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Zero-valent iron/persulfate(Fe0/PS) oxidation acetaminophen in water

  • J. Deng
  • Y. Shao
  • N. Gao
  • Y. Deng
  • C. Tan
  • S. Zhou
Original Paper

Abstract

Zero-valent iron (Fe0), as an alternative iron source, was evaluated to activate persulfate (PS) to degrade acetaminophen (APAP), a representative pharmaceutically active compound in water. Effects of key factors in the so-called Fe0/PS process, including Fe0 dosage, initial pH, temperatures and chelating agents, were studied. Under all the conditions tested, the APAP degradation followed a pseudo-first-order kinetics pattern. The degradation efficiency of APAP was highest when the Fe0 to PS molar ratio increased to 1:1, and the degradation rate constant and removal were 23.19 × 10−3 min−1 and 93.19 %, respectively. Comparing with Fe2+, Fe0 served as an alternative iron source that can gradually release Fe2+ into water, thereby consistently activating PS to produce sulfate radicals. The Fe0/PS system was effective in a broader pH range from 3 to 8.5. Heat could facilitate production of sulfate radicals and enhance the APAP degradation in the Fe0/PS system. High reaction temperature also improved the Fe2+/PS oxidation of APAP. Finally, sodium citrate (a chelating agent) at an appropriate concentration could improve the APAP degradation rate in the Fe2+/PS and Fe0/PS system. The optimal molar ratio of Fe0 to citrate depended on solution pH. Our results demonstrated that Fe0 was an alternative iron source to activate PS to degrade APAP in water.

Keywords

Affecting factors pH Sodium citrate Sulfate radicals Temperature 

Notes

Acknowledgments

Financial supports from the National Major Project of Science and Technology Ministry of China (2008ZX07421-002) and the research and development Project of Ministry of Housing and Urban–Rural Development (2009-K7-4). We are also thankful to the reviewers for their valuable advice to improve this manuscript.

References

  1. Anipsitakis GP, Dionysiou DD (2003) Degradation of organic contaminants in water with sulfate radicals generated by the conjunction of peroxymonosulfate with cobalt. Environ Sci Technol 37(20):4790–4797CrossRefGoogle Scholar
  2. Anipsitakis GP, Dionysiou DD (2004) Radical generation by the interaction of transition metals with common oxidants. Environ Sci Technol 38(13):3705–3712CrossRefGoogle Scholar
  3. Anoniou MG, De La Cruz AA, Dionysiou DD (2010) Degradation of microcystin-LR using sulfate radicals generated through photolysis, thermolysis and e transfer mechanisms. Appl Catal B Environ 96(3–4):290–298CrossRefGoogle Scholar
  4. Antoniou MG, De La Cruz AA, Dionysiou DD (2010) Intermediates and reaction pathways from the degradation of microcystin-LR with sulfate radicals. Environ Sci Technol 44(19):7238–7244CrossRefGoogle Scholar
  5. Buxton GV, Bydder M, Salmon GA (1999) The reactivity of chlorine atoms in aqueous solution. Part II. The equilibrium SO4·− + Cl reversible arrow Cl· + SO4 2−. Phys Chem Chem Phys 1(2):269–273CrossRefGoogle Scholar
  6. Cao JS et al (2008) Oxidation of lindane with Fe(II)-activated sodium persulfate. Environ Eng Sci 25(2):221–228CrossRefGoogle Scholar
  7. Choi KH, Lee WJ (2012) Enhanced degradation of trichloroethylene in nano-scale zero-valent iron Fenton system with Cu(II). J Hazard Mater 211–212(15):146–153CrossRefGoogle Scholar
  8. Criquet J, Vel Leitner NK (2009) Degradation of acetic acid with sulfate radical generated by persulfate ions photolysis. Chemosphere 77(2):194–200CrossRefGoogle Scholar
  9. Gayathri P, Dorathi RPJ, Palanivelu K (2010) Sonochemical degradation of textile dyes in aqueous solution using sulphate radicals activated by immobilized cobalt ions. Ultrason Sonochem 17(3):566–571CrossRefGoogle Scholar
  10. Ghauch A, Tuqan AM (2012) Oxidation of bisoprolol in heated persulfate/H2O system: kinetics and products. Chem Eng J 183(15):162–171CrossRefGoogle Scholar
  11. Guan YH et al (2011) Influence of pH on the formation of sulfate and hydroxyl radicals in the UV/peroxymonosulfate system. Environ Sci Technol 45(21):9308–9314CrossRefGoogle Scholar
  12. Hussain I et al (2012) Degradation of p-chloroaniline by persulfate activated with zero-valent iron. Chem Eng J 203:269–276CrossRefGoogle Scholar
  13. Johnson RL, Tratnyek PG, Johnson RO (2008) Persulfate persistence under thermal activation conditions. Environ Sci Technol 42(24):9350–9356CrossRefGoogle Scholar
  14. Li Y, Bachas LG, Bhattacharyya D (2005) Kinetic studies of trichlorophenol destruction by chelate-based Fenton reaction. Envion Eng Sci 22(6):756–771CrossRefGoogle Scholar
  15. Liang CJ et al (2004a) Persulfate oxidation for in situ remediation of TCE. I. Activated by ferrous ion with and without a persulfate-thiosulfate redox couple. Chemosphere 55(9):1213–1223CrossRefGoogle Scholar
  16. Liang CJ et al (2004b) Persulfate oxidation for in situ remediation of TCE. II. Activated by chelated ferrous ion. Chemosphere 55(9):1225–1233CrossRefGoogle Scholar
  17. Liang CJ et al (2007a) Hydroxypropyl-β-cyclodext-rin-mediated iron-activated persulfate oxidation of trichloroethylene and tetrachloroethylene. Ind Eng Chem Res 46:6466–6479CrossRefGoogle Scholar
  18. Liang CJ, Wang ZS, Bruell CJ (2007b) Influence of pH on persulfate oxidation of TCE at ambient temperatures. Chemosphere 66(1):106–113CrossRefGoogle Scholar
  19. Lin AY et al (2010) Potential for biodegradation and sorption of acetaminophen, caffeine, propranolol and acebutolol in lab-scale aqueous environments. J Hazard Mater 183(1–3):242–250CrossRefGoogle Scholar
  20. Lucking F et al (1998) Iron powder and graphite and activated carbon as catalyst for the oxidation of 4-chlorophenol with hydrogen peroxide in aqueous solution. Water Res 32(9):2607–2614CrossRefGoogle Scholar
  21. Matta R et al (2011) Removal of carbamazepine from urban wastewater by sulfate radical oxidation. Environ Chem Lett 9(3):347–353CrossRefGoogle Scholar
  22. Mora VC et al (2009) Thermally activated peroxydisulfate in the presence of additives: a clean method for the degradation of pollutants. Chemosphere 75(10):1405–1409CrossRefGoogle Scholar
  23. Neppolian B, Doronila A, Ashokkumar M (2010) Sonochemical oxidation of arsenic(III) to arsenic(V) using potassium peroxydisulfate as an oxidizing agent. Water Res 44(12):3687–3695CrossRefGoogle Scholar
  24. Nfodzo P, Choi H (2011) Triclosan decomposition by sulfate radicals: effects of oxidant and metal doses. Chem Eng J 174(2–3):629–634CrossRefGoogle Scholar
  25. Oh SY et al (2009) Oxidation of polyvinyl alcohol by persulfate activated with heat, Fe2+, and zero-valent iron. J Hazard Mater 168(1):346–351CrossRefGoogle Scholar
  26. Oh SK, Kang SG, Chiu PC (2010) Degradation of 2.4-dinitrotoluene by persulfate activated with zero-valent iron. Sci Total Environ 408(16):2464–3468CrossRefGoogle Scholar
  27. Rastogi A, Al-Abed SR, Dionysiou DD (2009a) Effect of inorganic, synthetic and naturally occurring chelating agents on Fe(II) mediated advanced oxidation of chlorophenols. Water Res 43(3):684–694CrossRefGoogle Scholar
  28. Rastogi A, Al-Abed SR, Dionysiou DD (2009b) Sulfate radical-based ferrous-peroxymonosulfate oxidative system for PCBs degradation in aqueous and sediment systems. Appl Catal B Environ 85(3–4):171–179CrossRefGoogle Scholar
  29. Romero A et al (2010) Diuron anatement using acitvated persulfate: effect of pH, Fe(II) and oxidant dosage. Chem Eng J 162(1):257–265CrossRefGoogle Scholar
  30. Sun JH et al (2009) Oxone/Co2+ oxidation as an advanced oxidation process: comparison with traditional Fenton oxidation for treatment of landfill leachate. Water Res 43(17):4363–4369CrossRefGoogle Scholar
  31. Tan CQ et al (2012a) Degradation of diuron by persulfate activated with ferrous ion. Sep Purif Technol 95(19):44–48CrossRefGoogle Scholar
  32. Tan CQ et al (2012b) Heat-activated persulfate oxidation of diuron in water. Chem Eng J 203(1):294–300CrossRefGoogle Scholar
  33. Verma PS, Saxena RC, Jayaraman A (1997) Cyclic voltammetric studies of certain industrially potential iron chelate catalysts. Fresenius’ J Anal Chem 357(1):56–60CrossRefGoogle Scholar
  34. Waldemer RH, Tratnyek PG, Johnson RL, Nurmi JT (2007) Oxidation of chlorinated ethenes by heat-activated persulfate: kinetics and products. Environ Sci Technol 41(3):1010–1015CrossRefGoogle Scholar
  35. Xu XR, Li XZ (2010) Degradation of azo dye Organge G in aqueous solutions by persulfate with ferrous ion. Sep Purif Technol 72:105–111CrossRefGoogle Scholar
  36. Zhang X et al (2008) Photodegradation of acetaminophen in TiO2 suspended solution. J Hazard Mater 157(2–3):300–307CrossRefGoogle Scholar
  37. Zhao JY et al (2010) Enhanced oxidation of 4-chlorophenol using sulfate radicals generated from zero-valent iron and peroxydisulfate at ambient temperature. Sep Purif Technol 71(3):302–307CrossRefGoogle Scholar
  38. Zhou T et al (2008) Oxidation of 4-chlorophenol in a heterogeneous zero valent iron/H2O2 Fenton-like system: kinetic, pathway and effect factors. Sep Purif Technol 62(3):551–558CrossRefGoogle Scholar

Copyright information

© Islamic Azad University (IAU) 2013

Authors and Affiliations

  • J. Deng
    • 1
  • Y. Shao
    • 1
    • 2
  • N. Gao
    • 1
  • Y. Deng
    • 3
  • C. Tan
    • 1
  • S. Zhou
    • 1
  1. 1.State Key Laboratory of Pollution Control ReuseTongji UniversityShanghaiChina
  2. 2.China Academy of Urban Planning and DesignBeijingChina
  3. 3.Department of Earth and Environmental StudiesMontclair State UniversityMontclairUSA

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