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Environmental Science and Pollution Research

, Volume 25, Issue 23, pp 22998–23008 | Cite as

Kinetics and mechanism of diclofenac removal using ferrate(VI): roles of Fe3+, Fe2+, and Mn2+

  • Junfeng Zhao
  • Qun Wang
  • Yongsheng Fu
  • Bo Peng
  • Gaofeng Zhou
Research Article

Abstract

In this study, the effect of Fe3+, Fe2+, and Mn2+ dose, solution pH, reaction temperature, background water matrix (i.e., inorganic anions, cations, and natural organic matters (NOM)), and the kinetics and mechanism for the reaction system of Fe(VI)/Fe3+, Fe(VI)/Fe2+, and Fe(VI)/Mn2+ were investigated systematically. Traces of Fe3+, Fe2+, and Mn2+ promoted the DCF removal by Fe(VI) significantly. The pseudo-first-order rate constant (kobs) of DCF increased with decreasing pH (9–6) and increasing temperature (10–30 °C) due to the gradually reduced stability and enhanced reactivity of Fe(VI). Cu2+ and Zn2+ ions evidently improved the DCF removal, while CO32− restrained it. Besides, SO42−, Cl, NO3, Mg2+, and Ca2+ almost had no influence on the degradation of DCF by Fe(VI)/Fe3+, Fe(VI)/Fe2+, and Fe(VI)/Mn2+ within the tested concentration. The addition of 5 or 20 mg L−1 NOM decreased the removal efficiency of DCF. Moreover, Fe2O3 and Fe(OH)3, the by-products of Fe(VI), slightly inhibited the DCF removal, while α-FeOOH, another by-product of Fe(VI), showed no influence at pH 7. In addition, MnO2 and MnO4, the by-products of Mn2+, enhanced the DCF degradation due to catalysis and superposition of oxidation capacity, respectively. This study indicates that Fe3+ and Fe2+ promoted the DCF removal mainly via the self-catalysis for Fe(VI), and meanwhile, the catalysis of Mn2+ and the effect of its by-products (i.e., MnO2 and MnO4) contributed synchronously for DCF degradation.

Graphical abstract

Keywords

Diclofenac Ferrate By-products Anionic effect Cationic effect 

Notes

Funding information

This work was supported by the Key R & D project of Science and Technology Department of Sichuan Province [No. 2017SZ0175], the Science and Technology Huimin Project of Chengdu [No. 2014-HM01-00278-SF], and the Joint Research Program about Sustainable Use of Water and Resources in the Upper Yangtze River [No. 2012DFG91520].

Compliance with ethical standards

Conflict of interest

The authors declare that they have no conflict of interest.

References

  1. Aguinaco A, Beltrán FJ, García-Araya JF, Oropesa A (2012) Photocatalytic ozonation to remove the pharmaceutical diclofenac from water: influence of variables. Chem Eng J 189-190:275–282CrossRefGoogle Scholar
  2. Anquandah GA, Sharma VK, Knight DA, Batchu SR, Gardinali PR (2011) Oxidation of trimethoprim by ferrate(VI): kinetics, products, and antibacterial activity. Environ Sci Technol 45:10575–10581CrossRefGoogle Scholar
  3. Buxton GV, Greenstock CL, Helman WP, Ross AB (1988) Critical review of rate constants for reactions of hydrated electrons, hydrogen atoms and hydroxyl radicals (·OH/·O− in aqueous solution). J Phys Chem Ref Data 17:513–886CrossRefGoogle Scholar
  4. Carr JD, Kelter PB, Tabatabai A, Splichal D, Erickson J, McLaughlin CW (1985) Properties of ferrate (VI) in aqueous solution: an alternate oxidant in wastewater treatment. In: Jolley RL (ed) Proceedings of Conference on Water Chlorination Chem. Environment Impact Health Eff. Lewis, Chelsew, pp 1285–1298Google Scholar
  5. Cheng H, Song D, Liu H, Qu J (2015) Permanganate oxidation of diclofenac: the pH-dependent reaction kinetics and a ring-opening mechanism. Chemosphere 136:297–304CrossRefGoogle Scholar
  6. Feng M, Cizmas L, Wang Z, Sharma VK (2017a) Activation of ferrate(VI) by ammonia in oxidation of flumequine: kinetics, transformation products, and antibacterial activity assessment. Chem Eng J 323:584–591CrossRefGoogle Scholar
  7. Feng M, Cizmas L, Wang Z, Sharma VK (2017b) Synergistic effect of aqueous removal of fluoroquinolones by a combined use of peroxymonosulfate and ferrate(VI). Chemosphere 177:144–148CrossRefGoogle Scholar
  8. Feng M, Sharma VK (2018) Enhanced oxidation of antibiotics by ferrate(VI)-sulfur(IV) system: elucidating multi-oxidant mechanism. Chem Eng J 341:137–145CrossRefGoogle Scholar
  9. Filip J, Yngard RA, Siskova K, Marusak Z, Ettler V, Sajdl P, Sharma VK, Zboril R (2011) Mechanisms and efficiency of the simultaneous removal of metals and cyanides by using ferrate(VI): crucial roles of nanocrystalline iron(III) oxyhydroxides and metal carbonates. Chemistry 17:10097–10105CrossRefGoogle Scholar
  10. Gan W, Sharma VK, Zhang X, Yang L, Yang X (2015) Investigation of disinfection byproducts formation in ferrate(VI) pre-oxidation of NOM and its model compounds followed by chlorination. J Hazard Mater 292:197–204CrossRefGoogle Scholar
  11. García-Araya JF, Beltrán FJ, Aguinaco A (2010) Diclofenac removal from water by ozone and photolytic TiO2 catalysed processes. J Chem Technol Biotechnol 85:798–804CrossRefGoogle Scholar
  12. Goodwill JE, Mai X, Jiang Y, Reckhow DA, Tobiason JE (2016) Oxidation of manganese(II) with ferrate: stoichiometry, kinetics, products and impact of organic carbon. Chemosphere 159:457–464CrossRefGoogle Scholar
  13. Graham N, Jiang CC, Li XZ, Jiang JQ, Ma J (2004) The influence of pH on the degradation of phenol and chlorophenols by potassium ferrate. Chemosphere 56:949–956CrossRefGoogle Scholar
  14. Gupta H, Gupta B (2015) Photocatalytic degradation of polycyclic aromatic hydrocarbon benzo[a]pyrene by iron oxides and identification of degradation products. Chemosphere 138:924–931CrossRefGoogle Scholar
  15. Guyer GT, Ince NH (2011) Degradation of diclofenac in water by homogeneous and heterogeneous sonolysis. Ultrason Sonochem 18:114–119CrossRefGoogle Scholar
  16. Han Q, Wang H, Dong W, Liu T, Yin Y (2014) WITHDRAWN: suppression of bromate formation in ozonation process by using ferrate(VI): batch study. Chem Eng J 236:110–120CrossRefGoogle Scholar
  17. Ho C-M, Lau T-C (2000) Lewis acid activated oxidation of alkanes by barium ferrate. New J Chem 24:587–590CrossRefGoogle Scholar
  18. Horst C, Sharma VK, Baum JC, Sohn M (2013) Organic matter source discrimination by humic acid characterization: synchronous scan fluorescence spectroscopy and ferrate(VI). Chemosphere 90:2013–2019CrossRefGoogle Scholar
  19. Hrostowski HJ, Scott AB (1950) The magnetic susceptibility of potassium ferrate. J Chem Phys 18:105–107CrossRefGoogle Scholar
  20. Huang J, Wang Y, Liu G, Chen P, Wang F, Ma J, Li F, Liu H, Lv W (2017) Oxidation of indometacin by ferrate (VI): kinetics, degradation pathways and toxicity assessment. Environ Sci Pollut Res Int 24:10786–10795CrossRefGoogle Scholar
  21. Huguet M, Deborde M, Papot S, Gallard H (2013) Oxidative decarboxylation of diclofenac by manganese oxide bed filter. Water Res 47:5400–5408CrossRefGoogle Scholar
  22. Jain A, Sharma VK, Mbuya OS (2009) Removal of arsenite by Fe(VI), Fe(VI)/Fe(III), and Fe(VI)/Al(III) salts: effect of pH and anions. J Hazard Mater 169:339–344CrossRefGoogle Scholar
  23. Jiang J-Q, Stanford C, Alsheyab M (2009) The online generation and application of ferrate(VI) for sewage treatment—a pilot scale trial. Sep Purif Technol 68:227–231CrossRefGoogle Scholar
  24. Jiang Y, Goodwill JE, Tobiason JE, Reckhow DA (2015) Effect of different solutes, natural organic matter, and particulate Fe(III) on ferrate(VI) decomposition in aqueous solutions. Environ Sci Technol 49:2841–2848CrossRefGoogle Scholar
  25. Johnson MD, Lorenz BB (2015) Antimony remediation using ferrate(VI). Sep Sci Technol 50:1611–1615CrossRefGoogle Scholar
  26. Kim C, Panditi VR, Gardinali PR, Varma RS, Kim H, Sharma VK (2015) Ferrate promoted oxidative cleavage of sulfonamides: kinetics and product formation under acidic conditions. Chem Eng J 279:307–316CrossRefGoogle Scholar
  27. Kralchevska RP, Prucek R, Kolarik J, Tucek J, Machala L, Filip J, Sharma VK, Zboril R (2016) Remarkable efficiency of phosphate removal: ferrate(VI)-induced in situ sorption on core-shell nanoparticles. Water Res 103:83–91CrossRefGoogle Scholar
  28. Lan B, Wang Y, Wang X, Zhou X, Kang Y, Li L (2016) Aqueous arsenic (As) and antimony (Sb) removal by potassium ferrate. Chem Eng J 292:389–397CrossRefGoogle Scholar
  29. Lee Y, Kissner R, von Gunten U (2014) Reaction of ferrate(VI) with ABTS and self-decay of ferrate(VI): kinetics and mechanisms. Environ Sci Technol 48:5154–5162CrossRefGoogle Scholar
  30. Luo Z, Li X, Zhai J (2016) Kinetic investigations of quinoline oxidation by ferrate(VI). Environ Technol 37:1249–1256CrossRefGoogle Scholar
  31. Manoli K, Nakhla G, Feng M, Sharma VK, Ray AK (2017a) Silica gel-enhanced oxidation of caffeine by ferrate(VI). Chem Eng J 330:987–994CrossRefGoogle Scholar
  32. Manoli K, Nakhla G, Ray AK, Sharma VK (2017b) Enhanced oxidative transformation of organic contaminants by activation of ferrate(VI): possible involvement of Fe V /Fe IV species. Chem Eng J 307:513–517CrossRefGoogle Scholar
  33. Manoli K, Nakhla G, Ray AK, Sharma VK (2017c) Oxidation of caffeine by acid-activated ferrate(VI): effect of ions and natural organic matter. AICHE J 63:4998–5006CrossRefGoogle Scholar
  34. Michael I, Achilleos A, Lambropoulou D, Torrens VO, Pérez S, Petrović M, Barceló D, Fatta-Kassinos D (2014) Proposed transformation pathway and evolution profile of diclofenac and ibuprofen transformation products during (sono)photocatalysis. Appl Catal B Environ 147:1015–1027CrossRefGoogle Scholar
  35. Nie E, Yang M, Wang D, Yang X, Luo X, Zheng Z (2014) Degradation of diclofenac by ultrasonic irradiation: kinetic studies and degradation pathways. Chemosphere 113:165–170CrossRefGoogle Scholar
  36. Noorhasan NN, Sharma VK (2008) Kinetics of the reaction of aqueous iron(vi) (FeVIO42-) with ethylenediaminetetraacetic acid. Dalton Trans 1883–1887.  https://doi.org/10.1039/b715154c
  37. Noorhasan N, Patel B, Sharma VK (2010) Ferrate(VI) oxidation of glycine and glycylglycine: kinetics and products. Water Res 44(3):927–935CrossRefGoogle Scholar
  38. Pochard I, Denoyel R, Couchot P, Foissy A (2002) Adsorption of barium and calcium chloride onto negatively charged α-Fe2O3 particles. J Colloid Interface Sci 255:27–35CrossRefGoogle Scholar
  39. Prucek R, Tucek J, Kolarik J, Huskova I, Filip J, Varma RS, Sharma VK, Zboril R (2015) Ferrate(VI)-prompted removal of metals in aqueous media: mechanistic delineation of enhanced efficiency via metal entrenchment in magnetic oxides. Environ Sci Technol 49:2319–2327CrossRefGoogle Scholar
  40. Rizzo L, Meric S, Kassinos D, Guida M, Russo F, Belgiorno V (2009) Degradation of diclofenac by TiO(2) photocatalysis: UV absorbance kinetics and process evaluation through a set of toxicity bioassays. Water Res 43:979–988CrossRefGoogle Scholar
  41. Rush JD, Zhao Z, Bielski BHJ (1996) Reaction of ferrate(VI)/ferrate(V) with hydrogen peroxide and superoxide anion-a stopped-flow and premix pulse radiolysis study. Free Rad Res 24:187–198CrossRefGoogle Scholar
  42. Sharma VK, O’Connor DB (2000) Ferrate(V) oxidation of thiourea: a premix pulse radiolysis study. Inorg Chim Acta 311:40–44CrossRefGoogle Scholar
  43. Sharma VK, Burnett CR, Millero FJ (2001) Dissociation constants of the monoprotic ferrate(VI) ion in NaCl media. Phys Chem Chem Phys 3:2059–2062CrossRefGoogle Scholar
  44. Sharma VK (2011) Oxidation of inorganic contaminants by ferrates (VI, V, and IV)—kinetics and mechanisms: a review. J Environ Manag 92:1051–1073CrossRefGoogle Scholar
  45. Sharma VK (2013) Ferrate(VI) and ferrate(V) oxidation of organic compounds: kinetics and mechanism. Coord Chem Rev 257:495–510CrossRefGoogle Scholar
  46. Sharma VK, Chen L, Zboril R (2015a) Review on high valent FeVI (ferrate): a sustainable green oxidant in organic chemistry and transformation of pharmaceuticals. ACS Sustain Chem Eng 4:18–34CrossRefGoogle Scholar
  47. Sharma VK, Zboril R, Varma RS (2015b) Ferrates: greener oxidants with multimodal action in water treatment technologies. Acc Chem Res 48:182–191CrossRefGoogle Scholar
  48. Shu Z, Bolton JR, Belosevic M, El Din MG (2013) Photodegradation of emerging micropollutants using the medium-pressure UV/H2O2 advanced oxidation process. Water Res 47:2881–2889CrossRefGoogle Scholar
  49. Snyder SA, Adham S, Redding AM, Cannon FS, DeCarolis J, Oppenheimer J, Wert EC, Yoon Y (2007) Role of membranes and activated carbon in the removal of endocrine disruptors and pharmaceuticals. Desalination 202:156–181CrossRefGoogle Scholar
  50. Song Y, Deng Y, Jung C (2016) Mitigation and degradation of natural organic matters (NOMs) during ferrate(VI) application for drinking water treatment. Chemosphere 146:145–153CrossRefGoogle Scholar
  51. Soufan M, Deborde M, Legube B (2012) Aqueous chlorination of diclofenac: kinetic study and transformation products identification. Water Res 46:3377–3386CrossRefGoogle Scholar
  52. Wang H, Liu Y, Jiang JQ (2016) Reaction kinetics and oxidation product formation in the degradation of acetaminophen by ferrate (VI). Chemosphere 155:583–590CrossRefGoogle Scholar
  53. Wang Y, Liu H, Liu G, Xie Y, Gao S (2015) Oxidation of diclofenac by potassium ferrate (VI): reaction kinetics and toxicity evaluation. Sci Total Environ 506-507:252–258CrossRefGoogle Scholar
  54. Weast RC (1970-1971) Handbook of Chemistry and Physics, vol 51. CRC Press, Cleveland, p 111Google Scholar
  55. Wood RH (1958) The heat, free energy, and entropy of the ferrate(VI) ion. J Amer Chem Soc 80:2038–2041CrossRefGoogle Scholar
  56. Xu GR, Zhang YP, Li GB (2009) Degradation of azo dye active brilliant red X-3B by composite ferrate solution. J Hazard Mater 161:1299–1305CrossRefGoogle Scholar
  57. Yang B, Ying GG (2013) Oxidation of benzophenone-3 during water treatment with ferrate(VI). Water Res 47:2458–2466CrossRefGoogle Scholar
  58. Yang Y-J, Liu E-H, Li L-M, Huang Z-Z, Shen H-J, Xiang X-X (2010) Nanostructured amorphous MnO2 prepared by reaction of KMnO4 with triethanolamine. J Alloys Compd 505:555–559CrossRefGoogle Scholar
  59. Yu W, Yang Y, Graham N (2016) Evaluation of ferrate as a coagulant aid/oxidant pretreatment for mitigating submerged ultrafiltration membrane fouling in drinking water treatment. Chem Eng J 298:234–242CrossRefGoogle Scholar
  60. Zhang P, Zhang G, Dong J, Fan M, Zeng G (2012) Bisphenol A oxidative removal by ferrate (Fe(VI)) under a weak acidic condition. Sep Purif Technol 84:46–51CrossRefGoogle Scholar
  61. Zhang T, Zhu H, Croue JP (2013) Production of sulfate radical from peroxymonosulfate induced by a magnetically separable CuFe2O4 spinel in water: efficiency, stability, and mechanism. Environ Sci Technol 47:2784–2791CrossRefGoogle Scholar
  62. Zhang Y, Geissen SU, Gal C (2008) Carbamazepine and diclofenac: removal in wastewater treatment plants and occurrence in water bodies. Chemosphere 73:1151–1161CrossRefGoogle Scholar
  63. Zhao J, Liu Y, Wang Q, Fu Y, Lu X, Bai X (2018) The self-catalysis of ferrate (VI) by its reactive byproducts or reductive substances for the degradation of diclofenac: kinetics, mechanism and transformation products. Sep Purif Technol 192:412–418CrossRefGoogle Scholar
  64. Zhou JH, Chen KB, Hong QK, Zeng FC, Wang HY (2017) Degradation of chloramphenicol by potassium ferrate (VI) oxidation: kinetics and products. Environ Sci Pollut Res Int 24:10166–10171CrossRefGoogle Scholar

Copyright information

© Springer-Verlag GmbH Germany, part of Springer Nature 2018

Authors and Affiliations

  1. 1.Faculty of Geosciences and Environmental EngineeringSouthwest Jiaotong UniversityChengduChina

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