天津市2017年重污染过程二次无机化学污染特征分析
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摘要
基于2017年天津市超级观测站数据,筛选出7次典型重污染过程,从污染物浓度、二次转化方面分析重污染过程二次无机化学污染特征.结果表明,重污染期间NO_3~-和SO_4~(2-)浓度较清洁天气增长幅度最高,显著高于PM_(2.5)的增长程度,说明二次无机转化是导致重污染期间PM_(2.5)污染加重的重要原因;下半年PM_(2.5)和SO_2污染程度较上半年减轻,与秋冬季采取燃煤治理等活动有关;重污染期间NO_2/SO_2比值为1.5～19.6,其中下半年NO_2/SO_2比值显著高于上半年,说明在各项污染源管控下移动源的影响比例相对增加;大部分重污染期间NO_3~-浓度大于SO_4~(2-)浓度,SOR值高于NOR值,说明重污染期间硫酸盐和硝酸盐转化均较重要;在SO_2浓度显著降低的情况下,重污染期间SO_4~(2-)浓度并未明显降低,说明除二次无机转化外,硫酸盐生成还受其他因素影响.
Based on monitoring data collected at the supersite of Tianjin in 2017,seven typical heavy pollution episodes were investigated. The concentrations of air pollutants and secondary inorganic transformation products were analyzed to study the secondary inorganic pollution characteristics during the heavy pollution episodes. Compared to clean weather,concentrations of NO_3~- and SO_4~(2-) during the heavy pollution episodes increased at rapid growth rates. These rates were obviously higher than the rate for PM_(2.5) increases,which indicates that the secondary inorganic reactions had an important influence on PM_(2.5) pollution during the episodes. The concentrations of PM_(2.5) and SO_2 during the episodes in the latter half of the year were lower than those in the first half of the year probably because a substantial amount of coal use had been controlled. During the heavy pollution episodes,the NO_2/SO_2 values were 1. 5 to 19. 6,with higher values in the latter half of the year than the first half of the year suggestive of a greater influence from mobile sources. During most episodes,NO_3~- concentrations were higher than SO_4~(2-) concentrations,and SOR values were higher than NOR values,which shows that the secondary transformation of nitrate and sulfate both played important roles during the heavy pollution episodes. When SO_2 concentrations decreased significantly,SO_4~(2-) concentrations did not decrease obviously,thus indicating that besides the secondary inorganic reactions,other factors also had a large impact on the generation of sulfate.
Based on monitoring data collected at the supersite of Tianjin in 2017,seven typical heavy pollution episodes were investigated. The concentrations of air pollutants and secondary inorganic transformation products were analyzed to study the secondary inorganic pollution characteristics during the heavy pollution episodes. Compared to clean weather,concentrations of NO_3~- and SO_4~(2-) during the heavy pollution episodes increased at rapid growth rates. These rates were obviously higher than the rate for PM_(2.5) increases,which indicates that the secondary inorganic reactions had an important influence on PM_(2.5) pollution during the episodes. The concentrations of PM_(2.5) and SO_2 during the episodes in the latter half of the year were lower than those in the first half of the year probably because a substantial amount of coal use had been controlled. During the heavy pollution episodes,the NO_2/SO_2 values were 1. 5 to 19. 6,with higher values in the latter half of the year than the first half of the year suggestive of a greater influence from mobile sources. During most episodes,NO_3~- concentrations were higher than SO_4~(2-) concentrations,and SOR values were higher than NOR values,which shows that the secondary transformation of nitrate and sulfate both played important roles during the heavy pollution episodes. When SO_2 concentrations decreased significantly,SO_4~(2-) concentrations did not decrease obviously,thus indicating that besides the secondary inorganic reactions,other factors also had a large impact on the generation of sulfate.
引文
[1]郝宏飞,杨婷,王自发,等. 2013—2015年北京污染频发期细颗粒物重污染成因与天气形势关系的研究[J].环境科学学报,2018,38(6):2201-2213.Hao H F,Yang T,Wang Z F,et al. Investigation of relationship between synoptic pattern and heavy air pollution during heating from 2013 to 2015 in megacity Beijing, China[J]. Acta Scientiae Circumstantiae,2018,38(6):2201-2213.
[2] Ji D S,Wang Y S,Wang L L,et al. Analysis of heavy pollution episodes in selected cities of northern China[J]. Atmospheric Environment,2012,50:338-348.
[3]姚青,刘子锐,韩素芹,等.天津冬季一次重污染过程颗粒物中水溶性离子粒径分布特征[J].环境科学,2017,38(12):4958-4967.Yao Q,Liu Z R,Han S Q,et al. Characteristics of the size distribution of water-soluble ions during a heavy pollution episode in the winter in Tianjin[J]. Environmental Science,2017,38(12):4958-4967.
[4] Tang G Q,Zhao P S,Wang Y H,et al. Mortality and air pollution in Beijing:the long-term relationship[J]. Atmospheric Environment,2017,150:238-243.
[5] Di Q,Wang Y,Zanobetti A,et al. Air pollution and mortality in the medicare population[J]. New England Journal of Medicine,2017,376(26):2513-2522.
[6]马笑.京津冀大气污染特征及PM2. 5健康效益预测评估[D].邯郸:河北工程大学,2018.Ma X. The characteristics of air pollution and health benefits assessment of PM2. 5based on the BenMAP in BTH[D].Handan:Hebei University of Engineering,2018.
[7] Lee Y J,Jo W K,Chun H H. Characteristics of atmospheric visibility and its relationship with air pollution in Korea[J].Journal of Environmental Quality,2014,43(5):1519-1526.
[8] Deng J J, Du K, Wang K, et al. Long-term atmospheric visibility trend in Southeast China,1973-2010[J]. Atmospheric Environment,2012,59:11-21.
[9] Wu D,Tie X X,Li C C,et al. An extremely low visibility event over the Guangzhou region:a case study[J]. Atmospheric Environment,2005,39(35):6568-6577.
[10] Ramanathan V,Crutzen P J,Lelieveld J,et al. Indian Ocean experiment:an integrated analysis of the climate forcing and effects of the great Indo-Asian haze[J]. Journal of Geophysical Research,2001,106(D22):28371-28398.
[11] Stanhill G,Cohen S. Global dimming:a review of the evidence for a widespread and significant reduction in global radiation with discussion of its probable causes and possible agricultural consequences[J]. Agricultural and Forest Meteorology,2001,107(4):255-278.
[12] Xie Z S,Fan C L,Lu R,et al. Characteristics of ambient bioaerosols during haze episodes in China:a review[J].Environmental Pollution,2018,243:1930-1942.
[13]褚建功.气象因子对京津冀区域大气污染的影响[D].石家庄:河北科技大学,2018.Chu J G. The influence of meteorological factors on air pollution in Beijing-Tianjin-Hebei regions[D]. Shijiazhuang:Hebei University of Science&Technology,2018.
[14]杨兴川,赵文吉,熊秋林,等. 2016年京津冀地区PM2. 5时空分布特征及其与气象因素的关系[J].生态环境学报,2017,26(10):1747-1754.Yang X C, Zhao W J, Xiong Q L, et al. Spatio-temporal distribution of PM2. 5in Beijing-Tianjin-Hebei(BTH)area in2016 and its relationship with meteorological factors[J]. Ecology and Environmental Sciences,2017,26(10):1747-1754.
[15] Miao Y C,Hu X M,Liu S H,et al. Seasonal variation of local atmospheric circulations and boundary layer structure in the Beijing-Tianjin-Hebei region and implications for air quality[J].Journal of Advances in Modeling Earth Systems,2015,7(4):1602-1626.
[16]张敏,蔡子颖,韩素芹,等.天津污染天气边界层温度层结变化特征及预报阈值确定[J].环境科学学报,2018,38(6):2270-2278.Zhang M,Cai Z Y,Han S Q,et al. The research on threshold and regularity of temperature stratification in heavy pollution weather in Tianjin[J]. Acta Scientiae Circumstantiae,2018,38(6):2270-2278.
[17]徐虹,肖致美,孔君,等.天津市冬季典型大气重污染过程特征[J].中国环境科学,2017,37(4):1239-1246.Xu H,Xiao Z M,Kong J,et al. Characteristic of atmospheric heavy pollution episodes in winter of Tianjin[J]. China Environmental Science,2017,37(4):1239-1246.
[18]程念亮,李云婷,张大伟,等. 2013年1月北京市一次空气重污染成因分析[J].环境科学,2015,36(4):1154-1163.Cheng N L,Li Y T,Zhang D W,et al. Formation mechanism of a serious pollution event in January 2013 in Beijing[J].Environmental Science,2015,36(4):1154-1163.
[19] Zhao P S,Zhang X L,Xu X F,et al. Long-term visibility trends and characteristics in the region of Beijing,Tianjin,and Hebei,China[J]. Atmospheric Research,2011,101(3):711-718.
[20] Chan C K,Yao X H. Air pollution in mega cities in China[J].Atmospheric Environment,2008,42(1):1-42.
[21] Song C B,Wu L,Xie Y C,et al. Air pollution in China:Status and spatiotemporal variations[J]. Environmental Pollution,2017,227:334-347.
[22] Wang Y J,Bao S W,Wang S X,et al. Local and regional contributions to fine particulate matter in Beijing during heavy haze episodes[J]. Science of the Total Environment,2017,580:283-296.
[23] Liu P F,Zhao C S,Gbel T,et al. Hygroscopic properties of aerosol particles at high relative humidity and their diurnal variations in the North China Plain[J]. Atmospheric Chemistry and Physics,2011,11(7):3479-3494.
[24]洪沁,常宏宏.典型时段西南地区PM2. 5及组分污染特征[J].环境工程,2018,36(4):108-112.Hong Q,Chang H H. Characteristics of PM2. 5and components pollution during typical period in southwestern region[J].Environmental Engineering,2018,36(4):108-112.
[25]石梦双,韩斌,杨文,等.北京市典型重污染过程中PM2. 5载带水溶性无机离子污染特征分析[J].中国环境监测,2018,34(3):21-29.Shi M S,Han B,Yang W,et al. Characteristics of water soluble inorganic ions carried in PM2. 5of typical heavy haze episodes in Beijing[J]. Environmental Monitoring in China,2018,34(3):21-29.
[26]程念亮,张大伟,陈添,等. 2015年北京市两次红色预警期间PM2. 5浓度特征[J].环境科学,2016,37(7):2409-2418.Cheng N L, Zhang D W, Chen T, et al. Concentration characteristics of PM2. 5in Beijing during two red alert periods[J]. Environmental Science,2016,37(7):2409-2418.
[27]刘景云,刘子锐,温天雪,等.石家庄秋季一次典型霾污染过程水溶性离子粒径分布特征[J].环境科学,2016,37(9):3258-3267.Liu J Y,Liu Z R,Wen T X,et al. Characteristics of the size distribution of water soluble inorganic ions during a typical haze pollution in the autumn in Shijiazhuang[J]. Environmental Science,2016,37(9):3258-3267.
[28]贾佳,韩力慧,程水源,等.京津冀区域PM2. 5及二次无机组分污染特征研究[J].中国环境科学,2018,38(3):801-811.Jia J,Han L H,Cheng S Y,et al. Pollution characteristic of PM2. 5and secondary inorganic ions in Beijing-Tianjin-Hebei region[J]. China Environmental Science,2018,38(3):801-811.
[29]中华人民共和国国家统计局.中国统计年鉴2017[M].北京:中国统计出版社,2017.National Bureau of Statistics of China. China statistical yearbook2017[M]. Beijing:China Statistics Press,2017.
[30] Zhao P S, Dong F, Yang Y D, et al. Characteristics of carbonaceous aerosol in the region of Beijing, Tianjin, and Hebei,China[J]. Atmospheric Environment,2013,71:389-398.
[31]环境保护部. HJ 633-2012,环境空气质量指数(AQI)技术规定(试行)[S].
[32] Gao J J, Wang K, Wang Y, et al. Temporal-spatial characteristics and source apportionment of PM2. 5as well as its associated chemical species in the Beijing-Tianjin-Hebei region of China[J]. Environmental Pollution,2018,233:714-724.
[33] Xu H,Bi X H,Zheng W W,et al. Particulate matter mass and chemical component concentrations over four Chinese cities along the western Pacific coast[J]. Environmental Science and Pollution Research,2015,22(3):1940-1953.
[34] Geng G N,Zhang Q,Tong D,et al. Chemical composition of ambient PM2. 5over China and relationship to precursor emissions during 2005-2012[J]. Atmospheric Chemistry and Physics,2017,17(14):9187-9203.
[35] Wang Y,Zhuang G S,Zhang X Y,et al. The ion chemistry,seasonal cycle,and sources of PM2. 5and TSP aerosol in Shanghai[J]. Atmospheric Environment,2006,40(16):2935-2952.
[36] Wang Y,Zhuang G S,Tang A H,et al. The ion chemistry and the source of PM2. 5aerosol in Beijing[J]. Atmospheric Environment,2005,39(21):3771-3784.
[37] Huang R J,Zhang Y L,Bozzetti C,et al. High secondary aerosol contribution to particulate pollution during haze events in China[J]. Nature,2014,514(7521):218-222.
[38] Zhang X Y,Wang Y Q,Niu T,et al. Atmospheric aerosol compositions in China:spatial/temporal variability, chemical signature,regional haze distribution and comparisons with global aerosols[J]. Atmospheric Chemistry and Physics,2012,12(2):779-799.
[2] Ji D S,Wang Y S,Wang L L,et al. Analysis of heavy pollution episodes in selected cities of northern China[J]. Atmospheric Environment,2012,50:338-348.
[3]姚青,刘子锐,韩素芹,等.天津冬季一次重污染过程颗粒物中水溶性离子粒径分布特征[J].环境科学,2017,38(12):4958-4967.Yao Q,Liu Z R,Han S Q,et al. Characteristics of the size distribution of water-soluble ions during a heavy pollution episode in the winter in Tianjin[J]. Environmental Science,2017,38(12):4958-4967.
[4] Tang G Q,Zhao P S,Wang Y H,et al. Mortality and air pollution in Beijing:the long-term relationship[J]. Atmospheric Environment,2017,150:238-243.
[5] Di Q,Wang Y,Zanobetti A,et al. Air pollution and mortality in the medicare population[J]. New England Journal of Medicine,2017,376(26):2513-2522.
[6]马笑.京津冀大气污染特征及PM2. 5健康效益预测评估[D].邯郸:河北工程大学,2018.Ma X. The characteristics of air pollution and health benefits assessment of PM2. 5based on the BenMAP in BTH[D].Handan:Hebei University of Engineering,2018.
[7] Lee Y J,Jo W K,Chun H H. Characteristics of atmospheric visibility and its relationship with air pollution in Korea[J].Journal of Environmental Quality,2014,43(5):1519-1526.
[8] Deng J J, Du K, Wang K, et al. Long-term atmospheric visibility trend in Southeast China,1973-2010[J]. Atmospheric Environment,2012,59:11-21.
[9] Wu D,Tie X X,Li C C,et al. An extremely low visibility event over the Guangzhou region:a case study[J]. Atmospheric Environment,2005,39(35):6568-6577.
[10] Ramanathan V,Crutzen P J,Lelieveld J,et al. Indian Ocean experiment:an integrated analysis of the climate forcing and effects of the great Indo-Asian haze[J]. Journal of Geophysical Research,2001,106(D22):28371-28398.
[11] Stanhill G,Cohen S. Global dimming:a review of the evidence for a widespread and significant reduction in global radiation with discussion of its probable causes and possible agricultural consequences[J]. Agricultural and Forest Meteorology,2001,107(4):255-278.
[12] Xie Z S,Fan C L,Lu R,et al. Characteristics of ambient bioaerosols during haze episodes in China:a review[J].Environmental Pollution,2018,243:1930-1942.
[13]褚建功.气象因子对京津冀区域大气污染的影响[D].石家庄:河北科技大学,2018.Chu J G. The influence of meteorological factors on air pollution in Beijing-Tianjin-Hebei regions[D]. Shijiazhuang:Hebei University of Science&Technology,2018.
[14]杨兴川,赵文吉,熊秋林,等. 2016年京津冀地区PM2. 5时空分布特征及其与气象因素的关系[J].生态环境学报,2017,26(10):1747-1754.Yang X C, Zhao W J, Xiong Q L, et al. Spatio-temporal distribution of PM2. 5in Beijing-Tianjin-Hebei(BTH)area in2016 and its relationship with meteorological factors[J]. Ecology and Environmental Sciences,2017,26(10):1747-1754.
[15] Miao Y C,Hu X M,Liu S H,et al. Seasonal variation of local atmospheric circulations and boundary layer structure in the Beijing-Tianjin-Hebei region and implications for air quality[J].Journal of Advances in Modeling Earth Systems,2015,7(4):1602-1626.
[16]张敏,蔡子颖,韩素芹,等.天津污染天气边界层温度层结变化特征及预报阈值确定[J].环境科学学报,2018,38(6):2270-2278.Zhang M,Cai Z Y,Han S Q,et al. The research on threshold and regularity of temperature stratification in heavy pollution weather in Tianjin[J]. Acta Scientiae Circumstantiae,2018,38(6):2270-2278.
[17]徐虹,肖致美,孔君,等.天津市冬季典型大气重污染过程特征[J].中国环境科学,2017,37(4):1239-1246.Xu H,Xiao Z M,Kong J,et al. Characteristic of atmospheric heavy pollution episodes in winter of Tianjin[J]. China Environmental Science,2017,37(4):1239-1246.
[18]程念亮,李云婷,张大伟,等. 2013年1月北京市一次空气重污染成因分析[J].环境科学,2015,36(4):1154-1163.Cheng N L,Li Y T,Zhang D W,et al. Formation mechanism of a serious pollution event in January 2013 in Beijing[J].Environmental Science,2015,36(4):1154-1163.
[19] Zhao P S,Zhang X L,Xu X F,et al. Long-term visibility trends and characteristics in the region of Beijing,Tianjin,and Hebei,China[J]. Atmospheric Research,2011,101(3):711-718.
[20] Chan C K,Yao X H. Air pollution in mega cities in China[J].Atmospheric Environment,2008,42(1):1-42.
[21] Song C B,Wu L,Xie Y C,et al. Air pollution in China:Status and spatiotemporal variations[J]. Environmental Pollution,2017,227:334-347.
[22] Wang Y J,Bao S W,Wang S X,et al. Local and regional contributions to fine particulate matter in Beijing during heavy haze episodes[J]. Science of the Total Environment,2017,580:283-296.
[23] Liu P F,Zhao C S,Gbel T,et al. Hygroscopic properties of aerosol particles at high relative humidity and their diurnal variations in the North China Plain[J]. Atmospheric Chemistry and Physics,2011,11(7):3479-3494.
[24]洪沁,常宏宏.典型时段西南地区PM2. 5及组分污染特征[J].环境工程,2018,36(4):108-112.Hong Q,Chang H H. Characteristics of PM2. 5and components pollution during typical period in southwestern region[J].Environmental Engineering,2018,36(4):108-112.
[25]石梦双,韩斌,杨文,等.北京市典型重污染过程中PM2. 5载带水溶性无机离子污染特征分析[J].中国环境监测,2018,34(3):21-29.Shi M S,Han B,Yang W,et al. Characteristics of water soluble inorganic ions carried in PM2. 5of typical heavy haze episodes in Beijing[J]. Environmental Monitoring in China,2018,34(3):21-29.
[26]程念亮,张大伟,陈添,等. 2015年北京市两次红色预警期间PM2. 5浓度特征[J].环境科学,2016,37(7):2409-2418.Cheng N L, Zhang D W, Chen T, et al. Concentration characteristics of PM2. 5in Beijing during two red alert periods[J]. Environmental Science,2016,37(7):2409-2418.
[27]刘景云,刘子锐,温天雪,等.石家庄秋季一次典型霾污染过程水溶性离子粒径分布特征[J].环境科学,2016,37(9):3258-3267.Liu J Y,Liu Z R,Wen T X,et al. Characteristics of the size distribution of water soluble inorganic ions during a typical haze pollution in the autumn in Shijiazhuang[J]. Environmental Science,2016,37(9):3258-3267.
[28]贾佳,韩力慧,程水源,等.京津冀区域PM2. 5及二次无机组分污染特征研究[J].中国环境科学,2018,38(3):801-811.Jia J,Han L H,Cheng S Y,et al. Pollution characteristic of PM2. 5and secondary inorganic ions in Beijing-Tianjin-Hebei region[J]. China Environmental Science,2018,38(3):801-811.
[29]中华人民共和国国家统计局.中国统计年鉴2017[M].北京:中国统计出版社,2017.National Bureau of Statistics of China. China statistical yearbook2017[M]. Beijing:China Statistics Press,2017.
[30] Zhao P S, Dong F, Yang Y D, et al. Characteristics of carbonaceous aerosol in the region of Beijing, Tianjin, and Hebei,China[J]. Atmospheric Environment,2013,71:389-398.
[31]环境保护部. HJ 633-2012,环境空气质量指数(AQI)技术规定(试行)[S].
[32] Gao J J, Wang K, Wang Y, et al. Temporal-spatial characteristics and source apportionment of PM2. 5as well as its associated chemical species in the Beijing-Tianjin-Hebei region of China[J]. Environmental Pollution,2018,233:714-724.
[33] Xu H,Bi X H,Zheng W W,et al. Particulate matter mass and chemical component concentrations over four Chinese cities along the western Pacific coast[J]. Environmental Science and Pollution Research,2015,22(3):1940-1953.
[34] Geng G N,Zhang Q,Tong D,et al. Chemical composition of ambient PM2. 5over China and relationship to precursor emissions during 2005-2012[J]. Atmospheric Chemistry and Physics,2017,17(14):9187-9203.
[35] Wang Y,Zhuang G S,Zhang X Y,et al. The ion chemistry,seasonal cycle,and sources of PM2. 5and TSP aerosol in Shanghai[J]. Atmospheric Environment,2006,40(16):2935-2952.
[36] Wang Y,Zhuang G S,Tang A H,et al. The ion chemistry and the source of PM2. 5aerosol in Beijing[J]. Atmospheric Environment,2005,39(21):3771-3784.
[37] Huang R J,Zhang Y L,Bozzetti C,et al. High secondary aerosol contribution to particulate pollution during haze events in China[J]. Nature,2014,514(7521):218-222.
[38] Zhang X Y,Wang Y Q,Niu T,et al. Atmospheric aerosol compositions in China:spatial/temporal variability, chemical signature,regional haze distribution and comparisons with global aerosols[J]. Atmospheric Chemistry and Physics,2012,12(2):779-799.
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