制取高浓度臭氧水的实验研究
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摘要
高浓度臭氧水是强氧化剂、杀菌消毒剂、漂白除味剂，在水处理和空气净化等环境保护领域具有重要的意义。本文结合国家自然科学基金重点资助项目“高气压下强电场电离气体的方法及其应用的基础研究”(项目编号：60031001)和辽宁省国际合作项目“高效率高浓度GGD型臭氧产生设备开发”(项目编号：98220013)，针对当前国内外臭氧和臭氧水产生技术现状，采用介质阻挡强电离放电方法，将非平衡等离子体的反应条件从低气压扩展到高气压，在分子层次上将O_2电离、离解，制成高浓度臭氧，并采用高效的溶解方法，将产生的高浓度臭氧溶解在水中，制取高浓度臭氧水溶液。
本文结合介质阻挡强电离放电制取高浓度臭氧的理论和当前臭氧溶解的理论及方法，进行了制取高浓度臭氧气体的实验研究。讨论了施加电压、气体流量、放电间隙、冷却水温度、能流密度、电源脉冲导通时间、模块叠加等对臭氧气体浓度和产生效率的影响，制取的臭氧浓度高达140.6g／m~3。在获得高浓度臭氧气体的前提下，对臭氧溶解进行了实验研究，讨论了应用臭氧量、气液比、系统压力、水流量、溶解方式、溶解时间等对臭氧溶解效率和臭氧水浓度的影响，臭氧的传质效率达到99％，有效溶解效率达到72％，产生的臭氧水浓度最高可达9.35g／m~3，并且实现了臭氧水产生设备的小型化。
高浓度的臭氧水可以作为药剂直接加入输水管道中，在水的输送过程中实现水的净化和污水的深度处理，省去传统方法中的反应池、氧化塔、曝气池等庞大设备，大幅度降低了能耗和运行成本。
High concentration ozone water is a kind of strong oxidant, disinfectant, deodorant and bleaching agent. It is widely used in water treatment, air treatment and other aspects of environmental protection. In this paper, following the key NSFC Project "Studies on the Method and Application of Gas Molecules Ionized with Strong Electric Field at High Pressure" and the International Cooperation Project of Liao Ning Province "Exploration of GGD Type Ozone Generator with High Efficiency and Concentration ", oxygen is ionized and dissociated on molecular scale, and high concentration ozone is generated by dielectric barrier aiscnarge with strong ionization which expands the reactive condition of plasma chemistry from low pressure to high pressure. Then high concentration ozone water is generated with the dissolution of ozone gas with high efficient dissolving methods.
The theory of generating high concentration ozone by dielectric barrier discharge with strong ionization, the theory of generating high concentration ozone water and the methods of dissolving ozone gas into water are presented. Experimental studies on the generation of high concentration ozone gas are carried out. Factors that affect the concentration of ozone gas and efficiency such as applied voltage, gas flux, discharge gap, cooling water temperature, energy density, breadth of impulse and modules splicing are discussed. The concentration of ozone gas is up to 140.6g/m3. Based on the generation of high concentration ozone, the experimental studies on the dissolution of ozone gas with different methods are carried out and the factors that affect the dissolving efficiency and concentration of ozone water such as applied ozone dose, gas to liquid ratio, system pressure, water flux, dissolving methods and dissolving time are discussed. The mass transfer efficiency of ozone is up to 99%. The effective dissolvi
ng efficiency of ozone is up to 72% and the concentration of ozone water is 9.35g/m3 in the maximum.
High concentration ozone water can be added to the pipelines directly to treat
wastewater during the course of water transportation. Thus it can avoid the use of reaction pool, oxidation tower and bubble chamber and reduce the energy consumption and running cost greatly.
本文结合介质阻挡强电离放电制取高浓度臭氧的理论和当前臭氧溶解的理论及方法，进行了制取高浓度臭氧气体的实验研究。讨论了施加电压、气体流量、放电间隙、冷却水温度、能流密度、电源脉冲导通时间、模块叠加等对臭氧气体浓度和产生效率的影响，制取的臭氧浓度高达140.6g／m~3。在获得高浓度臭氧气体的前提下，对臭氧溶解进行了实验研究，讨论了应用臭氧量、气液比、系统压力、水流量、溶解方式、溶解时间等对臭氧溶解效率和臭氧水浓度的影响，臭氧的传质效率达到99％，有效溶解效率达到72％，产生的臭氧水浓度最高可达9.35g／m~3，并且实现了臭氧水产生设备的小型化。
高浓度的臭氧水可以作为药剂直接加入输水管道中，在水的输送过程中实现水的净化和污水的深度处理，省去传统方法中的反应池、氧化塔、曝气池等庞大设备，大幅度降低了能耗和运行成本。
High concentration ozone water is a kind of strong oxidant, disinfectant, deodorant and bleaching agent. It is widely used in water treatment, air treatment and other aspects of environmental protection. In this paper, following the key NSFC Project "Studies on the Method and Application of Gas Molecules Ionized with Strong Electric Field at High Pressure" and the International Cooperation Project of Liao Ning Province "Exploration of GGD Type Ozone Generator with High Efficiency and Concentration ", oxygen is ionized and dissociated on molecular scale, and high concentration ozone is generated by dielectric barrier aiscnarge with strong ionization which expands the reactive condition of plasma chemistry from low pressure to high pressure. Then high concentration ozone water is generated with the dissolution of ozone gas with high efficient dissolving methods.
The theory of generating high concentration ozone by dielectric barrier discharge with strong ionization, the theory of generating high concentration ozone water and the methods of dissolving ozone gas into water are presented. Experimental studies on the generation of high concentration ozone gas are carried out. Factors that affect the concentration of ozone gas and efficiency such as applied voltage, gas flux, discharge gap, cooling water temperature, energy density, breadth of impulse and modules splicing are discussed. The concentration of ozone gas is up to 140.6g/m3. Based on the generation of high concentration ozone, the experimental studies on the dissolution of ozone gas with different methods are carried out and the factors that affect the dissolving efficiency and concentration of ozone water such as applied ozone dose, gas to liquid ratio, system pressure, water flux, dissolving methods and dissolving time are discussed. The mass transfer efficiency of ozone is up to 99%. The effective dissolvi
ng efficiency of ozone is up to 72% and the concentration of ozone water is 9.35g/m3 in the maximum.
High concentration ozone water can be added to the pipelines directly to treat
wastewater during the course of water transportation. Thus it can avoid the use of reaction pool, oxidation tower and bubble chamber and reduce the energy consumption and running cost greatly.
引文
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[9] S.Rilling. The basic clinical applications of ozone therapy. Ozone: Sci & Eng., 1985, 7: 259-274
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Venturi and Radial Mixing Nozzle. Proceedings of the 14th Ozone World Congress, Dearborn, Michigan, USA, 1999:527-538
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[28] 张维佳，王宝贞，伍悦滨，等．臭氧及深度氧化法去除水中污染物．给水排水，2000，26(5)：11～14
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[31] Pontius, FW. An update of the federal drinking water regs. AWWA, 1995, 87(2): 48-58
[32] M.bataller, E. Veliz, R.Perez-Rey, et al. Ozone swimming pool water treatment under tropicalconditions. Ozone: Sci & Eng., 2000, 22(6): 677-682
[33] D.Pacik, R.G Rice. The hydrozone kompact process-A new method for treatment and disinfection of swimming pools and bathing water. Ozone: Sci & Eng., 1991, 13(1): 63-70
[34] T.J.Morrison, L.L.Edwards, A.T. Wallace. Ozonation of water for salmonid fish rearing facilities-Pilot plant results. Ozone: Sci & Eng., 1979, 1:183-199
[35] R.G.Rice, J.F.Wilkes. Fundamental aspects of ozone chemistry in recirculating cooling water systems-Data evaluation needs. Ozone: Sci & Eng., 1992, 14:329-365
[36] 刘全校，安郁琴．臭氧用于治理制浆造纸废水．纸和造纸，2000,7(4)：44-45
[37] Clark, T. Jr., et al. A New Application of UV—Ozone Treatment in the
Preparation Substrade supported Mesoporous Thin Films. Chem.Mater, 2000, 12: 3879～3884
[38] Kuznetsova, A.Popova, I.Zhukov, et al. Making superior corrosion-resistant aluminum oxide films using ozone-electrochemical and electron microscopy studies. Vacuum Science and Technology. A. Vacuum, surfaces, and films, 2001, 19(4): 1971～1976
[39] J.Washuttl, E.Viebahn, I.Steiner. The influence of ozone on rumor tissue in comparison with healthy tissue. Ozone: Sci & Eng., 1990, 12: 65-72
[40] V.Bocci, E.Alinucci, E.borrelli, et al. Ozone in medicine. Ozone: Sci & Eng., 2001, 23: 207-218
[41] A.Filipi. Ozone in oral surgery-current status and prospects. Ozone: Sci & Eng.,1997, 19(3): 387-393
[42] R.G.Rice, J.W. Farquhar, L.J.Bollyky. Review of the applications of ozone for increasing storage times of perishable foods. Ozone: Sci & Eng., 1982, 4: 147-163
[43] Palou, L., Smilanick, et al. Effect of Gaseous Ozone Exposure on the Development of Green and Blue Molds on Cold Stored Citrus Fruit. Plant Disease, 2001, 85(6): 632～638
[44] 徐学基，诸定昌．气体放电物理，第一版，1996，上海复旦大学出版社，40-98
[45] 葛自良．放电等离子体臭氧发生技术的研究，高电压技术，1997，23(4)：65-70
[46] B Eliasson et al. Ozone synthesis from oxygen in dielectric barrier discharge, Phys. D: Appl. Phys, 1987, 20: 1421-1437
[47] B Eliasson et al. Modeling and Applications of Silent Discharge Plasmas. IEEE Trans on Plasma Science, 1991, 19(2): 309-323
[48] J Kitayama, M Kuzumoto. Aanalysis of ozone generation from air in silent discharge. J Phys. D: Appl. Phys, 1999, (32): 3032-3040
[49] 水野彰．放电排处理技术．静电气学会志，1995，19(4)：289—295
[50] 涂俊杰，分子筛变压吸附制氧在铜冶炼领域中的应用，节能技术，1998，90(4)，2-5
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[2] J.Perlowski, L.Kos, S.Ledakowicz. Application of ozone in textile wastewater treatment. Ozone: Sci&Eng., 1996, 18(1): 73-85
[3] R.Andreozzi, V.Caprio, A.Insola, et al. Advanced oxidation processes for the treatment of mineral oil contaminated wastewater. Wat. Res., 2000, 34: 620-628
[4] A.E. Pryor, M.Fisher. Practical guidelines for safe operation of cooling tower water ozonation systems. Ozone: Sci & Eng., 1994, 16: 505-536
[5] S.Hu, Y.Yu. Preozonation of chlorophenolic wastewater for subsequent biological treatment. Ozone: Sci&Eng., 1994, 16: 13-28
[6] F.J. Rivas, F.J. Beltran, O.Gimeno. Joint treatment ofwastewater from table olive processing and urban wastewater. Integrated ozonation-aerobic oxidation, Chem.Engrg Technol. 2000, 23: 177-181
[7] R.T.Meijers, E.J. Oderwald-Muller, P.A.Nuhn, etal. Degradation of pesticides by ozonation and advanced oxidation. Ozone: Sci & Eng., 1995, 17: 673-686
[8] P.Roche, M.Prados, Removal of pesticides by use of ozone or hydrogen peroxide/ozone. Ozone: Sci & Eng., 1995, 17: 657-672
[9] S.Rilling. The basic clinical applications of ozone therapy. Ozone: Sci & Eng., 1985, 7: 259-274
[10] Y.Fauvel, G.pons, J.P.Legeron. Seawater ozonation and shellfish depuration. Ozone: Sci & Eng., 1979, 1: 147-165
[11] Rounsaville, J. and Rice, R.G.. Evolution of Ozone for the Bleaching of Paper Pulps. Ozone: Sci & Eng., 1997, 18(6): 549～566
[12] 白希尧，张芝涛，白敏冬，等．高气压强电离放电等离子体学科的形成及应用展望．自然杂志，2000，22(3)：156-160
[13] R. Michael Meyer, Angelo L. Mazzei. Side stream Injection with High Efficiency
Venturi and Radial Mixing Nozzle. Proceedings of the 14th Ozone World Congress, Dearborn, Michigan, USA, 1999:527-538
[14] James R. Jackson, Paul K. Overbeck, John M. Overby. Dissolved Oxygen Control by Pressurized Side Stream Ozone Contacting and Degassing. Proceedings of the 14th Ozone World Congress, Dearborm, Michigan, USA, 1999: 561-574
[15] B.Eliasson, U.Kogelschatz. Nonequilibrium volume plasma chemical processing. IEEE transactions on plasma science, 1991, 19(6): 1063-1077
[16] Lutz Blaich, Michael Friedrich, Abdol Hossein Shadiakhy. Development of Ozone Technology and Application. Proceedings of the 14th Ozone World Congress, Dearborn, Michigan, USA, 1999:203-216
[17] J.Kitayama, M.Kuzumoto. Theoretical and experimental study on ozone generation characteristics of an oxygen-fed ozone generator in silent discharge, Phys.D: Appl.Phys, 1997, 30:2453-2461
[18] Yoichiro, Tabata, Masaki Kuzumoto. Development of a very narrow discharge gap ozone generator with lkg/hour production capacity. Proceeding of 13th ozone world congress, 1997, 2:901-906
[19] K.Hirose, T.Suzuki, et.al. Development of ultra-high concentration ozone generator, Proceedings of the 14th Ozone World Congress, Dearborn, Michigan, USA, 1999: 177-183
[20] B.Pashaie. Experimental investigation of microdischarges in a dielectric-barrier discharge. IEEE Transactions on Plasma Science, 1999, 27(1): 22-23
[21] 白希尧，白敏菂，扈群，等．高浓度臭氧水溶液研究．中国环境科学，2000，20(4)：309-312
[22] Z.Do-Quang, M.Roustan, J-M.Laine, J-P.Duguet. Deep U tube reactor: Resuluts from full-scale plants. Proceedings of 14th World Congress IOA, Dearbom, Michigan, USA, 1999: 540-541
[23] H.Fumio. Development of High Concentration Ozone Water Machine, Ishikawajima-Harima Engineering Review, 1996, 36(3): 159-164
[24] V.Farines, S.Baig, J. Albet, J. Molinier. Ozone Mass Transfer and Decomposition in a Fixed bed Reactor, Proceeding of the Fundamental and Engineering Concepts for Ozone Reactor Design, Toulouse, France, 2000
[25] M．A谢甫钦柯，等．臭氧化法水处理工艺学，刘存礼，第一版，1987．，清华大学出版社，1：50
[26] 陈凡植，颜幼平，林美强．硫化氢硫醇废弃的臭氧氧化试验．环境污染与防治，2000，22(3)：8-9
[27] 杨卓如，陈朝方，程江，等．臭氧法处理工业循环水的实验研究．工业水处理，1997，17(3)：11-13
[28] 张维佳，王宝贞，伍悦滨，等．臭氧及深度氧化法去除水中污染物．给水排水，2000，26(5)：11～14
[29] G.Boari, I.M.Mancini. Combined treatments of urban and olive mill effluents in Apulia, Wat.Sci.Tech., 1990, 22: 235-340
[30] J.Perkowski, L.Kos, S. Ledakowicz. Advanced oxidation of textile wastewaters. Ozone: Sci & Eng., 2000, 22(5): 535-550
[31] Pontius, FW. An update of the federal drinking water regs. AWWA, 1995, 87(2): 48-58
[32] M.bataller, E. Veliz, R.Perez-Rey, et al. Ozone swimming pool water treatment under tropicalconditions. Ozone: Sci & Eng., 2000, 22(6): 677-682
[33] D.Pacik, R.G Rice. The hydrozone kompact process-A new method for treatment and disinfection of swimming pools and bathing water. Ozone: Sci & Eng., 1991, 13(1): 63-70
[34] T.J.Morrison, L.L.Edwards, A.T. Wallace. Ozonation of water for salmonid fish rearing facilities-Pilot plant results. Ozone: Sci & Eng., 1979, 1:183-199
[35] R.G.Rice, J.F.Wilkes. Fundamental aspects of ozone chemistry in recirculating cooling water systems-Data evaluation needs. Ozone: Sci & Eng., 1992, 14:329-365
[36] 刘全校，安郁琴．臭氧用于治理制浆造纸废水．纸和造纸，2000,7(4)：44-45
[37] Clark, T. Jr., et al. A New Application of UV—Ozone Treatment in the
Preparation Substrade supported Mesoporous Thin Films. Chem.Mater, 2000, 12: 3879～3884
[38] Kuznetsova, A.Popova, I.Zhukov, et al. Making superior corrosion-resistant aluminum oxide films using ozone-electrochemical and electron microscopy studies. Vacuum Science and Technology. A. Vacuum, surfaces, and films, 2001, 19(4): 1971～1976
[39] J.Washuttl, E.Viebahn, I.Steiner. The influence of ozone on rumor tissue in comparison with healthy tissue. Ozone: Sci & Eng., 1990, 12: 65-72
[40] V.Bocci, E.Alinucci, E.borrelli, et al. Ozone in medicine. Ozone: Sci & Eng., 2001, 23: 207-218
[41] A.Filipi. Ozone in oral surgery-current status and prospects. Ozone: Sci & Eng.,1997, 19(3): 387-393
[42] R.G.Rice, J.W. Farquhar, L.J.Bollyky. Review of the applications of ozone for increasing storage times of perishable foods. Ozone: Sci & Eng., 1982, 4: 147-163
[43] Palou, L., Smilanick, et al. Effect of Gaseous Ozone Exposure on the Development of Green and Blue Molds on Cold Stored Citrus Fruit. Plant Disease, 2001, 85(6): 632～638
[44] 徐学基，诸定昌．气体放电物理，第一版，1996，上海复旦大学出版社，40-98
[45] 葛自良．放电等离子体臭氧发生技术的研究，高电压技术，1997，23(4)：65-70
[46] B Eliasson et al. Ozone synthesis from oxygen in dielectric barrier discharge, Phys. D: Appl. Phys, 1987, 20: 1421-1437
[47] B Eliasson et al. Modeling and Applications of Silent Discharge Plasmas. IEEE Trans on Plasma Science, 1991, 19(2): 309-323
[48] J Kitayama, M Kuzumoto. Aanalysis of ozone generation from air in silent discharge. J Phys. D: Appl. Phys, 1999, (32): 3032-3040
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