微泡强化臭氧传质及其对产生羟基自由基的影响
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摘要
为提高臭氧在水中的传质效率,设计了微泡反应器强化臭氧传质,考察了在该反应器中不同压力、温度、臭氧进口浓度及流量对液相中臭氧浓度以及羟基自由基产生的影响。结果表明,液相中臭氧浓度受压力影响较小,反应器压力增加可使液相中羟基自由基产生量增大;进口臭氧浓度及流量的增加,可使液相中臭氧浓度以及羟基自由基产生量增大;液相温度升高导致液相中臭氧浓度降低,但可以提高液相中羟基自由基产生量。同时还将该微泡反应体系与传统鼓泡反应器进行对比研究,结果表明,微泡反应器能有效地提高传质效率,液相中臭氧浓度达到稳定状态时约为14 mg/L,比鼓泡反应器高约10%。微泡加压反应器中羟基自由基产生效果更好,臭氧通入5 min,微泡反应器中羟基自由基浓度高达121.45×10~(-6)mol/L,比鼓泡反应器提高了约11倍,且微泡反应器中废水脱色及矿化效率都高于传统鼓泡反应器。
In order to improve the mass transfer efficiency of ozone in water, a microbubble reactor was designed to enhance the mass transfer of ozone. The effects of different reactor pressure, temperature, ozone inlet concentration and flow rates on the ozone concentration in the liquid phase and the generation of hydroxyl radicals were investigated. The results indicated that ozone concentration in liquid phase was less affected by the pressure, but the concentration of hydroxyl radicals in liquid phase increased with the increase of reactor pressure. With the increase of inlet ozone concentration and the flow rate, the ozone concentration in the liquid phase increased and more hydroxyl radicals were generated. Increasing the liquid temperature resulted in a reduction of the ozone concentration in the liquid phase, but it increased the amount of hydroxyl radicals produced in the liquid phase. The microbubble reaction system was also compared with the traditional bubbling reactor. The results showed that the microbubble reactor could effectively improve the mass transfer efficiency. When the ozone concentration in the liquid phase reached a steady state, it was about 14 mg/L, which was about 10% higher than that of a bubbling system. The hydroxyl radicals in the bubble reactor were more effectively generated than that in the traditional bubbling reactor. After 5 minutes of ozonation, the hydroxyl radical concentration in the microbubble reactor was as high as 121.45×10~(-6) mol/L, which was about 11 times higher than that of the bubbling reactor, and both the decolorization and mineralization efficiency of wastewater in the microbubble reactor were higher than that of the traditional bubbling reactor.
In order to improve the mass transfer efficiency of ozone in water, a microbubble reactor was designed to enhance the mass transfer of ozone. The effects of different reactor pressure, temperature, ozone inlet concentration and flow rates on the ozone concentration in the liquid phase and the generation of hydroxyl radicals were investigated. The results indicated that ozone concentration in liquid phase was less affected by the pressure, but the concentration of hydroxyl radicals in liquid phase increased with the increase of reactor pressure. With the increase of inlet ozone concentration and the flow rate, the ozone concentration in the liquid phase increased and more hydroxyl radicals were generated. Increasing the liquid temperature resulted in a reduction of the ozone concentration in the liquid phase, but it increased the amount of hydroxyl radicals produced in the liquid phase. The microbubble reaction system was also compared with the traditional bubbling reactor. The results showed that the microbubble reactor could effectively improve the mass transfer efficiency. When the ozone concentration in the liquid phase reached a steady state, it was about 14 mg/L, which was about 10% higher than that of a bubbling system. The hydroxyl radicals in the bubble reactor were more effectively generated than that in the traditional bubbling reactor. After 5 minutes of ozonation, the hydroxyl radical concentration in the microbubble reactor was as high as 121.45×10~(-6) mol/L, which was about 11 times higher than that of the bubbling reactor, and both the decolorization and mineralization efficiency of wastewater in the microbubble reactor were higher than that of the traditional bubbling reactor.
引文
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[23]Moslemi M,Davies S H,Masten S J.Ozone mass transfer in a recirculating loop semibatch reactor operated at high pressure[J].Journal of Advanced Oxidation Technologies,2010,13(1):79-88.
[24]Rischbieter E,Hendrik Stein A,Schumpe A.Ozone solubilities in water and aqueous salt solutions[J].J Chem Eng Data,2000,45(2):338-340.
[25]Nothe T,Fahlenkamp H,Sonntag C V.Ozonation of wastewater:rate of ozone consumption and hydroxyl radical yield[J].Environmental Science&Technology,2009,43(15):5990-5995.
[26]Song S,Liu Z,He Z,et al.Degradation of the biocide 4-chloro-3,5-dimethylphenol in aqueous medium with ozone in combination with ultraviolet irradiation:operating conditions influence and mechanism[J].Chemosphere,2009,77(8):1043-1051.
[27]Bai C P,Xiong X F,Gong W Q,et al.Removal of rhodamine B by ozone-based advanced oxidation process[J].Desalination,2011,278(1):84-90.
[28]Barik A J,Gogate P R.Degradation of 4-chloro 2-aminophenol using a novel combined process based on hydrodynamic cavitation,UV photolysis and ozone[J].Ultrasonics Sonochemistry,2016,30:70-78.
[29]Chen H W,Kuo Y L,Chiou C S,et al.Mineralization of reactive black 5 in aqueous solution by ozone/H2O2 in the presence of a magnetic catalyst[J].Journal of Hazardous Materials,2010,174(1):795-800.
[2]Sarkar S,Ali S,Rehmann L,et al.Degradation of estrone in water and wastewater by various advanced oxidation processes[J].Journal of Hazardous Materials,2014,278:16-24.
[3]Aken P V,Lambert N,Degreve J,et al.Comparison of different oxidation methods for recalcitrance removal of landfill leachate[J].Ozone:Science and Engineering,2011,33:294-300.
[4]laconi C D,Sanctis M D,Rossetti S,et al.Bio-chemical treatment of medium-aged sanitary landfill leachate in a high synergy system[J].Process Biochemistry,2011,46:2322-2329.
[5]Zhang Jianlin,Yu Hongtao,Quan Xie,et al.Ceramic membrane separation coupled with catalytic ozonation for tertiary treatment of dyestuff wastewater in a pilot-scale study[J].Chemical Engineering Journal,2016,301:19-26.
[6]Lu X,Ma H,Zhang Q,et al.Degradation of methyl orange by UV,O3 and UV/O3 systems:analysis of the degradation effects and mineralization mechanism[J].Research on Chemical Intermediates,2013,39(9):4189-4203.
[7]Gao M,Zeng Z,Sun B,et al.Ozonation of azo dye acid red 14 in a microporous tube-in-tube microchannel reactor:decolorization and mechanism[J].Chemosphere,2012,89(2):190-197.
[8]Zhang H,Jiang M,Zhang D,et al.Decomposition of 4-nitrophenol by ozonation in a hollow fiber membrane reactor[J].Chemical Engineering Communications,2009,197(3):377-386.
[9]Gao M,Zeng Z,Sun B,et al.Ozonation of azo dye acid red 14 in a microporous tube-in-tube microchannel reactor:decolorization and mechanism[J].Chemosphere,2012,89(2):190-197.
[10]Zhu Y,Chen S,Quan X,et al.Hierarchical porous ceramic membrane with energetic ozonation capability for enhancing water treatment[J].Journal of Membrane Science,2013,431:197-204.
[11]Song S,Ying H,He Z,et al.Mechanism of decolorization and degradation of CI direct red 23 by ozonation combined with sonolysis[J].Chemosphere,2007,66(9):1782-1788.
[12]He Z,Lin L,Song S,et al.Mineralization of CI reactive blue 19 by ozonation combined with sonolysis:performance optimization and degradation mechanism[J].Separation and Purification Technology,2008,62(2):376-381.
[13]Hsing H J,Chiang P C,Chang E E,et al.The decolorization and mineralization of acid orange 6 azo dye in aqueous solution by advanced oxidation processes:a comparative study[J].Journal of Hazardous Materials,2007,141(1):8-16.
[14]?zcan A,?ahin Y,Koparal A S,et al.Carbon sponge as a new cathode material for the electro-Fenton process:comparison with carbon felt cathode and application to degradation of synthetic dye basic blue 3 in aqueous medium[J].Journal of Electroanalytical Chemistry,2008,616(s 1/2):71-78.
[15]Xu Y,He Y,Cao X,et al.Ti O2/Ti rotating disk photoelectrocatalytic(PEC)reactor:a combination of highly effective thin-film PEC and conventional PEC processes on a single electrode[J].Environmental Science&Technology,2008,42(7):2612-2617.
[16]Chu L B,Xing X H,Yu A F,et al.Enhanced ozonation of simulated dyestuff wastewater by microbubbles[J].Chemosphere,2007,68(10):1854-1860.
[17]王璐,冯玥,韦彦斐,等.臭氧气泡大小对分散染料废水氧化处理效果的影响[J].环境污染与防治,2013,35(2):11-16.Wang Lu,Feng Yue,Wei Yanfei,et al.Influence of ozone bubble size on the treatment of dispersed dyestuff wastewater[J].Environmental Pollution&Control,2013,35(2):11-16.
[18]Takahashi M,Ishikawa H,Asano T,et al.Effect of microbubbles on ozonized water for photoresist removal[J].Journal of Physical Chemistry C,2012,116(23):12578-12583.
[19]朱兆亮,曹相生,孟雪征,等.气液混合泵气浮系统处理低浓度二级出水的研究[J].中国给水排水,2008,24(1):26-29.Zhu Zhaoliang,Cao Xiangsheng,Meng Xuezheng,et al.Study on advanced treatment of low concentration secondary effluent by DAF process with gas-liquid mixed pump[J].China Water&Wastewater,2008,24(1):26-29.
[20]朱兆亮,孟雪征,曹相生,等.三种气液混合泵气浮系统处理低浓度二级出水的对比研究[J].环境污染与防治,2008,30(8):4-7.Zhu Zhaoliang,Meng Xuezheng,Cao Xiangsheng,et al.Advanced treatment of secondary effluent by dissolved air flotation employing air-liquid mixing pump in three DAF systems[J].Environmental Pollution&Control,2008,30(8):4-7.
[21]Bader H,Hoigne J.Determination of ozone in water by the indigo method[J].Water Research,1981,15(4):449-456.
[22]Milan-Segovia N,Wang Y,Cannon F S,et al.Comparison of hydroxyl radical generation for various advanced oxidation combinations as applied to foundries[J].Ozone:Science and Engineering,2007,29(6):461-471.
[23]Moslemi M,Davies S H,Masten S J.Ozone mass transfer in a recirculating loop semibatch reactor operated at high pressure[J].Journal of Advanced Oxidation Technologies,2010,13(1):79-88.
[24]Rischbieter E,Hendrik Stein A,Schumpe A.Ozone solubilities in water and aqueous salt solutions[J].J Chem Eng Data,2000,45(2):338-340.
[25]Nothe T,Fahlenkamp H,Sonntag C V.Ozonation of wastewater:rate of ozone consumption and hydroxyl radical yield[J].Environmental Science&Technology,2009,43(15):5990-5995.
[26]Song S,Liu Z,He Z,et al.Degradation of the biocide 4-chloro-3,5-dimethylphenol in aqueous medium with ozone in combination with ultraviolet irradiation:operating conditions influence and mechanism[J].Chemosphere,2009,77(8):1043-1051.
[27]Bai C P,Xiong X F,Gong W Q,et al.Removal of rhodamine B by ozone-based advanced oxidation process[J].Desalination,2011,278(1):84-90.
[28]Barik A J,Gogate P R.Degradation of 4-chloro 2-aminophenol using a novel combined process based on hydrodynamic cavitation,UV photolysis and ozone[J].Ultrasonics Sonochemistry,2016,30:70-78.
[29]Chen H W,Kuo Y L,Chiou C S,et al.Mineralization of reactive black 5 in aqueous solution by ozone/H2O2 in the presence of a magnetic catalyst[J].Journal of Hazardous Materials,2010,174(1):795-800.
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