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Synthesis of magnetic CoFe2O4/ordered mesoporous carbon nanocomposites and application in Fenton-like oxidation of rhodamine B

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Abstract

CoFe2O4/ordered mesoporous carbon (OMC) nanocomposites were synthesized and tested as heterogeneous peroxymonosulfate (PMS) activator for the removal of rhodamine B. Characterization confirmed that CoFe2O4 nanoparticles were tightly bonded to OMC, and the hybrid catalyst possessed high surface area, pore volume, and superparamagnetism. Oxidation experiments demonstrated that CoFe2O4/OMC nanocomposites displayed favorable catalytic activity in PMS solution and rhodamine B degradation could be well described by pseudo-first-order kinetic model. Sulfate radicals (SO4 ·) were verified as the primary reactive species which was responsible for the decomposition of rhodamine B. The optimum loading ratio of CoFe2O4 and OMC was determined to be 5:1. Under optimum operational condition (catalyst dosage 0.05 g/L, PMS concentration 1.5 mM, pH 7.0, and 25 °C), CoFe2O4/OMC-activated peroxymonosulfate system could achieve almost complete decolorization of 100 mg/L rhodamine B within 60 min. The enhanced catalytic activity of CoFe2O4/OMC nanocomposites compared to that of CoFe2O4 nanoparticles could be attributable to the increased adsorption capacity and accelerated redox cycles between Co(III)/Co(II) and Fe(III)/Fe(II).

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References

  • Albuquerque LF, Salgueiro AA, Melo JLD, Chiavone O (2013) Coagulation of indigo blue present in dyeing wastewater using a residual bittern. Sep Purif Technol 104:246–249

    Article  CAS  Google Scholar 

  • Anipsitakis GP, Diounysiou DD (2004) Transition metal/UV-based advanced oxidation technologies for water decomposition. Appl Catal B Environ 54:155–163

    Article  CAS  Google Scholar 

  • Bo XJ, Zhang YF, Li M, Nsabimana A, Guo LP (2015) NiCo2O4 spinel/ordered mesoporous carbons as noble-metal free electrocatalysts for oxygen reduction reaction and the influence of structure of catalyst support on the electrochemical activity of NiCo2O4. J Power Sources 288:1–8

    Article  CAS  Google Scholar 

  • Chu WH, Li DM, Gao NY, Templeton MR, Tan CQ, Gao YQ (2015) The control of emerging haloacetamide DBP precursors with UV/persulfate treatment. Water Res 72:340–348

    Article  CAS  Google Scholar 

  • Deng J, Shao YS, Gao NY, Deng Y, Tan CQ, Zhou SQ, Hu XH (2012) Multiwalled carbon nanotubes as adsorbents for removal of herbicide diuron from aqueous solution. Chem Eng J 193-194:339–347

    Article  CAS  Google Scholar 

  • Deng J, Shao YS, Gao NY, Deng Y, Zhou SQ, Hu XH (2013a) Thermally activated persulfate (TAP) oxidation of antiepileptic drug carbamazepine in water. Chem Eng J 228:765–771

    Article  CAS  Google Scholar 

  • Deng J, Shao YS, Gao NY, Tan CQ, Zhou SQ, Hu XH (2013b) CoFe2O4 magnetic nanoparticles as a highly active heterogeneous catalyst of oxone for the degradation of diclofenac in water. J Hazard Mater 262:836–844

    Article  CAS  Google Scholar 

  • Deng J, Shao YS, Gao NY, Xia SJ, Tan CQ, Zhou SQ, Hu XH (2013c) Degradation of the antiepileptic drug carbamazepine upon different UV-based advanced oxidation processes in water. Chem Eng J 222:150–158

    Article  CAS  Google Scholar 

  • Deng J, Feng SF, Ma XY, Tan CQ, Wang HY, Zhou SQ, Zhang TQ, Li J (2016) Heterogeneous degradation of Orange II with peroxymonosulfate activated by ordered mesoporous MnFe2O4. Sep Purif Technol 167:181–189

    Article  CAS  Google Scholar 

  • Deng J, Feng SF, Zhang KJ, Li J, Wang HY, Zhang TQ, Ma XY (2017) Heterogeneous activation of peroxymonosulfate using ordered mesoporous Co3O4 for the degradation of chloramphenicol at neutral pH. Chem Eng J 308:505–515

    Article  CAS  Google Scholar 

  • Du YC, Ma WJ, Liu PX, Zou BH, Ma J (2016) Magnetic CoFe2O4 nanoparticles supported on titanate nanotubes (CoFe2O4/TNTs) as a novel heterogeneous catalyst for peroxymonosulfate activation and degradation of organic pollutants. J Harzard Mater 308:58–66

    Article  CAS  Google Scholar 

  • EI-Ashtoukhy ESZ, Amin NK (2010) Removal of acid green dye 50 from wastewater by anodic oxidation and electrocoagulation—a comparative study. J Hazard Mater 179:113–119

    Article  Google Scholar 

  • Furman O, Teel A, Watts RJ (2010) Mechanism of base activation of persulfate. Environ Sci Technol 44:6423–6428

    Article  CAS  Google Scholar 

  • Gao J, Wang XY, Zhang YW, Liu J, Lu Q, Chen MF, Bai YS (2016) Preparation and supercapacitive performance of nanosized manganese dioxide/ordered mesoporous carbon composites. Electrochim Acta 192:234–242

    Article  CAS  Google Scholar 

  • Garrido-Ramirez 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

    Article  CAS  Google Scholar 

  • Goscianska J, Marciniak M, Pietrzak R (2015) Ordered mesoporous carbons modified with cerium as effective adsorbents for azo dyes removal. Sep Purif Technol 154:236–245

    Article  CAS  Google Scholar 

  • Guan YH, Ma J, Li XC, Fang JY, Chen LW (2011) Influence of pH on the formation of sulfate and hydroxyl radicals in the UV/Peroxymonosulfate system. Environ Sci Technol 45:9308–9314

    Article  CAS  Google Scholar 

  • Hassan H, Hameed BH (2011) Fe-clay as effective heterogeneous Fenton catalyst for the decolorization of reactive blue 4. Chem Eng J 171:912–918

    Article  CAS  Google Scholar 

  • Hu PD, Long MC (2016) Cobalt-catalyzed sulfate radical-based advanced oxidation: a review on heterogeneous catalysts and applications. Appl Catal B Environ 181:103–117

    Article  CAS  Google Scholar 

  • Hu LX, Yang F, Lu WC, Hao Y, Yuan H (2013) Heterogeneous activation of oxone with CoMg/SBA-15 for the degradation of dye Rhodamine B in aqueous solution. Appl Catal B Environ 134-135:7–18

    Article  CAS  Google Scholar 

  • Huang RH, Yan HH, Li LS, Deng DY, Shu YH, Zhang QY (2011) Catalytic activity of Fe/SBA-15 for ozonation of dimethyl phthalate in aqueous solution. Appl Catal B Environ 106:264–271

    CAS  Google Scholar 

  • Kornaros M, Lyberatos G (2006) Biological treatment of wastewater from a dye manufacturing company using a tricking filter. J Hazard Mater 136:95–102

    Article  CAS  Google Scholar 

  • Li NW, Zheng MB, Chang XF, Ji GB, Lu HL, Xue LP, Pan LJ, Cao JM (2011) Preparation of magnetic CoFe2O4-functionalized graphene sheets via a facile hydrothermal method and their adsorption properties. J Solid State Chem 184:953–968

    Article  CAS  Google Scholar 

  • Li SM, Wang B, Liu JH, Yu M (2014) In situ one-step synthesis of CoFe2O4/graphene nanocomposites as high-performance anode for lithium-ion batteries. Electrochim Acta 129:33–39

    Article  CAS  Google Scholar 

  • Li XN, Wang ZH, Zhang B, Rykov AI, Ahmed MA, Wang JH (2016) FexCo3-xO4 nanocages derived from nanoscale metal-organic frameworks for removal of bisphenol A by activation of peroxymonosulfate. Appl Catal B Environ 181:788–799

    Article  CAS  Google Scholar 

  • Lien HL, Zhang WX (2007) Nanoscale Pd/Fe bimetallic particles: catalytic effects of palladium on hydrodechlorination. Appl Catal B Environ 77:110–116

    Article  CAS  Google Scholar 

  • Lin KA, Chang H (2015) Zeolitic imidazole framework-67 (ZIF-67) as a heterogeneous catalyst to active peroxymonosulfate for degradation of Rhodamine B in water. J Taiwan Inst Chem E 53:40–45

    Article  CAS  Google Scholar 

  • Lin JY, Ye WY, Zeng HM, Yang H, Shen JN, Darvishmanesh S, Luis P, Sotto A, Bruggen BV (2015) Fractionation of direct dyes and salts in aqueous solution using loose nanofiltration membranes. J Membrane Sci 477:183–193

    Article  CAS  Google Scholar 

  • Liu SQ, Xiao B, Feng LR, Zhou SS, Chen ZG, Liu CB, Chen F, Wu ZY, Xu N, Oh WC, Meng ZD (2013) Graphene oxide enhances the Fenton-like photocatalytic activity of nickel ferrite for degradation of dyes visible light irradiation. Carbon 64:197–206

    Article  CAS  Google Scholar 

  • Liu ZZ, Yang SJ, Yuan YN, Xu J, Zhu YF, Li JJ, Wu F (2017) A novel heterogeneous system for sulfate radical generated through sulfite activation on a CoFe2O4 nanocatalyst surface. J Harzard Mater 324:583–592

    Article  CAS  Google Scholar 

  • Lou XY, Wu LX, Guo YG, Chen CC, Wang ZH, Xiao DX, Fang CL, Liu JS, Zhao JC, Lu SY (2014) Peroxymonosulfate activation by phosphate anion for organics degradation in water. Chemosphere 117:582–585

    Article  CAS  Google Scholar 

  • Neta P, Huie RE, Ross AB (1998) Rate constants for reactions of inorganic radicals in aqueous solution. J Phys Chem Ref Data 17:1027–1284

    Article  Google Scholar 

  • Peng XM, Hu FP, Dai HL, Xiong Q, Xu CH (2016) Study of the adsorption mechanisms of ciprofloxacin antibiotics onto graphitic ordered mesoporous carbons. J Taiwan Inst Chem E 65:472–481

    Article  CAS  Google Scholar 

  • Ryoo R, Joon SH, Kruk M, Jaroniec M (2001) Ordered mesoporous carbons. Adv Mater 13:677–681

    Article  CAS  Google Scholar 

  • Shi PH, Su RJ, Wan FZ, Zhu MC, Li DX, Xu SH (2012) Co3O4 nanocrystals on graphene oxide as a synergistic catalyst for degradation of Orange II in water by advanced oxidation technology based on sulfate radicals. Appl Catal B Environ 123-124:265–272

    Article  CAS  Google Scholar 

  • Shi PH, Dai XF, Zheng HG, Li DX, Yao WF, Hu CY (2014) Synergistic catalysis of Co3O4 and graphene oxide on Co3O4/GO catalysts for degradation of Orange II in water by advanced oxidation technology based on sulfate radicals. Chem Eng J 240:264–270

    Article  CAS  Google Scholar 

  • Shin DW, Sung D, Hong JS, Kim MW, Yoon SS, Song Y, Kim G, Hong S, Yoo J (2016) Observation of graphene grain boundaries through selective adsorption of rhodamine B using fluorescence microscopy. Carbon 108:72–78

    Article  CAS  Google Scholar 

  • Soumia F, Petrier C (2016) Effect of potassium monopersulfate (oxone) and operating parameters on sonochemical degradation of cationic dye in an aqueous solution. Ultrason Sonochem 32:343–347

    Article  CAS  Google Scholar 

  • Sponza DT (2006) Toxicity studies in a chemical dye production industry in Turkey. J Hazard Mater 138:438–447

    Article  CAS  Google Scholar 

  • Su SN, Guo WL, Leng YQ, Yi CL, Ma ZM (2013) Heterogeneous activation of Oxone by CoxFe3-xO4 nanocatalysts for degradation of rhodamine B. J Hazard Mater 244-245:736–742

    Article  CAS  Google Scholar 

  • Tan CQ, Gao NY, Deng Y, Deng J, Zhou SQ, Li J, Xin XY (2014) Radical induced degradation of acetaminophen with Fe3O4 magnetic nanoparticles as heterogeneous activator of peroxymonosulfate. J Hazard Mater 279:452–460

    Article  Google Scholar 

  • Tang WX, Yao MS, Deng YZ, Li XF, Han N, Wu XF, Chen YF (2016) Decoration of one-dimensional MnO2 with Co3O4 nanoparticles: a heterogeneous interface for remarkably promoting catalytic oxidation activity. Chem Eng J 306:709–718

    Article  CAS  Google Scholar 

  • Waclawek S, Grubel K, Cernik M (2015) Simple spectrophotometric determination of monopersulfate. Spectrochim Acta A 149:928–933

    Article  CAS  Google Scholar 

  • Wang SL, Zhou N (2016) Removal of carbamazepine from aqueous solution using sono-activated persulfate process. Ultrason Sonochem 29:156–162

    Article  Google Scholar 

  • Wang YB, Zhao HY, Zhao GH (2015) Iron-copper bimetallic nanoparticles embedded within ordered mesoporous carbon as effective and stable heterogeneous Fenton catalyst for the degradation of organic contaminants. Appl Catal B Envion 164:396–406

    Article  CAS  Google Scholar 

  • Wei W, Yu C, Zhao QF, Qian XF, Li GS, Wan Y (2014) Synergy effect in photodegradation of contaminants from water using ordered mesoporous carbon-based titania catalyst. Appl Catal B Environ 146:151–161

    Article  CAS  Google Scholar 

  • Wei GL, Liang XL, He ZS, Liao YS, Xie ZY, Liu P, Ji SC, He HP, Li DQ, Zhang J (2015) Heterogeneous activation of Oxone by substituted magnetites Fe3-xMxO4 (Cr, Mn, Co, Ni) for degradation of acid orange II at neutral pH. J Mol Catal A Chem 398:86–94

    Article  CAS  Google Scholar 

  • Xu LJ, Chu W, Gan L (2015) Environmental application of graphene-based CoFe2O4 as an activator of peroxymonosulfate for the degradation of a plasticizer. Chem Eng J 263:435–443

    Article  CAS  Google Scholar 

  • Yao YJ, Cai YM, Lu F, Wei FY, Wang XY, Wang SB (2014) Magnetic recoverable MnFe2O4 and MnFe2O4-graphene hybrid as heterogeneous catalysts of peroxymonosulfate activation for efficient degradation of aqueous organic pollutants. J Harzard Mater 270:61–70

    Article  CAS  Google Scholar 

  • Zhang J, Shao XT, Shi C, Yang SY (2013) Decolorization of acid orange 7 with peroxymonosulfate oxidation catalyzed by granular activated carbon. Chem Eng J 232:259–265

    Article  CAS  Google Scholar 

  • Zhao DY, Feng JL, Huo QS, Melosh N, Fredrickson GH, Chmelka BF, Stucky GD (1998) Triblock copolymer syntheses of mesoporous silica with periodic 50 to 300 angstrom pores. Science 279:548–552

    Article  CAS  Google Scholar 

  • Zhao HY, Qian L, Guan XH, Wu DL, Zhao GH (2016) Continuous bulk FeCuC aerogel with ultradispersed metal nanoparticles: an efficient 3D heterogeneous electro-Fenton cathode over a wide range of pH 3-9. Environ Sci Technol 50(10):5225–5233

    Article  CAS  Google Scholar 

  • Zubir NA, Yacou C, Motuzas J, Zhang XW, Costa JCD (2014) Structural and functional investigation of graphene oxide-Fe3O4 nanocomposites for the heterogeneous Fenton-like reaction. Sci Rep 4:1–8

    Google Scholar 

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Acknowledgments

The authors would like to acknowledge the financial support from the National Natural Science Foundation of China (51508509, 51678527), the China Postdoctoral Science Foundation (2015M581936), and the Zhejiang Provincial Natural Science Foundation of China (LY15E080019).

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Correspondence to Jun Li.

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Responsible editor: Vítor Pais Vilar

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Deng, J., Chen, YJ., Lu, YA. et al. Synthesis of magnetic CoFe2O4/ordered mesoporous carbon nanocomposites and application in Fenton-like oxidation of rhodamine B. Environ Sci Pollut Res 24, 14396–14408 (2017). https://doi.org/10.1007/s11356-017-8941-5

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