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Fe-Mn bi-metallic oxides loaded on granular activated carbon to enhance dye removal by catalytic ozonation

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Abstract

A Fe-Mn bi-metallic oxide supported on granular activated carbon (Fe-Mn GAC) has been fabricated by an impregnation-desiccation method and tested in the catalytic ozonation of methyl orange (MO) degradation and mineralization. X-ray diffraction, scanning electron microscopy, and Fourier transform infrared spectroscopy characterizations revealed that Fe-Mn oxides were successfully loaded and uniformly distributed on the GAC, and nitrogen adsorption isotherms showed that the supported GAC retained a large surface area and a high pore volume compared with the pristine GAC. The catalytic activity was systematically assessed by monitoring the MO removal efficiencies at different operational parameters, such as catalyst dosage, initial solution pH, and ozone flow rate. The Fe-Mn GAC exhibited better catalytic activity relative to ozone alone and GAC alone, improving the TOC removal by 24.5 and 11.5 % and COD removal by 13.6 and 7.3 %, respectively. The reusability of the hybrid was examined over five consecutive cyclic treatments. The Fe-Mn GAC catalytic activity was only a slight loss in the cycles, showing good stability. The addition of Na2CO3 as hydroxyl radicals (•OH) scavengers proved that the catalytic ozonation mechanism was the enhanced generation of •OH by the Fe-Mn GAC. The above results render the Fe-Mn GAC an industrially promising candidate for catalytic ozonation of dye contaminant removal.

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References

  • Alvarez PM, Masa FJ, Jaramillo J, Beltran FJ, Gomez-Serrano V (2008) Kinetics of ozone decomposition by granular activated carbon. Ind Eng Chem Res 47(8):2545–2553

    Article  CAS  Google Scholar 

  • Biniak S, Pakula M, Szymanski GS, Swiatkowski A (1999) Effect of activated carbon surface oxygen- and/or nitrogen-containing groups on adsorption of copper(II) ions from aqueous solution. Langmuir 15(18):6117–6122

    Article  CAS  Google Scholar 

  • Chen C, Chen H, Guo X, Guo S, Yan G (2014a) Advanced ozone treatment of heavy oil refining wastewater by activated carbon supported iron oxide. J Ind Eng Chem 20(5):2782–2791

    Article  CAS  Google Scholar 

  • Chen C, Wei L, Guo X, Guo S, Yan G (2014b) Investigation of heavy oil refinery wastewater treatment by integrated ozone and activated carbon-supported manganese oxides. Fuel Process Technol 124:165–173

    Article  CAS  Google Scholar 

  • Ding Z, Hu XJ, Lu GQ, Yue PL, Greenfield PF (2000) Novel silica gel supported TiO2 photocatalyst synthesized by CVD method. Langmuir 16(15):6216–6222

    Article  CAS  Google Scholar 

  • Domingo-Garcia M, Lopez-Garzon FJ, Perez-Mendoza M (2000) Effect of some oxidation treatments on the textural characteristics and surface chemical nature of an activated carbon. J Colloid Interface Sci 222(2):233–240

    Article  CAS  Google Scholar 

  • Fanning PE, Vannice MA (1993) A drifts study of the formation of surface groups on carbon by oxidation. Carbon 31(5):721–730

    Article  CAS  Google Scholar 

  • Galán J, Rodríguez A, Gómez JM, Allen SJ, Walker GM (2013) Reactive dye adsorption onto a novel mesoporous carbon. Chem Eng J 219:62–68

    Article  Google Scholar 

  • Garcia-segura S, Dosta S, Guilemany JM, Brillas E (2013) Solar photoelectrocatalytic degradation of Acid Orange 7 azo dye using a highly stable TiO2 photoanode synthesized by atmospheric plasma spray. Appl Catal B Environ 133:142–150

    Article  Google Scholar 

  • Garoma T, Matsumoto S (2009) Ozonation of aqueous solution containing bisphenol A: effect of operational parameters. J Hazard Mater 167(1–3):1185–1191

    Article  CAS  Google Scholar 

  • Gomes AC, Fernandes LR, Simões RMS (2012) Oxidation rates of two textile dyes by ozone: effect of pH and competitive kinetics. Chem Eng J 189-190:175–181

    Article  CAS  Google Scholar 

  • Gordon G, Rakness K, Vornehm D, Wood D (1989) Limitations of the iodometric determination of ozone. J Am Water Works Assoc 81(6):72–76

    Google Scholar 

  • Hao L, Huiping D, Jun S (2012) Activated carbon and cerium supported on activated carbon applied to the catalytic ozonation of polycyclic aromatic hydrocarbons. J Mol Catal A Chem 363–364:101–107

    Article  Google Scholar 

  • Heisig C, Zhang W, Oyama ST (1997) Decomposition of ozone using carbon-supported metal oxide catalysts. Appl Catal B Environ 14(1):117–129

    Article  CAS  Google Scholar 

  • Huang Y, Cui C, Zhang D, Li L, Pan D (2015a) Heterogeneous catalytic ozonation of dibutyl phthalate in aqueous solution in the presence of iron-loaded activated carbon. Chemosphere 119:295–301

    Article  CAS  Google Scholar 

  • Huang H, Xiao D, Liu J H, Hou L, Ding L (2015b) Recovery and removal of nutrients from swine wastewater by using a novel integrated reactor for struvite decomposition and recycling. Sci Rep 5, 10183, doi:10.1038/srep10183

  • Huang H, Liu J, Xiao J, Zhang P, Gao F (2016) Highly efficient recovery of ammonium nitrogen from coking wastewater by coupling struvite precipitation and microwave radiation technology. ACS Sustain Chem Eng doi:10.1021/acssuschem

  • Ji S, Li X, Ren Y, Chen T, Cen K, Ni M, et al. (2013) Ozone-enhanced oxidation of PCDD/Fs over V2O5-TiO2-based catalyst. Chemosphere 92(3):265–272

    Article  CAS  Google Scholar 

  • Legube B, Karpel Vel Leitner N (1999) Catalytic ozonation: a promising advanced oxidation technology for water treatment. Catal Today 53(1):61–72

    Article  CAS  Google Scholar 

  • Lei L, Gu L, Zhang X, Su Y (2007) Catalytic oxidation of highly concentrated real industrial wastewater by integrated ozone and activated carbon. Appl Catal A Gen 327(2):287–294

    Article  CAS  Google Scholar 

  • Ling W, Qiang Z, Shi Y, Zhang T, Dong B (2011) Fe(III)-loaded activated carbon as catalyst to improve omethoate degradation by ozone in water. J Mol Catal A Chem 342-343:23–29

    Article  CAS  Google Scholar 

  • Liu S, Huang J, Ye Y, Zhang A, Pan L, Chen X (2013) Microwave enhanced Fenton process for the removal of methylene blue from aqueous solution. Chem Eng J 215-216:586–590

    Article  CAS  Google Scholar 

  • Lopez-Garzon FJ, Domingo-Garcia M, Perez-Mendoza M, Alvarez PM, Gomez-Serrano V (2003) Textural and chemical surface modifications produced by some oxidation treatments of a glassy carbon. Langmuir 19(7):2838–2844

    Article  CAS  Google Scholar 

  • Ma J, Sui M, Zhang T, Guan C (2005) Effect of pH on MnOx/GAC catalyzed ozonation for degradation of nitrobenzene. Water Res 39(5):779–786

    Article  CAS  Google Scholar 

  • Maddila S, Dasireddy V (2013) Ozone initiated dechlorination and degradation of trichlorophenol using Ce-Zr loaded metal oxides as catalysts. Appl Catal B Environ 143:129–141

    Article  Google Scholar 

  • Mangun CL, Benak KR, Economy J, Foster KL (2001) Surface chemistry, pore sizes and adsorption properties of activated carbon fibers and precursors treated with ammonia. Carbon 39(12):1809–1820

    Article  CAS  Google Scholar 

  • Nawrocki J, Kasprzyk-Hordern B (2010) The efficiency and mechanisms of catalytic ozonation. Appl Catal B Environ 99(1–2):27–42

    Article  CAS  Google Scholar 

  • Oliveira TF, Chedeville O, Cagnon B, Fauduet H (2011) Degradation kinetics of DEP in water by ozone/activated carbon process: influence of pH. Desalination 269(1–3):271–275

    Article  Google Scholar 

  • Purkait MK, Maiti A, DasGupta S, De S (2007) Removal of congo red using activated carbon and its regeneration. J Hazard Mater 145(1–2):287–295

    Article  CAS  Google Scholar 

  • Ren Y, Dong Q, Feng J, Ma J, Wen Q, Zhang M (2012) Magnetic porous ferrospinel NiFe2O4: a novel ozonation catalyst with strong catalytic property for degradation of di-n-butyl phthalate and convenient separation from water. J Colloid Interface Sci 382(1):90–96

    Article  CAS  Google Scholar 

  • Sabate J, Anderson MA, Kikkawa H, Xu Q, Cerveramarch S, Hill CG (1992) Nature and properties of pure and nb-doped TiO2 ceramic membranes affecting the photocatalytic degradation of 3-chlorosalicylic acid as a model of halogenated organic-compounds. J Catal 134(1):36–46

    Article  CAS  Google Scholar 

  • Sanchez-Polo A, Rivera-Utrilla J (2003) Effect of the ozone-carbon reaction on the catalytic activity of activated carbon during the degradation of 1,3,6-naphthalenetrisulphonic acid with ozone. Carbon 41(2):303–307

    Article  CAS  Google Scholar 

  • Sánchez-Polo M, von Gunten U, Rivera-Utrilla J (2005) Efficiency of activated carbon to transform ozone into OH radicals: influence of operational parameters. Water Res 39(14):3189–3198

    Article  Google Scholar 

  • Saroj S, Kumar K, Pareek N, Prasad R, Singh RP (2014) Biodegradation of azo dyes acid red 183, direct blue 15 and direct red 75 by the isolate Penicillium oxalicum SAR-3. Chemosphere 107:240–248

    Article  CAS  Google Scholar 

  • Shukla PR, Wang SB, Sun HQ, Ang HM, Tade M (2010) Activated carbon supported cobalt catalysts for advanced oxidation of organic contaminants in aqueous solution. Appl Catal B Environ 100(3–4):529–534

    Article  CAS  Google Scholar 

  • Tang S, Lu N, Li J, Shang K, Wu Y (2013) Improved phenol decomposition and simultaneous regeneration of granular activated carbon by the addition of a titanium dioxide catalyst under a dielectric barrier discharge plasma. Carbon 53:380–390

    Article  CAS  Google Scholar 

  • Torimoto T, Okawa Y, Takeda N, Yoneyama H (1997) Effect of activated carbon content in TiO2-loaded activated carbon on photodegradation behaviors of dichloromethane. J Photochem Photobiol A 103(1–2):153–157

    Article  CAS  Google Scholar 

  • Umar M, Roddick F, Fan LH, Aziz HA (2013) Application of ozone for the removal of bisphenol A from water and wastewater—a review. Chemosphere 90(8):2197–2207

    Article  CAS  Google Scholar 

  • Wang M, Zhang P, Li J, Jiang C (2014) The effects of Mn loading on the structure and ozone decomposition activity of MnOx supported on activated carbon. Chin J Catal 35(3):335–341

    Article  CAS  Google Scholar 

  • Wu C, Kuo C, Chang C (2008) Homogeneous catalytic ozonation of C.I. Reactive Red 2 by metallic ions in a bubble column reactor. J Hazard Mater 154(1–3):748–755

    Article  CAS  Google Scholar 

  • Wu J, Gao H, Yao S, Chen L, Gao Y, Zhang H (2015) Degradation of Crystal Violet by catalytic ozonation using Fe/activated carbon catalyst. Sep Purif Technol 147:179–185

    Article  CAS  Google Scholar 

  • Xing L, Xie Y, Minakata D, Cao H, Xiao J, Zhang Y, et al. (2014) Activated carbon enhanced ozonation of oxalate attributed to HO oxidation in bulk solution and surface oxidation: effect of activated carbon dosage and pH. J Environ Sci 26(10):2095–2105

    Article  Google Scholar 

  • Zeng Y, Hong PKA, Wavrek DA (2000) Chemical–biological treatment of pyrene. Water Res 34(4):1157–1172

    Article  Google Scholar 

  • Zhang H, Ji L, Wu F, Tan J (2005) In situ ozonation of anthracene in unsaturated porous media. J Hazard Mater 120(1–3):143–148

    Article  CAS  Google Scholar 

  • Zhang Q, Li C, Li T (2013) Rapid photocatalytic decolorization of methylene blue using high photon flux UV/TiO2/H2O2 process. Chem Eng J 217:407–413

    Article  CAS  Google Scholar 

  • Zhao H, Gao J, Zhao G, Fan J, Wang Y, Wang Y (2013) Fabrication of novel SnO2-Sb/carbon aerogel electrode for ultrasonic electrochemical oxidation of perfluorooctanoate with high catalytic efficiency. Appl Catal B Environ 136-137:278–286

    Article  CAS  Google Scholar 

Download references

Acknowledgments

The authors acknowledge the financial support supplied by the Natural Science Foundation of Hebei Province, P. R. China (Project Nos. B2015203303 and B2015203300), the China Postdoctoral Science Foundation (Project No. 2015M580216), the Youth Teacher Independent Research Program of Yanshan University (Project Nos. 15LGA013 and 14LGB021), and the Doctoral Foundation Program of Yanshan University (Project Nos. B849 and B878).

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Correspondence to Deling Yuan.

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Communicated by: Vítor Pais Vilar

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Tang, S., Yuan, D., Zhang, Q. et al. Fe-Mn bi-metallic oxides loaded on granular activated carbon to enhance dye removal by catalytic ozonation. Environ Sci Pollut Res 23, 18800–18808 (2016). https://doi.org/10.1007/s11356-016-7030-5

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