气体参数对沿面放电活性氧物质注入氧化亚硫酸铵的影响
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摘要
为提高铵法脱硫产物的氧化效率,采用气相沿面放电生成的活性氧物质替代强制氧化法中的空气用于氧化亚硫酸铵,考察了沿面放电等离子体装置中的空气流速、温度、湿度及曝气孔的孔径、氧化物质的传输距离等因素对亚硫酸铵氧化率的影响。结果表明:亚硫酸铵氧化率随空气流速增大而提高;空气湿度、温度的升高降低臭氧的生成,不利于亚硫酸铵的氧化;曝气孔的孔径增大、氧化物质输运距离增大,降低臭氧等活性氧物质的利用效率,进而降低亚硫酸铵的氧化率。同空气强制氧化相比,采用沿面放电生成的活性氧物质氧化亚硫酸铵,可提高亚硫酸铵氧化率达一倍以上。
To improve the oxidation efficiency of the sulfite product in wet ammonia flue gas desulfurization, we used reactive oxygen species(ROS) generated from gas-phase surface discharge instead of air to oxidize ammonium sulfite, and investigated how the variation of gas flow parameters, including air temperature, air humidity, pore diameter of bubbler, and the transport distance of oxidative species, influences the oxidation rate of ammonium sulfite. According to the experimental results, the oxidation efficiency of ammonia sulfite increases with air flow rate, but decreases with increasing air humidity and air temperature. It is mainly due to the reduction of ozone at higher air humidity and temperature. Increasing the diameter of bubbler' pores and the delivery distance of oxidative species reduces the utilization rate of oxidative species including ozone, which further reduces the oxidation efficiency of ammonium sulfite. Compared with air forced oxidation, the oxidation method using ROS produced by surface discharge can raise the oxidation efficiency of ammonium sulfite by over one time.
To improve the oxidation efficiency of the sulfite product in wet ammonia flue gas desulfurization, we used reactive oxygen species(ROS) generated from gas-phase surface discharge instead of air to oxidize ammonium sulfite, and investigated how the variation of gas flow parameters, including air temperature, air humidity, pore diameter of bubbler, and the transport distance of oxidative species, influences the oxidation rate of ammonium sulfite. According to the experimental results, the oxidation efficiency of ammonia sulfite increases with air flow rate, but decreases with increasing air humidity and air temperature. It is mainly due to the reduction of ozone at higher air humidity and temperature. Increasing the diameter of bubbler' pores and the delivery distance of oxidative species reduces the utilization rate of oxidative species including ozone, which further reduces the oxidation efficiency of ammonium sulfite. Compared with air forced oxidation, the oxidation method using ROS produced by surface discharge can raise the oxidation efficiency of ammonium sulfite by over one time.
引文
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[20]牛铮,邵涛,章程,等.空气中纳秒脉冲均匀DBD增加聚合物的表面亲水性[J].高电压技术,2011,37(6):1536-1541.NIU Zheng,SHAO Tao,ZHANG Cheng,et al.Hydrophilic improvement of polymers treated by homogeneous nanosecond pulse dielectric barrier discharge in atmospheric air[J].High Voltage Engineering,2011,37(6):1536-1541.
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[2]Jia Y,Zhong Q,Fan X,et al.Kinetics of oxidation of total sulfite in the ammonia-based wet flue gas desulfurization process[J].Chemical Engineering Journal,2010,164(1):132-138.
[3]赵博,李彦,佟会玲,等.亚硫酸盐强制氧化传递与化学反应动力学[J].化工学报,2005,56(11):2059-2064.ZHAO Bo,LI Yan,TONG Huiling,et al.Mass transfer and kinetics of sulfite forced oxidation reaction[J].Journal of Chemical Industry and Engineering,2005,56(11):2059-2064.
[4]Brogren C,Karlsson H T.A model for prediction of limestone dissolution in wet flue gas desulfurization applications[J].Industrial and Engineering Chemistry Research,1997,36(9):3889-3897.
[5]Kallinikos L E,Farsari E I,Spartinos D N,et al.Simulation of the operation of an industrial wet flue gas desulfurization system[J].Fuel Processing Technology,2010,91(12):1794-1802.
[6]Carletti C,Bjondahl F,De Blasio C,et al.Modeling limestone reactivity and sizing the dissolution tank in wet flue gas desulfurization scrubbers[J].Environmental Progress&Sustainable Energy,2013,32(3):663-672.
[7]杨剑,文娟,董凌燕,等.烟气脱硫过程锰催化氧化亚硫酸钙的研究[J].环境工程学报,2007,1(9):109-112.YANG Jian,WEN Juan,DONG Lingyan,et al.Study on catalytic oxidation of calcium sulfite in flue gas desulfurization process by using manganese sulfate[J].Chinese Journal of Environmental Engineering,2007,1(9):109-112.
[8]Wang L,Zhao Y.Kinetics of sulfite oxidation in wet desulfurization with catalyst of organic acid[J].Chemical Engineering Journal,2008,136(2/3):221-226.
[9]Karatza D,Prisciandaro M,Lancia A,et al.Reaction rate of sulfite oxidation catalyzed by cuprous ions[J].Chemical Engineering Journal,2008,145(2):285-289.
[10]Despina K,Marina P,Amedeo L,et al.Sulfite oxidation catalyzed by cobalt ions in flue gas desulfurization processes[J].Journal of the Air&Waste Management Association,2010,60(6):675-680.
[11]刘兆斌,童华,王京刚.锌、铁等离子对氧化锌烟气脱硫工艺中亚硫酸锌氧化的影响[J].环境工程学报,2014,8(1):290-293.LIU Zhaobin,TONG Hua,WANG Jinggang.Effects of Zn and Fe ion on zinc sulfite oxidation in flue gas desulfurization with zinc oxide[J].Journal of Environmental Engineering,2014,8(1):290-293.
[12]Hu X,Zhu T,Jiang X,et al.A pilot investigation on oxidation of ammonium sulfite by streamer corona plasma[J].Chemical Engineering Journal,2008,139(3):469-474.
[13]Li Y,Shang K,Lu N,et al.Oxidation of ammonium sulfite in aqueous solutions using ozone technology[J].Journal of Physics:Conference Series,2013,418(1):012130.
[14]李悦,商克峰,鲁娜,等.沿面放电氧化液相亚硫酸铵[J].环境工程学报,2013,7(9):3489-3493.LI Yue,SHANG Kefeng,LU Na,et al.Oxidation of ammonium sulfite in aqueous solutions using surface discharge[J].Chinese Journal of Environmental Engineering,2013,7(9):3489-3493.
[15]危海涛,吴春笃.臭氧对亚硫酸铵的氧化效果研究[J].安徽农业科学,2011,39(25):15588-15589,15611.WEI Haitao,WU Chundu.Oxidation effects of ozone on ammonium sulfite[J].Journal of Anhui Agricultural Sciences,2011,39(25):15588-15589,15611.
[16]欧阳吉庭,缪劲松.氧气沿面放电臭氧合成机理[J].北京理工大学学报,2005,25(增刊):263-266.OUYANG Jiting,MIAO Jinsong.Ozone synthesis in oxygen in surface discharge[J].Transaction of Beijing Institute of Technology,2005,25(Supplement):263-266.
[17]李娅西,邵先军,彭兆裕,等.介质阻挡放电对橙汁灭菌及其品质的影响[J].高电压技术,2012,38(1):211-216.LI Yaxi,SHAO Xianjun,PENG Zhaoyu,et al.Effect of dielectric barrier discharge on microorganism inactivation and quality of orange juice[J].High Voltage Engineering,2012,38(1):211-216.
[18]侯世英,曾鹏,孙韬,等.介质阻挡放电在水处理中的影响因素分析[J].高电压技术,2014,40(1):187-193.HOU Shiying,ZENG Peng,SUN Tao,et al.Analysis on influential factors of dielectric barrier discharge on water treatment[J].High Voltage Engineering,2014,40(1):187-193.
[19]郑其锋,聂勇,顾大勇,等.填充式介质阻挡放电等离子体脱除硫酰氟的研究[J].高电压技术,2012,38(5):1157-1162.ZHENG Qifeng,NIE Yong,GU Dayong,et al.Removal of SO2F2 by the packed bed dielectric barrier discharge plasma[J].High Voltage Engineering,2012,38(5):1157-1162.
[20]牛铮,邵涛,章程,等.空气中纳秒脉冲均匀DBD增加聚合物的表面亲水性[J].高电压技术,2011,37(6):1536-1541.NIU Zheng,SHAO Tao,ZHANG Cheng,et al.Hydrophilic improvement of polymers treated by homogeneous nanosecond pulse dielectric barrier discharge in atmospheric air[J].High Voltage Engineering,2011,37(6):1536-1541.
[21]王新新.介质阻挡放电及其应用[J].高电压技术,2009,35(1):1-11.WANG Xinxin.Dielectric barrier discharge and its applications[J].High Voltage Engineering,2009,35(1):1-11.
[22]邵涛,章程,于洋,等.空气中纳秒脉冲均匀介质阻挡放电研究[J].高电压技术,2012,38(5):1045-1050.SHAO Tao,ZHANG Cheng,YU Yang,et al.Study on homogeneous nanosecond-pulse dielectric barrier discharge in atmospheric air[J].High Voltage Engineering,2012,38(5):1045-1050.
[23]Birdsall C M,Jenkins A C,Spadinger E.Iodometric determination of ozone[J].Analytical Chemistry,1952,24(4):662-664.