SO_2-NO_2-NH_3-H_2O四元反应体系中气溶胶的生成特性
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摘要
通过烟雾箱实验,研究了SO_2-NO_2-NH_3-H_2O四元反应体系在气-粒转化过程中新形成颗粒物数浓度与粒径分布的变化.研究发现,SO_2-NO_2-NH_3-H_2O四元反应体系具有显著的成核能力,且其成核强度大,持续时间短.当SO_2、NO_2浓度为200mg/m~3,NH_3浓度为12×10~(-6)时,反应体系的气溶胶总个数浓度在2min时达到峰值2.5×10~6cm~(-3).缺少任一种气体均会使气溶胶成核强度下降.SO_2、NO_2及NH_3浓度分别为0的工况下气溶胶总个数浓度峰值分别下降了41.0%、83.6%及98.5%.在电厂污染气体排放浓度区间内,NO_2对气溶胶生成影响大于SO_2.燃煤电厂控制NO_x排放浓度对改善烟囱出口气溶胶数浓度更有效.在实验基础上,对颗粒物成核特性进行拟合,反应体系在气-粒转化过程中产生的新颗粒物总个数浓度及中值粒径与气态前体物浓度线性相关;采用布朗团聚模型对气溶胶成核后的团聚过程总个数浓度及粒径变化进行模拟计算,根据给定的燃煤电厂SO_2、NO_2、NH_3排放浓度,给出预测气溶胶颗粒成核速率、粒径分布及总个数浓度变化的方法.
The variations in concentration and diameter distribution of newly formed particulate matter,during the gas-to-solid conversion of the SO_2-NO_2-NH_3-H_2O quaternary system,were experimentally investigated with the smog chamber in this article.This quaternary system had a significant capability of nucleation,and a large nucleation intensity in such a short duration.When both of SO_2 and NO_2 concentrations were 200mg/m~3 and NH_3 concentration was 12×10~(-6),the total concentration of aerosols in this system reached a peak of 2.5×10~6cm~(-3) over two minute.Moreover,the nucleation strength of the aerosol would be reduced lacking in any one among three gases.Like this typical condition that SO_2,NO_2 or NH_3 concentration was zero,the maximum concentration of aerosols decreased by 41.0%,83.6%and 98.5%,respectively.Within the concentration ranges of SO_2,NO_2 or NH_3 emitted from coal-fired power plants,the NO_2 had a greater influence than SO_2 on the formation and agglomeration of newly formed particles.Based on experimental results,the fitting curves for nucleation characteristics of particulate matters were made.A linear correlation was observed between the total number concentration of newly formed particles and median particle diameter,and gaseous pollutant concentrations.The Brown agglomeration model was adopted to simulate the changes in total number concentration and particle size distribution of aerosols after nucleation in the agglomeration process.Finally,a method was proposed for predicting the change in the particle size distribution and total number concentration of aerosol particles,based on the typical emission concentrations of SO_2,NO_2 and NH_3 from coal-fired power plants.
The variations in concentration and diameter distribution of newly formed particulate matter,during the gas-to-solid conversion of the SO_2-NO_2-NH_3-H_2O quaternary system,were experimentally investigated with the smog chamber in this article.This quaternary system had a significant capability of nucleation,and a large nucleation intensity in such a short duration.When both of SO_2 and NO_2 concentrations were 200mg/m~3 and NH_3 concentration was 12×10~(-6),the total concentration of aerosols in this system reached a peak of 2.5×10~6cm~(-3) over two minute.Moreover,the nucleation strength of the aerosol would be reduced lacking in any one among three gases.Like this typical condition that SO_2,NO_2 or NH_3 concentration was zero,the maximum concentration of aerosols decreased by 41.0%,83.6%and 98.5%,respectively.Within the concentration ranges of SO_2,NO_2 or NH_3 emitted from coal-fired power plants,the NO_2 had a greater influence than SO_2 on the formation and agglomeration of newly formed particles.Based on experimental results,the fitting curves for nucleation characteristics of particulate matters were made.A linear correlation was observed between the total number concentration of newly formed particles and median particle diameter,and gaseous pollutant concentrations.The Brown agglomeration model was adopted to simulate the changes in total number concentration and particle size distribution of aerosols after nucleation in the agglomeration process.Finally,a method was proposed for predicting the change in the particle size distribution and total number concentration of aerosol particles,based on the typical emission concentrations of SO_2,NO_2 and NH_3 from coal-fired power plants.
引文
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[12]武卫玲,陈良富,陶金花,等.利用遥感数据评价燃煤电厂空气质量[J].遥感学报,2013,17(5):1235-1245.Wu W L,Chen L F,Tao J H,et al.Assessment of air in coal-fired power plants using satellite observations[J].Journal of Remote Sensing,2013,17(5):1235-1245.
[13]沙桐,马晓燕,王健颖,等.长江三角洲冬季电厂排放对大气污染的影响[J].中国环境科学,2018,38(9):90-99.Sha T,Ma X Y,Wang J Y,et al.The impact of power plant emission on air pollution during winter over Yangtze River Delta[J].China Environmental Science,2018,38(9):90-99.
[14]韩力慧,向欣,张海亮,等.北京市开发区PM1污染特征及影响霾形成的因素[J].中国环境科学,2018,38(8):48-58.Han L H,Xiang X,Zhang H L,et al.Pollution characteristics of PM1and factors affecting the formation of haze pollution at a developed zone in Beijing[J].China Environmental Science,2018,38(8):48-58.
[15]GB 13223-2011火电厂大气污染物排放标准[S].GB 13223-2011 Emission standard of air pollutants for thermal power plants[S].
[16]马双忱,金鑫,孙云雪,等.SCR烟气脱硝过程硫酸氢铵的生成机理与控制[J].热力发电,2010,39(8):12-17.Ma S C,Jin X,Sun Y X,et al.The formation mechanism of ammonium bisulfate in SCR flue gas denitrification process and control thereof[J].Thermal power generation,2010,39(8):12-17.
[17]Wang G,Zhang R,Gomez M E,et al.Persistent sulfate formation from London Fog to Chinese haze[J].Proceedings of the National Academy of Sciences of the United States of America,2016,48(113):13630-13635.
[18]Yang W W,He H,Ma Q X,et al.Synergistic formation of sulfate and ammonium resulting from reaction between SO2 and NH3 on typical mineral dust[J].Phys.Chem.Chem.Phys.,2016,18:956-964.
[19]Benner W H,Ogorevc B,Novakov T.Oxidation of SO2 in thin water films containing NH3[J].Atmospheric Environment.Part A.general Topics,1992,26(9):1713-1723.
[20]Kulmala M,Maso M D,M?kel?J M,et al.On the formation,growth and composition of nucleation mode particles[J].Tellus Series B-chemical&Physical Meteorology,2001,53(4):479-490.
[21]GieréR,Querol X.Solid particulate matter in the atmosphere[J].Elements,2010,6(4):215-222.
[22]Vu T V,Delgado-Saborit J M,Harrison R M.Review:Particle number size distributions from seven major sources and implications for source apportionment studies[J].Atmospheric Environment,2015,122:114-132.
[23]Landgrebe J D,Pratsinis S E.Gas-phase manufacture of particulates:interplay of chemical reaction and aerosol coagulation in the freemolecular regime[J].Industrial&Engineering Chemistry Research,1989,28(10):1474-1481.
[24]Friedlander S K,Marlow W H.Smoke,Dust and Haze:Fundamentals of Aerosol Behavior[J].Physics Today,1977,30(9):58-59.
[25]Sarabia R F D,Elvira-Segura L,I González-Gómez,et al.Investigation of the influence of humidity on the ultrasonic agglomeration of submicron particles in diesel exhausts[J].Ultrasonics,2004,41(4):277-281.
[26]Park S H,Lee K W,Otto E,et al.The log-normal size distribution theory of Brownian agglomeration for the entire particle size range[J].Journal of Aerosol Science,1999,30(28):S23-S24.
[2]Wang Q,Zhuang G,Huang K,et al.Probing the severe haze pollution in three typical regions of China:Characteristics,sources and regional impacts[J].Atmospheric Environment,2015,120:76-88.
[3]谢丹丹,祁建华,张瑞峰.青岛不同强度霾天气溶胶中二次无机离子的生成及粒径分布[J].环境科学,2017,38(7):2667-2678.Xie D D,Qi J H,Zhang R F.Formation and size distribution of the secondary aerosol inorganic ions in different intensity of haze in qingdao[J].Environmental Science,2017,38(7):2667-2678.
[4]陈静,杨鹏,韩军彩,等.基于高分辨率MARGA数据分析石家庄PM2.5成分谱特征[J].中国环境科学,2015,35(9):2594-2604.Chen J,Yang P,Han J C,et al.Analysis of PM2.5 spectrum characteristics in Shijiazhuang based on high resolution MARGA data[J].China Environmental Science,2015,35(9):2594-2604.
[5]郭振东,朱彬,王红磊,等.长江三角洲霾天气PM2.5中水溶性离子特征及来源解析[J].中国环境科学,2019,39(3):928-938.Guo Z D,Zhu B,Wang H L,et al.Characteristics and source analysis of water-soluble ions in PM2.5in the haze weather over in Yangtze River Delta[J].China Environmental Science,2019,39(3):928-938.
[6]王曼婷,朱彬,王红磊,等.长三角冬季一次霾过程气溶胶及其水溶性离子的区域分布特征[J].环境科学,2015,36(7):2337-2345.Wang M T,Zhu B,Wang H L,et al.Composition and regional characteristics of atmosphere aerosol and its water soluble ions over the Yangtze River Delta Region in a winter haze period[J].Environmental Science,2015,36(7):2337-2345.
[7]谭成好,赵天良,崔春光,等.近50年华中地区霾污染的特征[J].中国环境科学,2015,35(8):2272-2280.Tan C H,Zhao T L,Cui C G,et al.Characterization of haze pollution over Central China during the past 50years[J].China Environmental Science,2015,35(8):2272-2280.
[8]郭送军,谭吉华,段菁春,等.广州市灰霾期大气PM10中水溶性离子特征[J].环境科学与技术,2012,35(11):83-86.Guo S J,Tan J H,Duan J C,et al.Characteristics of water soluble ions in atmospheric PM10 during haze periods in Guangzhou[J].Environmental Science&Technology,2012,35(11):83-86.
[9]王开燕,王蓓蕾,王春林,等.广州2017年1月一次严重灰霾过程的影响因素分析[J].环境科技,2018,31(2):79-84.Wang K Y,Wang B L,Wang C L,et al.Analysis of influencing factors during a serious haze process in Guangzhou in January 2017[J].Environmental Science and Technology,2018,31(2):79-84.
[10]麦健华,邓涛,黄烨琪,等.中山市一次灰霾天气过程污染物来源数值模拟分析[J].中国环境科学,2017,37(9):3258-3267.Mai J H,Deng T,Huang Y Q,et al.Source analysis of a haze event in Zhongshan by numerical simulation[J].China Environmental Science,2017,37(9):3258-3267.
[11]Xue J,Yuan Z,Griffith S M,et al.Sulfate Formation Enhanced by a Cocktail of High NOx,SO2,Particulate Matter,and Droplet pH during Haze-Fog Events in Megacities in China:An Observation-Based Modeling Investigation[J].Environmental Science&Technology,2016,50(14):7325-7334.
[12]武卫玲,陈良富,陶金花,等.利用遥感数据评价燃煤电厂空气质量[J].遥感学报,2013,17(5):1235-1245.Wu W L,Chen L F,Tao J H,et al.Assessment of air in coal-fired power plants using satellite observations[J].Journal of Remote Sensing,2013,17(5):1235-1245.
[13]沙桐,马晓燕,王健颖,等.长江三角洲冬季电厂排放对大气污染的影响[J].中国环境科学,2018,38(9):90-99.Sha T,Ma X Y,Wang J Y,et al.The impact of power plant emission on air pollution during winter over Yangtze River Delta[J].China Environmental Science,2018,38(9):90-99.
[14]韩力慧,向欣,张海亮,等.北京市开发区PM1污染特征及影响霾形成的因素[J].中国环境科学,2018,38(8):48-58.Han L H,Xiang X,Zhang H L,et al.Pollution characteristics of PM1and factors affecting the formation of haze pollution at a developed zone in Beijing[J].China Environmental Science,2018,38(8):48-58.
[15]GB 13223-2011火电厂大气污染物排放标准[S].GB 13223-2011 Emission standard of air pollutants for thermal power plants[S].
[16]马双忱,金鑫,孙云雪,等.SCR烟气脱硝过程硫酸氢铵的生成机理与控制[J].热力发电,2010,39(8):12-17.Ma S C,Jin X,Sun Y X,et al.The formation mechanism of ammonium bisulfate in SCR flue gas denitrification process and control thereof[J].Thermal power generation,2010,39(8):12-17.
[17]Wang G,Zhang R,Gomez M E,et al.Persistent sulfate formation from London Fog to Chinese haze[J].Proceedings of the National Academy of Sciences of the United States of America,2016,48(113):13630-13635.
[18]Yang W W,He H,Ma Q X,et al.Synergistic formation of sulfate and ammonium resulting from reaction between SO2 and NH3 on typical mineral dust[J].Phys.Chem.Chem.Phys.,2016,18:956-964.
[19]Benner W H,Ogorevc B,Novakov T.Oxidation of SO2 in thin water films containing NH3[J].Atmospheric Environment.Part A.general Topics,1992,26(9):1713-1723.
[20]Kulmala M,Maso M D,M?kel?J M,et al.On the formation,growth and composition of nucleation mode particles[J].Tellus Series B-chemical&Physical Meteorology,2001,53(4):479-490.
[21]GieréR,Querol X.Solid particulate matter in the atmosphere[J].Elements,2010,6(4):215-222.
[22]Vu T V,Delgado-Saborit J M,Harrison R M.Review:Particle number size distributions from seven major sources and implications for source apportionment studies[J].Atmospheric Environment,2015,122:114-132.
[23]Landgrebe J D,Pratsinis S E.Gas-phase manufacture of particulates:interplay of chemical reaction and aerosol coagulation in the freemolecular regime[J].Industrial&Engineering Chemistry Research,1989,28(10):1474-1481.
[24]Friedlander S K,Marlow W H.Smoke,Dust and Haze:Fundamentals of Aerosol Behavior[J].Physics Today,1977,30(9):58-59.
[25]Sarabia R F D,Elvira-Segura L,I González-Gómez,et al.Investigation of the influence of humidity on the ultrasonic agglomeration of submicron particles in diesel exhausts[J].Ultrasonics,2004,41(4):277-281.
[26]Park S H,Lee K W,Otto E,et al.The log-normal size distribution theory of Brownian agglomeration for the entire particle size range[J].Journal of Aerosol Science,1999,30(28):S23-S24.
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