Abstract
A lab-scale reactor with a fixed-bed hematite catalyst for the effective decomposition of H2O2 and bacteria inactivation was designed. The bactericidal effect is the largest at a low initial bacterial count of 2·103 CFU/L, which is typical for natural surface waters. When using a 5 mM H2O2 solution and a residence time of 104 min, the reduction in the number of E. coli bacteria is about 3.5-log. At a higher initial bacterial count of 1-2·104 CFU/L, a 5 mM H2O2 solution reduces the bacteria number by about 4-log. The H2O2 decomposition follows the log-linear kinetics of a first-order reaction while the bacterial inactivation does not. The kinetics of bacterial inactivation was described using the Weibull model in the modified form: log10(N0/N) = b · tn. The values of the non-linearity parameter n were found to be lower than 1, indicating that bacterial inactivation slows down over time. With increasing initial H2O2 concentration, the rate parameter b increases while the non-linearity parameter n decreases. With increasing temperature, both parameters increase. The stability of the catalyst has been proved by XRD, FTIR, SEM, and ICP-OES. The concentration of iron leaching into water during disinfection is much lower than the limit declared by WHO for iron in drinking water. The results show that technical-grade hematite is a promising Fenton-like catalyst for water disinfection. The fixed-bed reactor can be the basis of the mobile installations for water purification in emergencies.
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References
Anit J, Praveena MG, Thoufeeq S et al (2023) A simple polyol one-shot synthesis of Maghemite and hematite from inexpensive precursors. Inorg Chem Commun 151:110590. https://doi.org/10.1016/j.inoche.2023.110590
Azam A, Ahmed AS, Oves M et al (2012) Antimicrobial activity of metal oxide nanoparticles against gram-positive and gram-negative bacteria: a comparative study. Int J Nanomedicine 7:6003–6009. https://doi.org/10.2147/IJN.S35347
Baldrian P, Merhautová V, Gabriel J et al (2006) Decolorization of synthetic dyes by hydrogen peroxide with heterogeneous catalysis by mixed iron oxides. Appl Catal B Environ 66:258–264. https://doi.org/10.1016/j.apcatb.2006.04.001
Bhushan M, Kumar Y, Periyasamy L, Viswanath AK (2018) Antibacterial applications of α-Fe2O3/Co3O4 nanocomposites and study of their structural, optical, magnetic and cytotoxic characteristics. Appl Nanosci 8:137–153. https://doi.org/10.1007/s13204-018-0656-5
Bögner D, Bögner M, Schmachtl F et al (2021) Hydrogen peroxide oxygenation and disinfection capacity in recirculating aquaculture systems. Aquac Eng 92:102140. https://doi.org/10.1016/j.aquaeng.2020.102140
Buzrul S (2022) The Weibull model for microbial inactivation. Food Eng Rev 14:45–61. https://doi.org/10.1007/s12393-021-09291-y
Chick M, Lourenco A, Maserati A et al (2022) Thermal death kinetics of three representative salmonella enterica strains in toasted oats cereal. Microorganisms 10. https://doi.org/10.3390/microorganisms10081570
Christenson EC, Cronk R, Atkinson H, Bhatt A, Berdiel E, Cawley M, Cho G, Coleman CK, Harrington C, Heilferty K et al (2021) Evidence map and systematic review of disinfection efficacy on environmental surfaces in healthcare facilities. Int J Environ Res Public Health 18:11100. https://doi.org/10.3390/ijerph182111100
Dash P, Raut S, Jena M, Nayak B (2020) Harnessing the biomedical properties of ferromagnetic α-Fe2O3 NPs with a plausible formation mechanism. Ceram Int 46:26190–26204. https://doi.org/10.1016/j.ceramint.2020.07.117
de Siqueira OL, Eça KS, de Aquino AC, Vasconcelos LB (2018) Chapter 4 - hydrogen peroxide (H2O2) for postharvest fruit and vegetable disinfection. In: Siddiqui MWBT-PD of F and V. Academic Press, pp 91–99
Esteves BM, Morales-Torres S, Maldonado-Hódar FJ, Madeira LM (2022) Sustainable iron-olive stone-based catalysts for Fenton-like olive mill wastewater treatment: development and performance assessment in continuous fixed-bed reactor operation. Chem Eng J 435:134809. https://doi.org/10.1016/j.cej.2022.134809
Garrido-Ramírez EG, Theng BKG, Mora ML (2010) Clays and oxide minerals as catalysts and nanocatalysts in Fenton-like reactions - a review. Appl Clay Sci 47:182–192. https://doi.org/10.1016/j.clay.2009.11.044
Gokulakrishnan B, Satishkumar G (2024) Facilely prepared heterogeneous Fenton catalyst Fe(Fe0.69Al0.31)2O4@C for catalytic wet peroxide oxidation of ciprofloxacin in batch and continuous reactor: reaction intermediates and toxicity evaluation. Sep Purif Technol 333:125690. https://doi.org/10.1016/j.seppur.2023.125690
Grunert A, Frohnert A, Selinka HC, Szewzyk R (2018) A new approach to testing the efficacy of drinking water disinfectants. Int J Hyg Environ Health 221:1124–1132. https://doi.org/10.1016/j.ijheh.2018.07.010
Huang X, Hou X, Zhao J, Zhang L (2016) Hematite facet confined ferrous ions as high efficient Fenton catalysts to degrade organic contaminants by lowering H2O2 decomposition energetic span. Appl Catal B Environ 181:127–137. https://doi.org/10.1016/J.APCATB.2015.06.061
Jia R, Du J, Cao L et al (2021) Application of transcriptome analysis to understand the adverse effects of hydrogen peroxide exposure on brain function in common carp (Cyprinus carpio). Environ Pollut 286:117240. https://doi.org/10.1016/j.envpol.2021.117240
Jin Y, Shi Y, Chen Z et al (2020) Combination of sunlight with hydrogen peroxide generated at a modified reticulated vitreous carbon for drinking water disinfection. J Clean Prod 252:119794. https://doi.org/10.1016/j.jclepro.2019.119794
Khandelwal A, Lapolla B, Bair T et al (2022) Enhanced disinfection with hybrid hydrogen peroxide fogging in a critical care setting. BMC Infect Dis 22:758. https://doi.org/10.1186/s12879-022-07704-9
Kremer ML (1999) Mechanism of the Fenton reaction. Evidence for a new intermediate. Phys Chem Chem Phys 1:3595–3605. https://doi.org/10.1039/a903915e
Lai L, He Y, Zhou H et al (2021) Critical review of natural iron-based minerals used as heterogeneous catalysts in peroxide activation processes: characteristics, applications and mechanisms. J Hazard Mater 416:125809. https://doi.org/10.1016/j.jhazmat.2021.125809
Leonard LT, Vanzin GF, Garayburu-Caruso VA et al (2022) Disinfection byproducts formed during drinking water treatment reveal an export control point for dissolved organic matter in a subalpine headwater stream. Water Res X 15:100144. https://doi.org/10.1016/j.wroa.2022.100144
Li J, Zhao J, Li B et al (2022) Effective inactivation of Escherichia coli in aqueous solution by activated carbon-supported α-FeOOH as heterogeneous Fenton catalyst with high stability and reusability. J Environ Chem Eng 10:107347. https://doi.org/10.1016/j.jece.2022.107347
Liang C, Yin S, Huang P et al (2024) The critical role of minerals in persulfate-based advanced oxidation process: catalytic properties, mechanism, and prospects. Chem Eng J 482:148969. https://doi.org/10.1016/j.cej.2024.148969
Lin S-S, Gurol MD (1998) Catalytic decomposition of hydrogen peroxide on iron oxide: kinetics, mechanism, and implications. Environ Sci Technol 32:1417–1423. https://doi.org/10.1021/es970648k
Liu J, Peng C, Shi X (2022) Preparation, characterization, and applications of Fe-based catalysts in advanced oxidation processes for organics removal: a review. Environ Pollut 293:118565. https://doi.org/10.1016/j.envpol.2021.118565
Liu X (2018) Progress in the mechanism and kinetics of Fenton reaction. MOJ Ecol Environ Sci 3:10–14. https://doi.org/10.15406/mojes.2018.03.00060
Lu Y, Song Z-M, Wang C et al (2021) Combining high resolution mass spectrometry with a halogen extraction code to characterize and identify brominated disinfection byproducts formed during ozonation. Sci Total Environ 796:149016. https://doi.org/10.1016/j.scitotenv.2021.149016
Ma Y, Meng S, Qin M et al (2012) New insight on kinetics of catalytic decomposition of hydrogen peroxide on ferrihydrite: based on the preparation procedures of ferrihydrite. J Phys Chem Solids 73:30–34. https://doi.org/10.1016/j.jpcs.2011.09.015
Marugán J, van Grieken R, Pablos C et al (2015) Photocatalytic inactivation of Escherichia coli aqueous suspensions in a fixed-bed reactor. Catal Today 252:143–149. https://doi.org/10.1016/j.cattod.2014.10.031
Moacă EA, Socoliuc V, Stoian D et al (2022) Synthesis and characterization of bioactive magnetic nanoparticles from the perspective of hyperthermia applications. Magnetochemistry 8:1–21. https://doi.org/10.3390/magnetochemistry8110145
Mohammadi S, Moussavi G, Shekoohiyan S et al (2021) A continuous-flow catalytic process with natural hematite-alginate beads for effective water decontamination and disinfection: Peroxymonosulfate activation leading to dominant sulfate radical and minor non-radical pathways. Chem Eng J 411:127738. https://doi.org/10.1016/j.cej.2020.127738
More S, Raut S, Premkumar S et al (2020) Structural and morphological tuning of iron oxide polymorphs by ECR plasma-assisted thermal oxidation. RSC Adv 10:32088–32101. https://doi.org/10.1039/d0ra05410k
Múčka V, Mižík P (1991) Radiation effects on the activity of ferric oxide catalysts for the decomposition of hydrogen peroxide. Int J Radiat Appl Instrumentation Part C Radiat Phys Chem 38:291–294. https://doi.org/10.1016/1359-0197(91)90095-J
Natarajan S, Harini K, Gajula GP et al (2019) Multifunctional magnetic iron oxide nanoparticles: diverse synthetic approaches, surface modifications, cytotoxicity towards biomedical and industrial applications. BMC Mater 1:1–22. https://doi.org/10.1186/s42833-019-0002-6
Nidheesh PV (2015) Heterogeneous Fenton catalysts for the abatement of organic pollutants from aqueous solution: a review. RSC Adv 5:40552–40577. https://doi.org/10.1039/c5ra02023a
Nordholt N, Lewerenz D, Schreiber F (2022) Time-kill kinetics reveal heterogeneous tolerance to disinfectants. bioRxiv. https://doi.org/10.1101/2022.06.22.497202
Nurdini N, Ilmi MM, Maryanti E et al (2022) Thermally-induced color transformation of hematite: insight into the prehistoric natural pigment preparation. Heliyon 8:10377. https://doi.org/10.1016/j.heliyon.2022.e10377
Odonkor ST, Mahami T (2020) Escherichia coli as a tool for disease risk assessment of drinking water sources. Int J Microbiol 2020:2534130. https://doi.org/10.1155/2020/2534130
Oskoui PR, Rezvani M (2023) Structure and magnetic properties of SiO2−FeO−CaO−Na2O bioactive glass-ceramic system for magnetic fluid hyperthermia application. Heliyon 9:18519. https://doi.org/10.1016/j.heliyon.2023.e18519
Pariente MI, Molina R, Melero JA et al (2015) Intensified-Fenton process for the treatment of phenol aqueous solutions. Water Sci Technol 71:359–365. https://doi.org/10.2166/wst.2014.515
Patyuk LK, Klymenko NA, Nevynna LV, Pupkova OB (2021) Formation and removal of Trihalomethanes and trichloroethylene at different stages of tap water Aftertreatment for beverage production. J Water Chem Technol 43:100–107. https://doi.org/10.3103/S1063455X21020089
Peleg M, Cole MB (1998) Reinterpretation of microbial survival curves. Crit Rev Food Sci Nutr 38:353–380. https://doi.org/10.1080/10408699891274246
Richardson SD, Plewa MJ (2020) To regulate or not to regulate? What to do with more toxic disinfection by-products? J Environ Chem Eng 8:103939. https://doi.org/10.1016/j.jece.2020.103939
Rufus A, Sreeju N, Philip D (2019) Size tunable biosynthesis and luminescence quenching of nanostructured hematite (α-Fe2O3) for catalytic degradation of organic pollutants. J Phys Chem Solids 124:221–234. https://doi.org/10.1016/j.jpcs.2018.09.026
Rufus A, Sreeju N, Vilas V, Philip D (2017) Biosynthesis of hematite (α-Fe2O3) nanostructures: size effects on applications in thermal conductivity, catalysis, and antibacterial activity. J Mol Liq 242:537–549. https://doi.org/10.1016/j.molliq.2017.07.057
Sanchís J, Redondo-Hasselerharm PE, Villanueva CM, Farré MJ (2022) Non targeted screening of nitrogen containing disinfection by-products in formation potential tests of river water and subsequent monitoring in tap water samples. Chemosphere 303:135087. https://doi.org/10.1016/j.chemosphere.2022.135087
Shao Y, Chen H (2018) Heterogeneous Fenton oxidation of phenol in fixed-bed reactor using Fe nanoparticles embedded within ordered mesoporous carbons. Chem Eng Res Des 132:57–68. https://doi.org/10.1016/j.cherd.2017.12.039
Silva MA, Rocha CV, Gallo J et al (2020) Porous composites based on cellulose acetate and alfa-hematite with optical and antimicrobial properties. Carbohydr Polym 241:116362. https://doi.org/10.1016/j.carbpol.2020.116362
Stach R, Barone T, Cauda E et al (2020) Direct infrared spectroscopy for the size-independent identification and quantification of respirable particles relative mass in mine dusts. Anal Bioanal Chem 412:3499–3508. https://doi.org/10.1007/s00216-020-02565-0
Sundara Selvam PS, Govindan S, Perumal B, Kandan V (2021) Screening of in vitro antibacterial property of hematite (α-Fe2O3) nanoparticles: a green approach. Iran J Sci Technol Trans A Sci 45:177–187. https://doi.org/10.1007/s40995-020-00995-0
Tatarchuk T, Danyliuk N, Lapchuk I et al (2022) Oxytetracycline removal and E. Coli inactivation by decomposition of hydrogen peroxide in a continuous fixed bed reactor using heterogeneous catalyst. J Mol Liq 366:120267
Tharani K, Jegatha Christy A, Sagadevan S, Nehru LC (2021) Photocatalytic and antibacterial performance of iron oxide nanoparticles formed by the combustion method. Chem Phys Lett 771:138524. https://doi.org/10.1016/j.cplett.2021.138524
Thomas N, Dionysiou DD, Pillai SC (2021) Heterogeneous Fenton catalysts: a review of recent advances. J Hazard Mater 404:124082. https://doi.org/10.1016/j.jhazmat.2020.124082
Tsuneda T (2020) Fenton reaction mechanism generating no OH radicals in Nafion membrane decomposition. Sci Rep 10:1–13. https://doi.org/10.1038/s41598-020-74646-0
Vafaei Molamahmood H, Geng W, Wei Y et al (2022) Catalyzed H2O2 decomposition over iron oxides and oxyhydroxides: insights from oxygen production and organic degradation. Chemosphere 291:133037. https://doi.org/10.1016/j.chemosphere.2021.133037
van Boekel MAJS (2022) Kinetics of heat-induced changes in dairy products: developments in data analysis and modelling techniques. Int Dairy J 126:105187. https://doi.org/10.1016/j.idairyj.2021.105187
Varouqa IF (2021) Detecting the concentration of aldehydes disinfection by-products formed due to the application of the ozonation process in water treatment plants. Mater Today Proc 45:5631–5634. https://doi.org/10.1016/j.matpr.2021.02.352
Vihodceva S, Šutka A, Sihtmäe M et al (2021) Antibacterial activity of positively and negatively charged hematite (α-fe2 o3) nanoparticles to escherichia coli, staphylococcus aureus and vibrio fischeri. Nanomaterials 11:1–26. https://doi.org/10.3390/nano11030652
Villar-Navarro E, Levchuk I, Rueda-Márquez JJ, Manzano M (2019) Combination of solar disinfection (SODIS) with H2O2 for enhanced disinfection of marine aquaculture effluents. Sol Energy 177:144–154. https://doi.org/10.1016/j.solener.2018.11.018
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 L, Hua B, Yang J et al (2021) Control of disinfection byproduct formation in drinking water by ferrous iron-hydrogen peroxide oxidation. Environ Eng Sci 39:105–113. https://doi.org/10.1089/ees.2020.0481
Weisman RJ, Heinrich A, Letkiewicz F et al (2022) Estimating National Exposures and potential bladder cancer cases associated with chlorination DBPs in U.S. drinking water. Environ Health Perspect 130:87002. https://doi.org/10.1289/EHP9985
World Health Organization (2003) Iron in drinking-water. WHO guidelines for drinking-water quality. Who/Sde/Wsh/0304/08 2:4
Zhang H, Xu Z, Sun W et al (2023) Hydroxylation structure of quartz surface and its molecular hydrophobicity. Appl Surf Sci 612:155884. https://doi.org/10.1016/j.apsusc.2022.155884
Zhao G, Liang L, Wang E et al (2021) Fenton chemistry enables the catalytic oxidative rearrangement of indoles using hydrogen peroxide. Green Chem 23:2300–2307. https://doi.org/10.1039/d1gc00297j
Zhu Y, Zhu R, Xi Y et al (2019) Strategies for enhancing the heterogeneous Fenton catalytic reactivity: a review. Appl Catal B Environ 255:117739. https://doi.org/10.1016/j.apcatb.2019.05.041
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Tetiana Tatarchuk: conceptualization, methodology, supervision, project administration, characterization, data analysis, formal analysis, writing – review & editing and funding acquisition. Alexander Shyichuk: conceptualization, methodology, data analysis, formal analysis, writing – original draft, and writing – review & editing. Nazarii Danyliuk: performing the experiments. Ivanna Lapchuk: performing the experiments. Wojciech Macyk: writing – review & editing.
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Tatarchuk, T., Shyichuk, A., Danyliuk, N. et al. Water disinfection using hydrogen peroxide with fixed bed hematite catalyst – kinetic and activity studies. Environ Sci Pollut Res 31, 26592–26605 (2024). https://doi.org/10.1007/s11356-024-32794-0
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DOI: https://doi.org/10.1007/s11356-024-32794-0