Abstract
In this study, coal bottom ash from a thermoelectric plant was tested as an alternative Fenton catalyst for phenol degradation in water. The effect of operating parameters such as initial pH, catalyst dosage and H2O2 concentration were evaluated. The characterization results indicated that the material has a mesoporous structure, with active species (Fe) well distributed on its surface. Under the optimal reaction conditions (6 mM H2O2, 1 g L−1 of catalyst and pH = 3), 98.7% phenol degradation efficiency was achieved in 60 min, as well as 71.6% TOC removal after 150 min. Hydroxyl radical was identified as the main oxidizing agent involved on the cleavage of the phenol molecule. After four consecutive reuse cycles, phenol degradation efficiency was around 80%, indicating good reusability and stability of the catalyst. Therefore, the obtained results demonstrated that the bottom ash presents remarkable activity for application in the Fenton reaction towards phenol degradation.
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The datasets used and analyzed during the current study are available from the corresponding author on reasonable request.
References
Akram A, Ikhlaq A, Javed F et al (2021) Uv-irradiated fly ash-catalyzed fenton-type process for the removal of paracetamol in wastewater: Nickel, copper, and manganese as active sites. Desalin Water Treat 215:160–166. https://doi.org/10.5004/dwt.2021.26753
Anchieta CG, Severo EC, Rigo C et al (2015) Rapid and facile preparation of zinc ferrite (ZnFe2O4) oxide by microwave-solvothermal technique and its catalytic activity in heterogeneous photo-Fenton reaction. Mater Chem Phys 160:141–147. https://doi.org/10.1016/j.matchemphys.2015.04.016
Anku WW, Mamo MA, Govender PP (2017) Phenolic Compounds in water: sources, reactivity, toxicity and treatment methods. Phenolic compounds - natural sources, importance and applications. InTech. https://doi.org/10.5772/66927
Becelic M, Dalmacija B, Rajic L et al (2014) Degradation of anthraquinone dye reactive blue 4 in pyrite ash catalyzed fenton reaction. Sci World J 2014:1–8. https://doi.org/10.1155/2014/234654
Cahan R, Stein M, Anker Y et al (2013) Innovative utilization of coal bottom ash for bioremediation of toxic organic pollutants. Inter Biodeterior Biodegrad 85:421e42. https://doi.org/10.1016/j.ibiod.2013.08.010
Chakraborty A, Sarangapany S, Mishra U et al (2022) Green synthesized magnetically separable iron oxide nanoparticles for efficient heterogeneous photo-Fenton degradation of dye pollutants. J Clust Sci 33:675–685. https://doi.org/10.1007/s10876-021-02010-x
Chen H, Zhang Z, Yang Z et al (2015) Heterogeneous fenton-like catalytic degradation of 2,4-dichlorophenoxyacetic acid in water with FeS. Chem Eng J 273:481–489. https://doi.org/10.1016/j.cej.2015.03.079
CONAMA (National Environment Council) (2011) Resolution 430. Provisions the conditions and standards of effluents (in Portuguese). http://www2.mma.gov.br/port/conama/legiabre.cfm?codlegi=646. Accessed 09 Feb 2023
Drumm FC, Oliveira JS, Foletto EL et al (2018) Response surface methodology approach for the optimization of tartrazine removal by heterogeneous photo-Fenton process using mesostructured Fe2O3-supported ZSM-5 prepared by chitin-templating. Chem Eng Commun 205:445–455. https://doi.org/10.1080/00986445.2017.1402009
Drumm FC, Franco DS, Grassi P et al (2022b) Effective adsorptive removal of textile pollutant using coal bottom ash with high surface area obtained by alkaline fusion route. Environ Technol 43(16):2418–2429. https://doi.org/10.1080/09593330.2021.1881828
Drumm FC, Grassi P, Georgin J et al (2022b) Applicability of amethyst mining rejects as a novel photo-fenton catalyst for the abatement of an emerging pollutant in water. Appl Geochem 136:105136. https://doi.org/10.1016/j.apgeochem.2021.105136
Drumm FC, Grassi P, Sulkovski AA et al (2019) Applicability of coal bottom ash from thermoelectric power plant as an alternative heterogeneous catalyst in photo-Fenton reaction. Water Air Soil Pollut 230. https://doi.org/10.1007/s11270-019-4327-2
Ely C, Hoefling Souza D, Fernandes M et al (2021) Enhanced removal of phenol from biorefinery wastewater treatment using enzymatic and Fenton process. Environ Technol (UK) 42:2733–2739. https://doi.org/10.1080/09593330.2020.1713220
Faheem M, Jiang X, Wang L et al (2018) Synthesis of Cu2O-CuFe2O4 microparticles from Fenton sludge and its application in the Fenton process: The key role of Cu2O in the catalytic degradation of phenol. RSC Adv 8:5740–5748. https://doi.org/10.1039/c7ra13608k
Fan X, Cao Q, Meng F et al (2021) A Fenton-like system of biochar loading Fe–Al layered double hydroxides (FeAl-LDH@BC)/H2O2 for phenol removal. Chemosphere 266:128992. https://doi.org/10.1016/j.chemosphere.2020.128992
Feng Z, Yang J, Zhu L et al (2023) Bromine functionalized Fe/Cu bimetallic MOFs for accelerating Fe(III)/Fe(II) cycle and efficient degradation of phenol in Fenton-like system. Colloids Surf A Physicochem Eng Asp. 658:130701. https://doi.org/10.1016/j.colsurfa.2022.130701
Gao P, Song Y, Hao M et al (2018) An effective and magnetic Fe2O3-ZrO2 catalyst for phenol degradation under neutral pH in the heterogeneous Fenton-like reaction. Sep Purif Technol 201:238–243. https://doi.org/10.1016/j.seppur.2018.03.017
Grassi P, Drumm FC, da Silveira SJ et al (2020a) Investigation of the reaction pathway for degradation of emerging contaminant in water by photo-Fenton oxidation using fly ash as low-cost raw catalyst. Int J Environ Res 14:427–438. https://doi.org/10.1007/s41742-020-00266-1
Grassi P, Drumm FC, Georgin J et al (2020b) Water treatment plant sludge as iron source to catalyze a heterogeneous photo-Fenton reaction. Environ Technol Innov. 17:100544. https://doi.org/10.1016/j.eti.2019.100544
Grassi P, Drumm FC, Franco DS et al (2020c) Application of fly ash modified by alkaline fusion as an effective adsorbent to remove methyl violet 10B in water. Chem Eng Commun 209(2):184–195. https://doi.org/10.1080/00986445.2020.1852222
Hollanda LR, Santos SBF, Faustino JG et al (2021) Oil field–produced water treatment: characterization, photochemical systems, and combined processes. Environ Sci Pollut Res 28:52744–52763. https://doi.org/10.1007/s11356-021-16222-1
Hussain S, Aneggi E, Maschio S et al (2021) Steel Scale Waste as a Heterogeneous Fenton-like Catalyst for the Treatment of Landfill Leachate. Ind Eng Chem Res 60:11715–11724. https://doi.org/10.1021/acs.iecr.1c01901
Ioffe M, Kundu S, Perez-Lapid N et al (2022) Heterogeneous Fenton catalyst based on clay decorated with nano-sized amorphous iron oxides prevents oxidant scavenging through surface complexation. Chem Eng J. 433:134609. https://doi.org/10.1016/j.cej.2022.134609
Labidi A, Ren H, Sial A, Wang H, Lichtfouse E, Wang C (2023) Coal ash for removing toxic metals and phenolic contaminants from wastewater: A brief review. Crit Rev Environ Sci Technol 53:2006–2029. https://doi.org/10.1080/10643389.2023.2206781
Ling Y, Long M, Hu P et al (2014) Magnetically separable core-shell structural γ-Fe2O3@Cu/Al-MCM-41 nanocomposite and its performance in heterogeneous Fenton catalysis. J Hazard Mater 264:195–202. https://doi.org/10.1016/j.jhazmat.2013.11.008
Luna AJ, Nascimento CAO, Foletto EL, Moraes JEF, Chiavone-Filho O (2014) Photo-Fenton degradation of phenol, 2,4-dichlorophenoxyacetic acid and 2,4-dichlorophenol mixture in saline solution using a falling-film solar reactor. Environ Technol 35:364–371. https://doi.org/10.1080/09593330.2013.828762
Luo W, Zhu L, Wang N et al (2010) Efficient removal of organic pollutants with magnetic nanoscaled BiFeO 3 as a reusable heterogeneous fenton-like catalyst. Environ Sci Technol 44:1786–1791. https://doi.org/10.1021/es903390g
Magalhães VMA, Mendes GP, Costa-Filho JDB et al (2020) Clay-based catalyst synthesized for chemical oxidation of phenanthrene contaminated soil using hydrogen peroxide and persulfate. J Environ Chem Eng. 8(2):103568. https://doi.org/10.1016/j.jece.2019.103568
Mani A, Kulandaivellu T, Govindaswamy S et al (2018) Fe3O4 nanoparticle-encapsulated mesoporous carbon composite: An efficient heterogeneous Fenton catalyst for phenol degradation. Environ Sci Pollut Res 25:20419–20429. https://doi.org/10.1007/s11356-017-9663-4
Martinez AA, Fixman EM, Cánepa AL et al (2020) Preparation, characterization, and application of nano-FeOx/Al2O3/cordierite monolithic catalysts for heterogeneous dark Fenton reaction. J Chem Technol Biotechnol 95:2868–2878. https://doi.org/10.1002/jctb.6446
Martins RC, Henriques LR, Quinta-Ferreira RM (2013) Catalytic activity of low cost materials for pollutants abatement by Fenton’s process. Chem Eng Sci 100:225–233. https://doi.org/10.1016/j.ces.2013.03.024
Mashayekh-Salehi A, Akbarmojeni K, Roudbari A et al (2021) Use of mine waste for H2O2-assisted heterogeneous Fenton-like degradation of tetracycline by natural pyrite nanoparticles: Catalyst characterization, degradation mechanism, operational parameters and cytotoxicity assessment. J Clean Prod. 291:125235. https://doi.org/10.1016/j.jclepro.2020.125235
Miceli M, Frontera P, Macario A et al (2021) Recovery/reuse of heterogeneous supported spent catalysts. Catalysts 11(5):591. https://doi.org/10.3390/catal11050591
Mossmann A, Dotto GL, Hotza D, Jahn SL, Foletto EL (2019) Preparation of polyethylene–supported zero–valent iron buoyant catalyst and its performance for Ponceau 4R decolorization by photo–Fenton process. J Environ Chem Eng 4:102963. https://doi.org/10.1016/j.jece.2019.102963
Muhammad S, Saputra E, Sun H et al (2012) Coal fly ash supported Co 3O 4 catalysts for phenol degradation using peroxymonosulfate. RSC Adv 2:5645–5650. https://doi.org/10.1039/c2ra20346d
Nadeem N, Abbas Q, Yaseen M et al (2021) Coal fly ash-based copper ferrite nanocomposites as potential heterogeneous photocatalysts for wastewater remediation. Appl Surf Sci. 565:150542. https://doi.org/10.1016/j.apsusc.2021.150542
Narayani H, Augustine R, Sumi S et al (2017) Removal of basic and industrial azo reactive dyes from aqueous solutions via Fenton-like reactions using catalytic non-magnetic Pd-flyash and magnetic Pd-Fe3O4-flyash composite particles. Sep Purif Technol 172:338–349. https://doi.org/10.1016/j.seppur.2016.08.027
Niveditha S, Gandhimathi R (2020) Flyash augmented Fe3O4 as a heterogeneous catalyst for degradation of stabilized landfill leachate in Fenton process. Chemosphere. 242:125189. https://doi.org/10.1016/j.chemosphere.2019.125189
Oliveira JS, Mazutti MA, Urquieta-González EA et al (2016a) Preparation of Mesoporous Fe2O3-Supported ZSM-5 Zeolites by Carbon-Templating and their Evaluation as Photo-Fenton Catalysts to Degrade Organic Pollutant. Mat Res 19(6):1399–1406. https://doi.org/10.1590/1980-5373-MR-2016-0367
Oliveira JS, Drumm FC, Mazutti MA et al (2016b) Preparation of Fe2O3/ZSM-5 system for use as catalyst in photo-Fenton reaction. Cerâmica 62(281):287. https://doi.org/10.1590/0366-69132016623632022
Oppenländer T (2002) Photochemical purification of water and air: Advanced Oxidation Processes (AOPs): principles, reaction mechanisms, reactor concepts. Wiley‐VCH Verlag GmbH & Co. KGaA.https://doi.org/10.1002/9783527610884
Rahim Pouran S, Abdul Raman AA, Wan Daud WMA (2014) Review on the application of modified iron oxides as heterogeneous catalysts in Fenton reactions. J Clean Prod 64:24–35. https://doi.org/10.1016/j.jclepro.2013.09.013
Ramírez-Franco JH, Galeano LA, Vicente MA (2019) Fly ash as photo-Fenton catalyst for the degradation of amoxicillin. J Environ Chem Eng. 7(5):103274. https://doi.org/10.1016/j.jece.2019.103274
Rashidi NA, Yusup S (2016) Overview on the Potential of Coal-Based Bottom Ash as Low-Cost Adsorbents. ACS Sustain Chem Eng 4:1870–1884. https://doi.org/10.1021/acssuschemeng.5b01437
Salla JS, Martinello K, Dotto GL et al (2020) Synthesis of citrate–modified CuFeS2 catalyst with significant effect on the photo–Fenton degradation efficiency of bisphenol a under visible light and near–neutral pH. Coll Surf A: Physicochem Eng Aspects 595:124679. https://doi.org/10.1016/j.colsurfa.2020.124679
Sashkina KA, Labko VS, Rudina NA et al (2013) Hierarchical zeolite FeZSM-5 as a heterogeneous Fenton-type catalyst. J Catal 299:44–52. https://doi.org/10.1016/j.jcat.2012.11.028
Severo EC, Anchieta CG, Foletto VS et al (2016) Degradation of Amaranth azo dye in water by heterogeneous photo-Fenton process using FeWO4 catalyst prepared by microwave irradiation. Water Sci Technol 73:88–94. https://doi.org/10.2166/wst.2015.469
Shen J, Zhou Y, Li S et al (2019) Hydrogel-coated Fe3O4 nanoparticles as an efficient heterogeneous Fenton catalyst for degradation of phenol. J Mater Sci 54:10684–10694. https://doi.org/10.1007/s10853-019-03661-y
Shi X, Tian A, You J et al (2018) Degradation of organic dyes by a new heterogeneous Fenton reagent - Fe2GeS4 nanoparticle. J Hazard Mater 353:182–189. https://doi.org/10.1016/j.jhazmat.2018.04.018
Shin J, Bae S, Chon K (2021) Fenton oxidation of synthetic food dyes by Fe-embedded coffee biochar catalysts prepared at different pyrolysis temperatures: A mechanism study. Chem Eng J 421:129943. https://doi.org/10.1016/j.cej.2021.129943
Silvestri S, Foletto EL (2017) Preparation and characterization of Fe2O3/TiO2/clay plates and their use as photocatalysts. Ceram Int 43(16):14057–14062. https://doi.org/10.1016/j.ceramint.2017.07.140
Silvestri S, Stefanello N, Sulkovski AA, Foletto EL (2020) Preparation of TiO2 supported on MDF biochar for simultaneous removal of methylene blue by adsorption and photocatalysis. J Chem Technol Biotechnol 95(10):2723–2729. https://doi.org/10.1002/jctb.6279
Tavares MG, Duarte JL da S, Oliveira LMTM et al (2022) Reusable iron magnetic catalyst for organic pollutant removal by adsorption, Fenton and photo Fenton process. J Photochem Photobiol A Chem. 432:114089. https://doi.org/10.1016/j.jphotochem.2022.114089
Thommes M, Kaneko K, Neimark AV et al (2015) Physisorption of gases, with special reference to the evaluation of surface area and pore size distribution (IUPAC Technical Report). Pure Appl Chem 87:1051–1069. https://doi.org/10.1515/pac-2014-1117
Velosa AC, Nascimento CAO (2017) Evaluation of sulfathiazole degradation by persulfate in Milli-Q water and in effluent of a sewage treatment plant. Environ Sci Pollut Res 24:6270–6277. https://doi.org/10.1007/s11356-016-7036-z
Vieira Y, Leichtweis J, Foletto EL, Silvestri S (2020) Reactive oxygen species-induced heterogeneous photocatalytic degradation of organic pollutant rhodamine B by copper and zinc aluminate spinels. J Chem Technol Biotechnol 95(3):791–797. https://doi.org/10.1002/jctb.6267
Wang J, Tang J (2021) Fe-based Fenton-like catalysts for water treatment: Catalytic mechanisms and applications. J Mol Liq. 332:115755. https://doi.org/10.1016/j.molliq.2021.115755
Wang P, Zhou X, Zhang Y et al (2017) Unveiling the mechanism of electron transfer facilitated regeneration of active Fe2+ by nano-dispersed iron/graphene catalyst for phenol removal. RSC Adv 7:26983–26991. https://doi.org/10.1039/c7ra04312k
Wang H, Jing M, Wu Y et al (2018) Effective degradation of phenol via Fenton reaction over CuNiFe layered double hydroxides. J Hazard Mater 353:53–61. https://doi.org/10.1016/j.jhazmat.2018.03.053
Wang Y, Zhu Q, Xie T et al (2022a) Performance and mechanism of FeS2/FeSxOy as highly effective Fenton-like catalyst for phenol degradation. Environ Technol (UK). https://doi.org/10.1080/09593330.2022.2071640
Wang C, Jiang R, Yang J et al (2022b) Enhanced heterogeneous Fenton degradation of organic pollutants by CRC/Fe3O4 catalyst at neutral pH. Front Chem 10. https://doi.org/10.3389/fchem.2022.892424
Wei X, Wu H, Sun F (2017) Magnetite/Fe-Al-montmorillonite as a Fenton catalyst with efficient degradation of phenol. J Colloid Interface Sci 504:611–619. https://doi.org/10.1016/j.jcis.2017.05.110
Wei X, Xie X, Wang Y et al (2020) Shape-dependent Fenton-like catalytic activity of Fe3O4 nanoparticles. J Environ Eng 146. https://doi.org/10.1061/(asce)ee.1943-7870.0001648
Xia M, Chen C, Long M et al (2011) Magnetically separable mesoporous silica nanocomposite and its application in Fenton catalysis. Microporous Mesoporous Mater 145:217–223. https://doi.org/10.1016/j.micromeso.2011.05.017
Xia Q, Jiang Z, Wang J et al (2017) A facile preparation of hierarchical dendritic zero-valent iron for Fenton-like degradation of phenol. Catal Commun 100:57–61. https://doi.org/10.1016/j.catcom.2017.06.017
Xia Q, Jiang Z, Li D et al (2018) Green synthesis of a dendritic Fe3O4@Feo composite modified with polar C-groups for Fenton-like oxidation of phenol. J Alloys Compd 746:453–461. https://doi.org/10.1016/j.jallcom.2018.02.311
Xia Q, Yao Z, Zhang D et al (2019) Rational synthesis of micronano dendritic ZVI@Fe 3 O 4 modified with carbon quantum dots and oxygen vacancies for accelerating Fenton-like oxidation. Sci Total Environ 671:1056–1065. https://doi.org/10.1016/j.scitotenv.2019.03.435
Xiao C, Li J, Zhang G (2018) Synthesis of stable burger-like α-Fe2O3 catalysts: Formation mechanism and excellent photo-Fenton catalytic performance. J Clean Prod 180:550–559. https://doi.org/10.1016/j.jclepro.2018.01.127
Xie Y, Xiong R, Li J et al (2023) Insight into n-CaO2/SBC/Fe(II) Fenton-like system for glyphosate degradation: pH change, iron conversion, and mechanism. J Environ Manag 333:117428. https://doi.org/10.1016/j.jenvman.2023.117428
Xu X, Zong S, Chen W et al (2019) Comparative study of Bisphenol A degradation via heterogeneously catalyzed H2O2 and persulfate: Reactivity, products, stability and mechanism. Chem Eng J 369:470–479. https://doi.org/10.1016/j.cej.2019.03.099
Xu Y, Guo X, Zha F et al (2020) Efficient photocatalytic removal of orange II by a Mn3O4–FeS2/Fe2O3 heterogeneous catalyst. J Environ Manage. 253:109695. https://doi.org/10.1016/j.jenvman.2019.109695
Yan J, Tang H, Lin Z et al (2012) Efficient degradation of organic pollutants with ferrous hydroxide colloids as heterogeneous Fenton-like activator of hydrogen peroxide. Chemosphere 87:111–117. https://doi.org/10.1016/j.chemosphere.2011.11.069
Yan J, Gao W, Dong M et al (2016) Degradation of trichloroethylene by activated persulfate using a reduced graphene oxide supported magnetite nanoparticle. Chem Eng J 295:309–316. https://doi.org/10.1016/j.cej.2016.01.085
Yang B, Tian Z, Zhang L et al (2015) Enhanced heterogeneous Fenton degradation of Methylene Blue by nanoscale zero valent iron (nZVI) assembled on magnetic Fe3O4/reduced graphene oxide. J Water Process Eng 5:101–111. https://doi.org/10.1016/j.jwpe.2015.01.006
Yang G, Mo S, Xing B et al (2020) Effective degradation of phenol via catalytic wet peroxide oxidation over N, S, and Fe-tridoped activated carbon. Environ Pollut 258:113687. https://doi.org/10.1016/j.envpol.2019.113687
Zhang A, Wang N, Zhou J et al (2012) Heterogeneous Fenton-like catalytic removal of p-nitrophenol in water using acid-activated fly ash. J Hazard Mater 201–202:68–73. https://doi.org/10.1016/j.jhazmat.2011.11.033
Zhou H, Bhattarai R, Li Y et al (2022) Towards sustainable coal industry: Turning coal bottom ash into wealth. Sci Total Environ 804:149985. https://doi.org/10.1016/j.scitotenv.2021.149985
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The authors thank the Coordination for the Improvement of Higher Education Personnel (CAPES) and the National Agency for Petroleum, Natural Gas, and Biofuels (ANP) for financial support. In addition, the authors gratefully acknowledge the analysis support from the Chemistry Institute (IQ), Laboratório de Peneiras Moleculares (LABPEMOL), Núcleo de Processamento Primário e Reúso de Água Produzida e Resíduos (NUPPRAR), and Materials Engineering Department (DEMat) from UFRN.
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This work was supported by CAPES (Coordination for the Improvement of Higher Education Personnel) and CNPq (National Council for Scientific and Technological Development) for financial support.
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Conceptualization: (Luana Rabelo Hollanda, Osvaldo Chiavone-Filho); Methodology: (Joyce Azevedo Bezerra de Souza), Formal analysis and investigation: (Luana Rabelo Hollanda, Joyce Azevedo Bezerra de Souza); Writing—original draft preparation: (Luana Rabelo Hollanda, Edson Luiz Foletto, Guilherme Luiz Dotto); Writing—review and editing: (Guilherme Luiz Dotto, Edson Luiz Foletto); Funding acquisition: (Osvaldo Chiavone-Filho); Supervision: (Osvaldo Chiavone-Filho). All authors read and approved the final manuscript.
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Hollanda, L.R., de Souza, J.A.B., Foletto, E.L. et al. Applying bottom ash as an alternative Fenton catalyst for effective removal of phenol from aqueous environment. Environ Sci Pollut Res 30, 120763–120774 (2023). https://doi.org/10.1007/s11356-023-30890-1
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DOI: https://doi.org/10.1007/s11356-023-30890-1