Journal of Korean Society of Environmental Engineers (대한환경공학회지)

Korean Society of Environmental Engineers (대한환경공학회)
권호 표지

Effects of Operating Parameters on Phenol Degradation by Pulsed Corona Discharges in Aqueous Solutions

펄스 코로나 방전에 의한 페놀 분해에 미치는 운전변수의 영향

  • Chung, Jae-Woo (Department of Environmental Engineering, Jinju National University) ;
  • Moon, Ji-Hoon (Department of Environmental Engineering, Jinju National University) ;
  • Park, Eun-Ok (Department of Environmental Engineering, Jinju National University)
  • 정재우 (국립진주산업대학교 환경공학과) ;
  • 문지훈 (국립진주산업대학교 환경공학과) ;
  • 박은옥 (국립진주산업대학교 환경공학과)
  • Received : 2009.10.27
  • Accepted : 2010.01.04
  • Published : 2010.01.31
Download PDF
⟨ Previous Next ⟩

Abstract

Effects of operating parameters such as applied voltage, solution conductivity, ferrous ion concentration, electrode material on phenol degradation by pulsed corona discharges were investigated in laboratory scale experiments. The increase of applied voltage enhanced the phenol degradation by generating more energetic electrons. The solution conductivity inversely affected phenol removal rate in the tested ranges because the increase of conductivity decreased the electric field strength through the liquid phase. The addition of ferrous sulfate promoted the phenol degradation through the OH radical production by the Fentonlike reactions between ferrous ion and hydrogen peroxide generated by pulsed corona discharges. Catechol and hydroquinone were detected as primary intermediates of phenol degradation and the decrease of pH and the increase of conductivity were observed probably due to the generation of organic acids. Almost all of the initial phenol was disappeared and 29% of total organic corbon (TOC) was removed in the condition of 0.5 mM of ferrous sulfate after approximately 230 kJ of discharge energy transferred to the reactor.

펄스 코로나 방전에서 인가전압, 용액 전도도, 전극 재질, 철염 주입 등의 운전변수가 페놀 분해에 미치는 영향에 관해 실험실 규모의 실험을 수행하였다. 인가전압이 증가할수록 높은 에너지를 가진 전자들에 의한 물 분자의 충돌분해 반응에 의한 OH 라디칼 생성량이 증가하므로 페놀 분해 속도를 증가시키며 실험된 조건에서의 용액 전도도 증가는 용액을 통한 전기장 강도를 감소시켜 페놀 분해 속도를 낮추는 것으로 나타났다. 방전 반응기로 주입된 철염($FeSO_4$)은 방전에 의해 생성된 과산화수소와 펜톤 유사 반응을 통해 OH 라디칼을 생성시켜 페놀 분해를 증가시키는 것으로 나타났다. 펄스 코로나 방전에 의한 페놀 분해의 중간 생성물질로 catechol과 hydroquinone이 검출되었으며 분석을 수행하지는 않았으나 유기산의 생성으로 인해 pH가 감소되고 전도도가 증가하는 현상이 관찰되었다. 철염이 주입된 조건에서 백금 전극은 3가 철이온($Fe^{3+}$)을 2가 철이온($Fe^{2+}$)으로 환원시킴으로써 페놀 분해 속도를 증가시키는 것으로 나타났다. 산제일철($FeSO_4$) 0.5 mM이 주입된 조건에서 약 230 kJ의 방전 에너지가 유입될 때 거의 모든 페놀이 분해되었으며 약 29%의 총유기탄소(TOC) 제거효율을 얻을 수 있었다.

Keywords

References

  1. Muhammad, A. M., Abdul, G., and Salman, A. M., "Water purification by electrical discharges,"Plasma Sources Sci. Technol., 10, 82-91(2001). https://doi.org/10.1088/0963-0252/10/1/311
  2. Locke, B. R., Sato, M., Sunka, P., Hoffmann, M. R. and Chang, J. S., "Electrohydraulic discharge and nonthermal plasma for water treatment,"Ind. Eng. Chem. Res., 45, 882-905(2006). https://doi.org/10.1021/ie050981u
  3. Sunka, P., Babicky, V., Clupek, M., Lukes, P., Simek, M., Schmidt, J. and Cernak, M., "Generation of chemically active species by electrical discahrges in water,"Plasma Sources Sci. Technol., 8, 258-265(1999). https://doi.org/10.1088/0963-0252/8/2/006
  4. Bian, W., Ying, X. and Shi, J., "Enhanced degradation of pchlorophenol in a novel pulsed high voltage discharge reactor," J. Hazard. Mater., 162, 906-912(2009). https://doi.org/10.1016/j.jhazmat.2008.05.156
  5. Ohshima, T., Sato, K, Terauchi, H, and Sato, Masayuki, "Physical and chemical modifications of high-voltage pulse sterilization,"J. Electrostatics, 42, 159-166(1997). https://doi.org/10.1016/S0304-3886(97)00152-6
  6. Lukes, P., "Water treatment by pulsed streamer corona discharge,"Ph. D. Thesis, Institute of Plasma Physics, Academy of Science of the Czech Republic(2001).
  7. Kusic, H., Koprivanac, N. and Locke, B. R., "Decomposition of phenol by hybrid gas/liquid electrical discharge reactors with zeolite catalysts,"J. Hazard. Mater., B125, 190-200(2005).
  8. Clements, J. S., Sato, M., and Davis, R. H., "Preliminary investigation of prebreakdown phenomena and chemical reactions using a pulsed high voltage discharge in water," IEEE Trans. Ind. Appl., IA-23, 224(1987). https://doi.org/10.1109/TIA.1987.4504897
  9. Hoeben, W. F. L. M., Veldhuizen, E. M., Rutgers, W. R., Cramers, C. A. M. G., and Kroesen, G. M. W.," The degradation of aqueous phenol solutions by pulsed positive corona discharges,"Plasma Sources Sci. Technol., 9, 361-369(2000). https://doi.org/10.1088/0963-0252/9/3/315
  10. Sahni, M., and Locke, B. R.", Quantification of reductive species produced by high voltage electrical discharges in water,"Plasma Processes and Polymers, 3, 342-354(2006). https://doi.org/10.1002/ppap.200600006
  11. Sahni, M. and Locke, B. R., "The effects of reaction conditions on liquid-phase hydroxyl radical production in gas-liquid pulsedelectrical- discharge reactors,"Plasma Processes and Polymers, 3, 668-681(2006). https://doi.org/10.1002/ppap.200600020
  12. 이현돈, 정재우, 조무현", 펄스코로나방전에의한액체상페놀전환특성,"대한환경공학회지, 29(1), 40-46(2007).
  13. Joshi, A. A., Locke, B. R., Arce, P., and Finney, W. C., "Formation of hydroxyl radicals, hydrogen peroxide and aqueous electrons by pulsed streamer corona discharge in aqueous solution,"J. Hazard. Mater., 41, 3-30(1995). https://doi.org/10.1016/0304-3894(94)00099-3
  14. Lukes, P., Appleton, T., and Locke, B. R., "Hydrogen peroxide and ozone formation in hybrid gas-liquid electrical discharge reactors,"IEEE Transactions in Industry Applications, 40(1), 60-67(2004). https://doi.org/10.1109/TIA.2003.821799
  15. 정재우, Locke, B. R., "기체-액체 혼합 방전에 의한 화학적 활성종생성특성,"대한환경공학회지, 29(5), 556-563(2007).
  16. Grymonpre, D. R., Sharma, A. K., Finney W. C., and Locke, B. R., "The role of Fenton's reactions in aqueous phase pulsed streamer corona reactors,"Chem. Eng. J., 82, 189-207(2001). https://doi.org/10.1016/S1385-8947(00)00345-4
  17. Eisenberg, G. M., "Colorimetric determination of hydrogen peroxide,"Ind. Eng. Chem. Anal. Ed., 15(5), 327-328(1943). https://doi.org/10.1021/i560117a011
  18. Sun. B., Sato, M. and Clements, J. S., "Optical study of active species produced by a pulsed streamer corona discharge in water,"J. Electrostatics, 39, 189-202(1997). https://doi.org/10.1016/S0304-3886(97)00002-8
  19. Kirkpatrick, M. J., and Locke, B. R., "Effects of platinum electrode on hydrogen, oxygen, and hydrogen peroxide formation in aqueous phase pulsed corona electrical discharge," Ind. Eng. Chem. Res., 45, 2138-2142(2006). https://doi.org/10.1021/ie0511480
  20. Mededovic, S., and Locke, B. R., "Platinum catalyzed decomposition of hydrogen peroxide in aqueous-phase pulsed corona electrical discharge,"Appl. Catal. B : Environ., 67, 149- 159(2006). https://doi.org/10.1016/j.apcatb.2006.05.001
  21. 문지훈, 이현돈, 이명은, 박현건, 전기일, 정재우", 수중펄스코로나 방전에 의한 과산화수소 생성 특성,"대한환경공학회 2008 춘계학술대회발표회논문집, 608-610(2008).
  22. Mededovic, S., and Locke, B. R., "The role of platinum as the high voltage electrode in the enhancement of Fenton's reaction in liquid phase electrical discharge,"App. Catal. B : Environ., 72, 342-350(2007). https://doi.org/10.1016/j.apcatb.2006.11.014