lorenzo C, Gallardo JJ, Blanco G, Martín-Calleja J (2013) A route for the synthesis of Cu-doped TiO2 nanoparticles with a very low band gap. Chem Phys Lett 571:49–53

    Article  CAS  Google Scholar 

  • Ahmed ZT, Hand DW (2014) Quantification of the adsorption capacity of fly ash. Ind Eng Chem Res 53:6985–6989

    Article  CAS  Google Scholar 

  • Ali Z, Shah AU, Ali Z, Mahmood A (2020) Influence of Cu modified surface states by sol gel technique on photocatalytic activity of titanium dioxide. Mater Chem Phys 249:123169

  • Andriantsiferana C, Mohamed EF, Delmas H (2014) Photocatalytic degradation of an azo-dye on TiO2/activated carbon composite material. Environ Technol (United Kingdom) 35:355–363

    CAS  Google Scholar 

  • Andronic L, Isac L, Miralles-Cuevas S, Visa M, Oller I, Duta A, Malato S (2016) Pilot-plant evaluation of TiO2 and TiO2-based hybrid photocatalysts for solar treatment of polluted water. J Hazard Mater 320:469–478

    Article  CAS  Google Scholar 

  • Anwer H, Mahmood A, Lee J, Kim KH, Park JW, Yip ACK (2019) Photocatalysts for degradation of dyes in industrial effluents: opportunities and challenges. Nano Res 12:955–972

    Article  CAS  Google Scholar 

  • Arslan-Alaton I, Tureli G, Olmez-Hanci T (2009) Treatment of azo dye production wastewaters using photo-Fenton-like advanced oxidation processes: optimization by response surface methodology. J. Photochem. Photobiol. A: Chem 202:142–153

    CAS  Google Scholar 

  • Balık M, Bulut V, Erdogan IY (2019) Optical, structural and phase transition properties of Cu2O, CuO and Cu2O/CuO: their photoelectrochemical sensor applications. Int J Hydrog Energy 44:18744–18755

    Article  Google Scholar 

  • Baruah M, Supong A, Bhomick PC, Karmaker R, Pongener C, Sinha D (2020) Batch sorption–photodegradation of Alizarin Red S using synthesized TiO2/activated carbon nanocomposite: an experimental study and computer modelling. Nanotechnol Environ Eng 5:8(2020)

  • Carp O, Huisman CL, Reller A (2004) Photoinduced reactivity of titanium dioxide. Prog Solid State Chem 32:33–177

    Article  CAS  Google Scholar 

  • Chaudhary N, Balomajumder C (2014) Optimization study of adsorption parameters for removal of phenol on aluminum impregnated fly ash using response surface methodology. J Taiwan Inst Chem Eng 45:852–859

    Article  CAS  Google Scholar 

  • Chen D, Cheng Y, Zhou N, Chen P, Wang Y, Li K, Huo S, Cheng P, Peng P, Zhang R, Wang L, Liu H, Liu Y, Ruan R (2020) Photocatalytic degradation of organic pollutants using TiO2-based photocatalysts: a review. J Clean Prod 268:121725

  • Cheng JN, Zhao LZ, Li GB, Li F, Yao MM (2020) B/Co/Fe tridoped TiO2/SiO2 composite films for improved photocatalytic degradation of organic pollutants under visible light. Inorg Chem Commun 119:108089

  • Delsouz Khaki MR, Shafeeyan MS, Raman AAA, Daud WMAW (2018) Evaluating the efficiency of nano-sized Cu doped TiO2/ZnO photocatalyst under visible light irradiation. J Mol Liq 258:354–365

    Article  CAS  Google Scholar 

  • Dong H, Zeng G, Tang L, Fan C, Zhang C, He X, He Y (2015) An overview on limitations of TiO2-based particles for photocatalytic degradation of organic pollutants and the corresponding countermeasures. Water Res 79:128–146

    Article  CAS  Google Scholar 

  • Etacheri V, Di Valentin C, Schneider J, Bahnemann D, Pillai SC (2015) Visible-light activation of TiO2 photocatalysts: advances in theory and experiments. J Photochem Photobiol C: Photochem Rev 25:1–29

    Article  CAS  Google Scholar 

  • Ferreira SLC, Bruns RE, Ferreira HS, Matos GD, David JM, Brandão GC, da Silva EGP, Portugal LA, dos Reis PS, Souza AS, dos Santos WNL (2007) Box-Behnken design: an alternative for the optimization of analytical methods. Anal Chim Acta 597:179–186

    Article  CAS  Google Scholar 

  • Ganesh I, Kumar PP, Annapoorna I, Sumliner JM, Ramakrishna M, Hebalkar NY, Padmanabham G, Sundararajan G (2014) Preparation and characterization of Cu-doped TiO2 materials for electrochemical, photoelectrochemical, and photocatalytic applications. Appl Surf Sci 293:229–247

    Article  CAS  Google Scholar 

  • Gaya UI, Abdullah AH (2008) Heterogeneous photocatalytic degradation of organic contaminants over titanium dioxide: a review of fundamentals, progress and problems. J Photochem Photobiol C-Photochem Rev 9:1–12

    Article  CAS  Google Scholar 

  • Gilja V, Katancic Z, Krehula LK, Mandic V, Hrnjak-Murgic Z (2019) Eflciency of TiO2 catalyst supported by modified waste fly ash during photodegradation of RR45 dye. IEEE J Sel Top Quantum Electron 26:292–300

    CAS  Google Scholar 

  • Giwa A, Yusuf A, Balogun HA, Sambudi NS, Bilad MR, Adeyemi I, Chakraborty S, Curcio S (2021) Recent advances in advanced oxidation processes for removal of contaminants from water: A comprehensive review. Process Saf Environ Prot 146:220–256

    Article  CAS  Google Scholar 

  • Gopinath KP, Madhav NV, Krishnan A, Malolan R, Rangarajan G (2020) Present applications of titanium dioxide for the photocatalytic removal of pollutants from water: a review. J Environ Manag 270:110906

    Article  CAS  Google Scholar 

  • Jin Y, Wu Y, Cao J, Wu Y (2014) Optimizing decolorization of Methylene Blue and Methyl Orange dye by pulsed discharged plasma in water using response surface methodology. J Taiwan Inst Chem Eng 45:589–595

    Article  CAS  Google Scholar 

  • Joo Kim H, Raj Pant H, Hee Kim J, Jung Choi N, Sang Kim C (2014) Fabrication of multifunctional TiO2-fly ash/polyurethane nanocomposite membrane via electrospinning. Ceram Int 40:3023–3029

    Article  Google Scholar 

  • Jorfi S, Mirali S, Mostoufi A, Ahmadi M (2018) Visible light photocatalytic degradation of azo dye and a real textile wastewater using Mn, Mo, La/TiO2/ac nanocomposite. Chem Biochem Eng Q 32:215–227

    Article  CAS  Google Scholar 

  • Kanakaraju D, Wong SP (2018) Photocatalytic efficiency of TiO2 biomass loaded mixture for wastewater treatment. J Chemother 2018:4314969

    Google Scholar 

  • Kanakaraju D, Ravichandar S, Lim YC (2017) Combined effects of adsorption and photocatalysis by hybrid TiO2/ZnO-calcium alginate beads for the removal of copper. J Environ Sci (China) 55:214–223

    Article  CAS  Google Scholar 

  • Kanakaraju D, Shahdad NRBM, Lim YC, Pace A (2018a) Magnetic hybrid TiO2/Alg/FeNPs triads for the efficient removal of methylene blue from water. Sustain Chem Pharm 8:50–62

    Article  Google Scholar 

  • Kanakaraju D, Soon Pang W, Wan Abu Bakar WA (2018b) Photo-fenton treatment of sago wastewater: RSM optimization and toxicity evaluation. J Teknol 80:153–163

    Google Scholar 

  • Kanakaraju D, Bin Ya MH, Lim YC, Pace A (2020) Combined Adsorption/Photocatalytic dye removal by copper-titania-fly ash composite. Surf Interfaces 19:100534

  • Kaushik P, Malik A (2011) Process optimization for efficient dye removal by Aspergillus lentulus FJ172995. J Hazard Mater 185:837–843

    Article  CAS  Google Scholar 

  • Khosravi M, Arabi S (2016) Application of response surface methodology (RSM) for the removal of methylene blue dye from water by nano zero-valent iron (NZVI). Water Sci Technol 74:343–352

    Article  CAS  Google Scholar 

  • Körbahti BK, Tanyolaç A (2008) Electrochemical treatment of simulated textile wastewater with industrial components and Levafix Blue CA reactive dye: optimization through response surface methodology. J Hazard Mater 151:422–431

    Article  Google Scholar 

  • Kumaravel V, Mathew S, Bartlett J, Pillai SC (2019) Photocatalytic hydrogen production using metal doped TiO2: a review of recent advances. Appl. Catal. B: Environ 244:1021–1064

    CAS  Google Scholar 

  • Luévano-Hipólito E, Torres-Martínez LM, Cantú-Castro LVF (2019) Self-cleaning coatings based on fly ash and bismuth-photocatalysts: Bi2O3, Bi2O2CO3, BiOI, BiVO4, BiPO4. Constr Build Mater 220:206–213

    Article  Google Scholar 

  • Moztahida M, Lee DS (2020) Photocatalytic degradation of methylene blue with P25/graphene/polyacrylamide hydrogels: optimization using response surface methodology. J Hazard Mater 400:123314

    Article  CAS  Google Scholar 

  • Muhd Julkapli N, Bagheri S, Bee Abd Hamid S (2014) Recent advances in heterogeneous photocatalytic decolorization of synthetic dyes. Sci World J 2014:Article ID 692307

  • Najafi H, Farajfaed S, Zolgharnian S, Mosavi Mirak SH, Asasian-Kolur N, Sharifian S (2021) A comprehensive study on modified-pillared clays as an adsorbent in wastewater treatment processes. Process Saf Environ Prot 147:8–36

    Article  CAS  Google Scholar 

  • Pant B, Ojha GP, Kim HY, Park M, Park SJ (2019) Fly-ash-incorporated electrospun zinc oxide nanofibers: potential material for environmental remediation. Environ Pollut 245:163–172

    Article  CAS  Google Scholar 

  • Pava-Gómez B, Vargas-Ramírez X, Díaz-Uribe C (2018) Physicochemical study of adsorption and photodegradation processes of methylene blue on copper-doped TiO2 films. J. Photochem. Photobiol. A: Chem 360:13–25

    Google Scholar 

  • Pedroza-Herrera G, Medina-Ramírez IE, Lozano-Álvarez JA, Rodil SE (2020) Evaluation of the photocatalytic activity of copper doped TiO2 nanoparticles for the purification and/or disinfection of industrial effluents. Catal Today 341:37–48

    Article  CAS  Google Scholar 

  • Qian S, Pu S, Zhang Y, Wang P, Bai Y, Lai B (2021) New insights on the enhanced non-hydroxyl radical contribution under copper promoted TiO2/GO for the photodegradation of tetracycline hydrochloride. J Environ Sci (China) 100:99–109

    Article  Google Scholar 

  • Reza KM, Kurny ASW, Gulshan F (2017) Parameters affecting the photocatalytic degradation of dyes using TiO2: a review. Appl Water Sci 7:1569–1578

    Article  CAS  Google Scholar 

  • Rtimi S, Pulgarin C, Robyr M, Aybush A, Shelaev F, Gostev F, Nadtochenko V, Kiwi J (2017) Insight into the catalyst/photocatalyst microstructure presenting the same composition but leading to a variance in bacterial reduction under indoor visible light. Appl. Catal. B: Environ 208:135–147

    CAS  Google Scholar 

  • Shafei A, Sheibani S (2019) Visible light photocatalytic activity of Cu doped TiO2-CNT nanocomposite powder prepared by sol–gel method. Mater Res Bull 110:198–206

    Article  CAS  Google Scholar 

  • Shan R, Lu L, Gu J, Zhang Y, Yuan H, Chen Y, Luo B (2020) Photocatalytic degradation of methyl orange by Ag/TiO2/biochar composite catalysts in aqueous solutions. Mater Sci Semicond Process 114:105088

    Article  CAS  Google Scholar 

  • Shijitha T, Baiju KV, Shukla S, Patil K, Warrier KGK (2009) Novel electroless process for copper coating of flyash using titania/ultraviolet-radiation/metal catalyst-system. Appl Surf Sci 255:6696–6704

    Article  CAS  Google Scholar 

  • Talebi S, Chaibakhsh N, Moradi-Shoeili Z (2017) Application of nanoscale ZnS/TiO2 composite for optimized photocatalytic decolorization of a textile dye. J Appl Res Technol 15:378–385

    Article  Google Scholar 

  • Visa M, Bogatu C, Duta A (2015a) Tungsten oxide - fly ash oxide composites in adsorption and photocatalysis. J Hazard Mater 289:244–256

    Article  CAS  Google Scholar 

  • Visa M, Isac L, Duta A (2015b) New fly ash TiO2 composite for the sustainable treatment of wastewater with complex pollutants load. Appl Surf Sci 339:62–68

    Article  CAS  Google Scholar 

  • Xin B, Wang P, Ding D, Liu J, Ren Z, Fu H (2008) Effect of surface species on Cu-TiO2 photocatalytic activity. Appl Surf Sci 254:2569–2574

    Article  CAS  Google Scholar 

  • Xu J, Sun X, Shan Y, Xu J, Wang G, Wang L (2019) Enhanced UV-light driven photocatalytic performances and recycling properties of TiO2/AlON composite photocatalyst. Ceram Int 45:6767–6773

    Article  CAS  Google Scholar 

  • Yu L, Xi J, Li M-D, Chan HT, Su T, Phillips DL, Chan WK (2012) The degradation mechanism of methyl orange under photo-catalysis of TiO2. Phys Chem Chem Phys 14:3589–3595

    Article  CAS  Google Scholar 

  • Yu J, Kiwi J, Wang T, Pulgarin C, Rtimi S (2019) Evidence for a dual mechanism in the TiO2/CuxO photocatalyst during the degradation of sulfamethazine under solar or visible light: critical issues. J Photochem Photobiol A Chem 375:270–279

    Article  CAS  Google Scholar 

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Funding

This work was supported by the Universiti Malaysia Sarawak under the Tun Openg Chair (F07/ TOC/1737/2018).

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Authors and Affiliations

  1. Resource Chemistry Programme, Faculty of Resource Science and Technology, Universiti Malaysia Sarawak, 94300, Kota Samarahan, Sarawak, Malaysia

    Devagi Kanakaraju, Muhamad Akif Aizuddin Jasni & Muhamad Hazim Ya

  2. Dipartimento di Scienze e Tecnologie Biologiche Chimiche e Farmaceutiche – STEBICEF, Università degli Studi di Palermo, Viale delle Scienze, Edificio 17, I-90128, Palermo, Italy

    Andrea Pace

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  1. Devagi Kanakaraju
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  2. Muhamad Akif Aizuddin Jasni
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  3. Andrea Pace
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  4. Muhamad Hazim Ya
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Contributions

Devagi Kanakaraju involved in research grant acquisition, research project administration, experimental design, supervision, interpretation of data, and revising the manuscript. Muhamad Akif Aizuddin bin Jasni contributed to performing experiments, data analyses, and writing the manuscript. Andrea Pace contributed in reviewing the manuscript and interpretation of data. Muhamad Hazim bin Ya conducted synthesis of samples, data collection, and data analyses.

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Correspondence to Devagi Kanakaraju.

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Kanakaraju, D., Jasni, M.A.A., Pace, A. et al. Enhanced dye-removal performance of Cu-TiO2-fly ash composite by optimized adsorption and photocatalytic activity under visible light irradiation. Environ Sci Pollut Res 28, 68834–68845 (2021). https://doi.org/10.1007/s11356-021-15440-x

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