Abstract
The mechanism of methylene blue (MB) oxidation initiated by hydroxyl radicals (·OH) in a gas–liquid multiphase plasma reactor was investigated. Direct current corona plasma was applied to produce ·OH. The effects of liquid solution pH and plasma-forming gas components (air, N2, He, CO2) were evaluated. The removal of MB exceeded 90 % after 3 h of treatment under an air atmosphere at neutral pH, and it was shown to be mainly through the function of ·OH. Further experiments demonstrated that ·OH was mainly produced through electron-molecule collision processes. The energy efficiency of the process was assessed to be as high as 3.8 × 10−3 mol/kWh when the removal of MB reached 95.7 %. This high value was due to the countless liquid droplets greatly increasing the contact surface area. The results using CO2 as the forming gas indicated that the carbonate in solution has a negative effect on the generation of ·OH.
Similar content being viewed by others
References
Lee CH, Lee YH, Yoon JY (2006) Oxidative degradation of dimethylsulfoxide by locally concentrated hydroxyl radicals in streamer corona discharge process. Chemosphere 65:1163–1170
Shi JW, Bian WJ, Yin XL (2009) Organic contaminants removal by the technique of pulsed high-voltage discharge in water. J Hazard Mater 171:924–931
Zhang X, Feng W, Yu Z, Li S, Zhu J, Yan K (2013) Comparison of styrene removal in air by positive and negative DC corona discharges. Int J Environ Sci Technol 10:1377–1382
Zhang Y, Zhou MH, Lei LC (2007) Degradation of 4-chlorophenol in different gas–liquid electrical discharge reactors. Chem Eng J 132:325–333
Liao XB, Guo YF, He JH, Ou WJ, Ye DQ (2010) Hydroxyl radicals formation in dielectric barrier discharge during decomposition of toluene. Plasma Chem Plasma Process 30:841–853
Robert DB, Olga D (2006) The “Somersault” mechanism for the P-450 hydroxylation of hydrocarbons. The intervention of transient inverted metastable hydroperoxides. J Am Chem Soc 128:474–1488
Ryo O, Tetsuji O (2002) Measurement of hydroxyl radicals in pulsed corona discharge. J Electrost 55:333–342
Malik MA (2003) Synergistic effect of plasma catalyst and ozone in a pulsed corona discharge reactor on the decomposition of organic pollutants in water. Plasma Sources Sci Technol 12:S26–S32
Muhammad AM (2010) Water purification by plasmas: which reactors are most energy efficient. Plasma Chem Plasma Process 30:21–31
Sugiarto AT, Sato M (2001) Pulsed plasma processing of organic compounds in aqueous solution. Thin Solid Films 386:295–299
Malik MA, Ghaffer AG, Malik SA (2001) Water purification by electrical discharges. Plasma Sources Sci Technol 10:82–91
Sunka P (2001) Pulse electrical discharges in water and their applications Phys Plasma 8:2587–2594
Handa T, Minamitani Y (2009) The effect of a water-droplet spray and gas discharge in water treatment by pulsed power. IEEE Trans Plasma Sci 37:179–183
Minamitani Y, Shoji S, Ohba Y, Higashiyama Y (2008) Decomposition of dye in water solution by pulsed power discharge in a water droplet spray. IEEE Trans Plasma Sci 36:2586–2591
Lindsay HR, Geoffrey DS (2009) The importance of phase in the radical-initiated oxidation of model organic aerosols: reactions of solid and liquid brassidic acid particles. Phys Chem Chem Phys 11:2441–2451
Atkinson R (1997) Evaluated kinetic and photochemical data for atmospheric chemistry: supplement VI—IUPAC subcommittee on gas kinetic data evaluation for atmospheric chemistry. J Phys Chem Ref Data 26:215–290
John DH, Amanda JL, Geoffrey DS (2005) Ozonolysis of oleic acid particles: evidence for a surface reaction and secondary reactions involving Criegee intermediates. Phys Chem Chem Phys 7:501–511
Alexander L, Hai W, William HR, James PC, Michael JE, Barbara JF (2006) A new approach to determining gas-particle reaction probabilities and application to the heterogeneous reaction of deliquesced sodium chloride particles with gas-phase hydroxyl radicals. J Phys Chem A 110:10619–10627
Zou F, Wu ZC, Kang Y, Ma XJ (2010) Electrochemical process of heteroatom degradation by DC corona discharge. CIESC J 61:91–95
Li FS, Li JY (2004) To determination ozone in drinking water with the method of spectrophotometry. J Environ Occup Med 4:318–319
APHA, AWWA, WEF (1998) Standard methods for the examination of water and wastewater. American Public Health Association, Washington
Nosaka Y, Ohtaka K, Kitazawa M, Kishioka S, Nosaka AY (2009) Spin-trapping ESR detection of OH radicals generated in the electrode reactions for PEFCs. Electrochem Solid State Lett 2:B14–B17
Brisset JL, Mousa D, Doubla A, Hnatiuc E, Hnatiuc B, Youbi GK, Herry JM, Naitali M (2008) Chemical reactivity of discharges and temporal post-discharges in plasma treatment of aqueous media: examples of gliding discharge treated solutions. Ind Eng Chem Res 47:5761–5781
Parkansky N, Yakubov V, Simon EF, Alterkop BA, Boxman RL, Berkh O (2014) Removal of methylene blue from aging water solutions treated by a submerged arc. Plasma Chem Plasma Process 4:745–754
Merouani DR, Abdelmalek F, Ghezzar MR, Semmoud A, Addou A, Brisset JL (2013) Influence of peroxynitrite in gliding arc discharge treatment of alizarin Red S and postdischarge effects. Ind Eng Chem Res 52:1471–1480
Dockery KP, Sieber KD, Knapp FA, Wilson TE (2007) Surface acid chemistry associated with dielectric barrier discharge (DBD) treatment of polyethylene. Plasma Sources Sci Technol 1:42–49
Kang Y (2008) Artificial generation of oxidative radicals for the abatement of gaseous pollutants and its mechanism. Hangzhou, China
Liu YG (2013) Time-resolved emission spectroscopy characteristics of dielectric barrier discharges in atmospheric-pressure noble gases. Guangzhou, China
Wang HJ, Li J, Quan X, Wu Y, Li GF, Wang FZ (2007) Formation of hydrogen peroxide and degradation of phenol in synergistic system of pulsed corona discharge combined with TiO2 photocatalysis. J Hazard Mater 141:336–343
Benstaali B, Boubert P, Cheron BG, Addou A, Brisset JL (2002) Density and rotational temperature measurements of the ·OH ·NO radicals produced by a gliding arc in humid air. Plasma Chem Plasma P 4:553–571
Doubla A, Bello LB, Fotso M, Brisset JL (2008) Plasmachemical decolourisation of Bromothymol Blue by gliding electric discharge at atmospheric pressure. Dyes Pigments 77:118–124
Cong YQ, Wu ZC (2007) Electrocatalytic generation of radical intermediates over lead dioxide electrode doped with fluoride. J Phys Chem C 8:3442–3446
David M, Doubla A, Youbi GK, Brisset JL (2007) Postdischarge long life reactive intermediates involved in the plasma chemical degradation of an azoic dye. IEEE Trans Plasma Sci 2:444–453
Kang Y, Wu ZC (2008) Formation of hydroxyl radicals and oxidation of toluene under corona discharge with water vapor as radical source. Chin Bull 14:2248–2252
Peter L, Bruce RL (2005) Plasma chemical oxidation processes in a hybrid gas-liquid electrical discharge reactor. J Phys D Appl Phys 38:4074–4081
Oumghar A, Legrand JC, Diamy AM, Turillon N (1995) Methane conversion by an air microwave plasma. Plasma Chem Plasma Process 15:87–107
Magne L, Pasquiers S, Blin-Simiand N, Postel C (2007) Production and reactivity of the hydroxyl radical in homogeneous high pressure plasmas of atmospheric gases containing traces of light olefins. J Phys D Appl Phys 40:3112–3127
Ono R, Oda T (2008) Measurement of gas temperature and OH density in the afterglow of pulsed positive corona discharge. J Phys D Appl Phys 41:1–11
Mededovic S, Locke BR (2007) Primary chemical reactions in pulsed electrical discharge channels in water. J Phys D Appl Phys 40:7734–7746
Bonilla KAS, Souza AAU, Souza SMAGU (2010) Removal of COD and color from hydrolyzed textile azo dye by combined ozonation and biological treatment. J Hazard Mater 179:35–42
Soares OSGP, Orfao JJM, Portela D, Vieira A (2006) Ozonation of textile effluents and dye solutions under continuous operation: influence of operating parameters. J Hazard Mater B 137:1664–1673
Cope VW, Chen SN, Hoffman MZ (1973) Intermediates in the photochemistry of carbonato-amine complexes of cobalt (III). CO3·− radicals and the aquocarbonato complex. J Am Chem Soc 95:3116–3121
Janele G, Joseph JP, William AM (2010) Effect of halide ions and carbonates on organic contaminant degradation bu hydroxyl radical-based advanced oxidation processes in saline waters. Environ Sci Technol 44:6822–6828
Acknowledgments
This work is financially supported by the National NSFC (21073161, 21173188, 21473158) and partially 863 Program (2013AA065900).
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Liu, X., Zhang, H., Qin, D. et al. Radical-Initiated Decoloration of Methylene Blue in a Gas–Liquid Multiphase System Via DC Corona Plasma. Plasma Chem Plasma Process 35, 321–337 (2015). https://doi.org/10.1007/s11090-014-9606-5
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11090-014-9606-5