上海市空气污染排放清单及大气中高浓度细颗粒物的形成机制
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摘要
上海是中国经济活动总量最大、工业门类最全、能源消耗强度最大、污染物排放密度最高的城市。近年来,随着产业结构和工业布局的调整、清洁能源替代及工业区环境综合整治等系列污染控制措施的实施,上海市环境空气质量总体上得到了改善。2008年上海市环境空气中PM_(10)的年日均浓度为0.084毫克/立方米,比2004年下降了15%;SO_2年日均浓度同比下降了5.6%;NO_2下降了9.7%。但是,与国际大都市相比,上海环境空气质量仍处于较高污染的水平。以PM_(10)为主的大气污染指标是发达国家城市的2—5倍,特别是细颗粒物PM_(2.5)的年平均浓度高达0.050—0.059mg/m~3,超过国际卫生组织年平均值标准0.015 mg/m~3的3—4倍。以PM_(2.5)为代表的细颗粒物已成为制约上海市环境空气质量改善的关键问题。
本博士论文,以上海市环境空气中PM_(10)和PM_(2.5)的污染因子为研究对象,以大气污染物排放清单的建立和分担率研究为核心,结合现场监测、实验室分析、统计分析和数值模型,开展了上海市细颗粒气溶胶污染的时空分布、化学组成、形成机制和来源研究。本研究通过对污染源的全面识别和梳理,结合全国污染源普查及重点国控企业大气污染物排放核查的创新工作方法,应用及修订多种污染物排放定量技术方法和手段,探索了石化行业VOCs无组织排放的定量难题,建立了以气溶胶污染为控制目标,以常规大气污染物(PM、PM_(10)、PM_(2.5)、SO_2、NOx、CO、VOCs和NH_3)为目标污染物的2006年上海市大气污染物排放清单及改进的2007年点源大气污染物排放清单。该清单空间精度为1×1km~2网格精度、高度1km,涉及33种工业行业点源(12896家工业企业)、20种民用与工业面源以及机动车、船舶、飞机和火车在内的流动污染源。
2006年排放清单研究显示,上海市各类污染源向环境空气中排放的总量分别为:PM—58.2万吨、PM_(10)—27.9万吨、PM_(2.5)—11.1万吨、SO_2—56.4万吨、NOx—46.4万吨、CO—141.7万吨、VOC—57.4万吨和NH_3—1.4万吨,是全世界污染物排放量最多的城市。面源是PM、PM_(10)、PM_(2.5)、VOC和NH_3的首要来源;点源是SO_2和NOx的第一来源;流动源是CO的第一来源,分担率为46%。其中,道路扬尘是上海市一次颗粒物(PM、PM_(10)和PM_(2.5))的首要来源,对全市总量的分担率为54%、45%和26%。造成上海环境空气中气溶胶二次组分的主要污染物SO_2的主要来源是电站锅炉和工业分散燃料,其分担率分别为57%和12%;主要污染物NOx的主要排放来源是电站锅炉和机动车,分别为全市总量的36%和18%;有机气溶胶的来源即污染物VOC的主要排放源是涂料、生产工艺储罐和机动车,其分担率分别为28%、23%和16%。NH_3的排放主要来自畜禽养殖和点源生产工艺,分别占全市总量的66.7%和19.7%。
本研究还应用MODELS3/CMAQ数值模型对上海冬季污染的来源开展了情景模拟分析,测试了电厂、非电工业源、流动源和面源等主要污染源类别对上海市细颗粒污染的贡献和影响。2008年冬季数值模型模拟结果显示,上海市气溶胶PM_(10)、PM_(2.5)的浓度受面源排放的影响较其它排放源更大,浓度贡献率为68.3%;其次是流动源和非电站点源排放。电站点源是造成SO_2连续多天较高浓度的最主要排放源,浓度贡献率为32.1%;其次是流动源和非电站点源,周边外来源的影响占15.3%。造成NO_2高浓度的最主要排放源则是流动源,其次是电站点源和非电站点源。
本研究利用2004-2008期间上海市环境空气中PM_(10)及PM_(2.5)自动监控网络和气溶胶滤膜现场监测,深入分析了所采集的35万余个监测数据。结果表明,上海细颗粒污染呈现冬春季节高(1、3、4、11和12月)、夏秋季节(7、8和9月)较低,日变化双峰(6:00—8:00、18:00—19:00)双谷,以及东部沿海区域低、西北部污染浓度高的时空间分布特点。PM_(2.5)/PM_(10)常年平均值在0.5以上,不同污染类别下,气态污染物与颗粒物的污染呈现出显著差异。重霾污染日,SO_2/PM_(10)(0.38)和NO_2/PM_(10)(0.24)明显低于优良日(0.51和0.62),而PM_(2.5)/PM_(10)比值显著升高达到61%。PM_(2.5)中水可溶性组分占到59%,硫的转化率(SOR)和氮的转化率(NOR)分别达到0.67和0.61,表明一次SO_2和NOx转化成的硫酸盐、硝酸盐以及铵盐是形成上海PM_(2.5)高浓度的主要因素。在受沙尘输送影响下的高污染日,上海市环境空气中SO_2/PM_(10)、NO_2/PM_(10)、PM_(2.5)/PM_(10)进一步降至0.066、0.073和15.5%。SO_2/PM_(10)、NO_2/PM_(10)和PM_(2.5)/PM_(10)比值可作为判断沙尘日、非沙尘日和霾污染日的重要指标。
本研究成果揭示了上海市细颗粒气溶胶的污染特性及变化规律,阐明了沙尘长距离输送影响条件下,上海市气溶胶尤其是典型重霾污染的特性、来源、形成机制及其对大气空气质量的影响。
本研究已经在国际SCI杂志和中国核心期刊、书籍上发表了9篇论文,其中第一作者4篇;还有1篇已投到国际SCI杂志,1篇拟投国际SCI杂志,均为第一作者。本研究主要成果已获得2008年度“上海市科学技术进步奖”二等奖。
Shanghai has been one of the largest cities with rapid economic development, which processes the most complete industry categories, the largest energy consumption intensity and the highest density of emission sources. During the past decades, with the application of air pollution control measures, such as the adjustment of industrial structure and layout, alternatives of cleaner energy and comprehensive pollution control on the industrial parks, the ambient air quality in Shanghai has been improved generally. The annual average of daily concentration for PM_(10) was 0.084mg/m~3 in 2008, which has decreased by 15% comparing to 2004. The annual average of daily concentration for SO_2 has decreased by 5.6%, The annual average of daily concentration for NO_2 has decreased by 9.7%. However, the air pollution is still serious in shanghai comparing with the other international megacity. The pollution level of PM_(10) is 2 to 5 times of that in developed cities. Furthermore, the annual daily concentration of fine particle matter (PM_(2.5)) is about 0.050 to 0.059 mg/m~3, which is 3 or 4 times greater than the annual average guideline value(0.015 mg/m~3) set by World health organization. The fine particle pollutiion represented by PM2.5 has become the key issue of air quality improvement in Shanghai.
In this study, the PM_(10) and PM_(2.5) in ambient air was observed in shanghai. With the development of air pollution emission invertory and its contribution as the basic research content, combining with the on-site monitoring, laboratory analysis, statistical analysis and numerical models, the spatial and temporal distribution of fine particle aerosol pollution, the chemical composition, formation mechanism and source identification were analyzed. In this study, according to the comprehensive identidication of pollution sources, the methods and measures of emission inventory quantification were applied and revised for the key pollution plant, combining with the national pollution census and the innovative methods for verifying the emission sources of key national controlled enterprises. The quantitative changellenge for fugitive emission of VOCs in petrochemical industry was studied and practiced. Additionally, the air pollution emission inventory in shanghai was developed, which contained the criteria pollutants of PM, PM_(10), PM_(2.5), SO_2, NO_X, CO, VOCs and NH_3 aiming for aerosol pollution control. The grid resolution of this emission inventory is for 1km×1km and the height is 1km, including 33 kinds of industrial point sources (12896 industrial enterprises), 20 kinds of domestic and industrial point sources, as well as the mobile sources such as motor vehicles, ships, aircraft and trains.
As shown by emission inventory of 2006, the total mass of all kinds of emission sources are 582,000 tons for PM, 279000 tons for PM_(10), 111000 tons for PM_(2.5), 564000 tons for SO_2, 464000 tons for NO_X, 1417000 tons for CO, 574000 tons for VOC, 14000 tons for NH_3, which is the highest in the world. Area emission is the major sources for PM, PM_(10), PM_(2.5), VOC and NH3. Point emission is the major source for SO_2 and NO_X. Mobil emission is the major source for CO, which contributed 46% of the total. The road dust is the major source for primary pollutants such as PM, PM_(10) and PM_(2.5), which contributed 54%, 45% and 26% respectively. The power plant and the fuel-firing of industry, contributing 57% and 12% of the total and was the key source of SO_2 which would transform into the secondary aerosol pollutant. The major source for NO_X is power plant and vehicles, which contributed 36% and 18% of the total mass in shanghai. The major sources for VOCs pollutant are coatings, tank and motor vehicles production process, which contributed 28%, 23% and 16% respectively. The major source of NH3 pollutant is from the breeding of livestock feeding, poultry and industrial process, which contributed 66.7% and 19.7% of the total emission mass in Shanghai.
In this study, MODEL3-CMAQ was used to analyze the source of the pollution in winter in shanghai, the scenario simulation was developed to analyze the contribution of different emission sources to the fine particle pollution in shanghai. The results showed that the concentration of PM_(10), PM_(2.5) in Shanghai was mainly influenced by area emission which contributed 68.3% of the concentration, and the mobile emission as well as the non-power plant next. The power plant emission was the major factor caused the continual high concentration of SO_2, which contributed the 32.1%, secondly is mobile and non power plant emission. The contribution of sources outside Shanghai was 15.3%. The mobile source is the major factor caused the high concentration of NO_2, next is power plant and non power generating industrial plant.
In this study, a great number of PM_(10) and PM_(2.5) data from ambient air monitoring network and aerosol sampling was analyzed. The results showed that the temporal variation exhibited high concentration in winter and spring (Jan. Mar. April, Nov. and Dec), low concentration in summer and autumn (Jul, Aug and Sep). The diurnal variation showed two peaks. And the spatial variation showed that low concentration of PM_(10) in eastern coastal areas and high concentration in northwestern areas. The average concentration of PM25/PM10 was more than 0.5 in Shanghai. The variation of gaseous pollutants was different from that of particle matter in different pollution episode. The SO_2/PM_(10) (0.38) value in serious haze days was significantly lower than that in good or moderate days, while PM_(2.5)/PM_(10) value significantly increased to 61%. The proportion of water-soluble components in PM_(2.5) accounted for 59%. SOR and NOR was to 0.67 and 0.61, respectively, which meant the sulfate, nitrate and ammonium transformed from primary SO_2 and NO_X. It was the key mechanism for the high concentration of PM_(2.5) in Shanghai. In the high pollution days influenced by long distance transport of dust storm, the ratios of SO_2/PM_(10),NO_2/PM_(10),PM_(2.5)/PM_(10) in ambient air of Shanghai have decreased to 0.066, 0.073 and 0.155. The values of SO_2/PM_(10),NO_2/PM_(10) and PM_(2.5)/PM_(10) could be used as the important index to identify the dust day, non-dust day or haze day in Shanghai.
The results of this study revealed the fine particle aerosol characteristics and changes in Shanghai. The characteristics, source and formation mechanism of aerosol, especially under the typical serious haze pollution and its impact on air quality, impact by the long distance transport of dust storm was clarified.
本博士论文,以上海市环境空气中PM_(10)和PM_(2.5)的污染因子为研究对象,以大气污染物排放清单的建立和分担率研究为核心,结合现场监测、实验室分析、统计分析和数值模型,开展了上海市细颗粒气溶胶污染的时空分布、化学组成、形成机制和来源研究。本研究通过对污染源的全面识别和梳理,结合全国污染源普查及重点国控企业大气污染物排放核查的创新工作方法,应用及修订多种污染物排放定量技术方法和手段,探索了石化行业VOCs无组织排放的定量难题,建立了以气溶胶污染为控制目标,以常规大气污染物(PM、PM_(10)、PM_(2.5)、SO_2、NOx、CO、VOCs和NH_3)为目标污染物的2006年上海市大气污染物排放清单及改进的2007年点源大气污染物排放清单。该清单空间精度为1×1km~2网格精度、高度1km,涉及33种工业行业点源(12896家工业企业)、20种民用与工业面源以及机动车、船舶、飞机和火车在内的流动污染源。
2006年排放清单研究显示,上海市各类污染源向环境空气中排放的总量分别为:PM—58.2万吨、PM_(10)—27.9万吨、PM_(2.5)—11.1万吨、SO_2—56.4万吨、NOx—46.4万吨、CO—141.7万吨、VOC—57.4万吨和NH_3—1.4万吨,是全世界污染物排放量最多的城市。面源是PM、PM_(10)、PM_(2.5)、VOC和NH_3的首要来源;点源是SO_2和NOx的第一来源;流动源是CO的第一来源,分担率为46%。其中,道路扬尘是上海市一次颗粒物(PM、PM_(10)和PM_(2.5))的首要来源,对全市总量的分担率为54%、45%和26%。造成上海环境空气中气溶胶二次组分的主要污染物SO_2的主要来源是电站锅炉和工业分散燃料,其分担率分别为57%和12%;主要污染物NOx的主要排放来源是电站锅炉和机动车,分别为全市总量的36%和18%;有机气溶胶的来源即污染物VOC的主要排放源是涂料、生产工艺储罐和机动车,其分担率分别为28%、23%和16%。NH_3的排放主要来自畜禽养殖和点源生产工艺,分别占全市总量的66.7%和19.7%。
本研究还应用MODELS3/CMAQ数值模型对上海冬季污染的来源开展了情景模拟分析,测试了电厂、非电工业源、流动源和面源等主要污染源类别对上海市细颗粒污染的贡献和影响。2008年冬季数值模型模拟结果显示,上海市气溶胶PM_(10)、PM_(2.5)的浓度受面源排放的影响较其它排放源更大,浓度贡献率为68.3%;其次是流动源和非电站点源排放。电站点源是造成SO_2连续多天较高浓度的最主要排放源,浓度贡献率为32.1%;其次是流动源和非电站点源,周边外来源的影响占15.3%。造成NO_2高浓度的最主要排放源则是流动源,其次是电站点源和非电站点源。
本研究利用2004-2008期间上海市环境空气中PM_(10)及PM_(2.5)自动监控网络和气溶胶滤膜现场监测,深入分析了所采集的35万余个监测数据。结果表明,上海细颗粒污染呈现冬春季节高(1、3、4、11和12月)、夏秋季节(7、8和9月)较低,日变化双峰(6:00—8:00、18:00—19:00)双谷,以及东部沿海区域低、西北部污染浓度高的时空间分布特点。PM_(2.5)/PM_(10)常年平均值在0.5以上,不同污染类别下,气态污染物与颗粒物的污染呈现出显著差异。重霾污染日,SO_2/PM_(10)(0.38)和NO_2/PM_(10)(0.24)明显低于优良日(0.51和0.62),而PM_(2.5)/PM_(10)比值显著升高达到61%。PM_(2.5)中水可溶性组分占到59%,硫的转化率(SOR)和氮的转化率(NOR)分别达到0.67和0.61,表明一次SO_2和NOx转化成的硫酸盐、硝酸盐以及铵盐是形成上海PM_(2.5)高浓度的主要因素。在受沙尘输送影响下的高污染日,上海市环境空气中SO_2/PM_(10)、NO_2/PM_(10)、PM_(2.5)/PM_(10)进一步降至0.066、0.073和15.5%。SO_2/PM_(10)、NO_2/PM_(10)和PM_(2.5)/PM_(10)比值可作为判断沙尘日、非沙尘日和霾污染日的重要指标。
本研究成果揭示了上海市细颗粒气溶胶的污染特性及变化规律,阐明了沙尘长距离输送影响条件下,上海市气溶胶尤其是典型重霾污染的特性、来源、形成机制及其对大气空气质量的影响。
本研究已经在国际SCI杂志和中国核心期刊、书籍上发表了9篇论文,其中第一作者4篇;还有1篇已投到国际SCI杂志,1篇拟投国际SCI杂志,均为第一作者。本研究主要成果已获得2008年度“上海市科学技术进步奖”二等奖。
Shanghai has been one of the largest cities with rapid economic development, which processes the most complete industry categories, the largest energy consumption intensity and the highest density of emission sources. During the past decades, with the application of air pollution control measures, such as the adjustment of industrial structure and layout, alternatives of cleaner energy and comprehensive pollution control on the industrial parks, the ambient air quality in Shanghai has been improved generally. The annual average of daily concentration for PM_(10) was 0.084mg/m~3 in 2008, which has decreased by 15% comparing to 2004. The annual average of daily concentration for SO_2 has decreased by 5.6%, The annual average of daily concentration for NO_2 has decreased by 9.7%. However, the air pollution is still serious in shanghai comparing with the other international megacity. The pollution level of PM_(10) is 2 to 5 times of that in developed cities. Furthermore, the annual daily concentration of fine particle matter (PM_(2.5)) is about 0.050 to 0.059 mg/m~3, which is 3 or 4 times greater than the annual average guideline value(0.015 mg/m~3) set by World health organization. The fine particle pollutiion represented by PM2.5 has become the key issue of air quality improvement in Shanghai.
In this study, the PM_(10) and PM_(2.5) in ambient air was observed in shanghai. With the development of air pollution emission invertory and its contribution as the basic research content, combining with the on-site monitoring, laboratory analysis, statistical analysis and numerical models, the spatial and temporal distribution of fine particle aerosol pollution, the chemical composition, formation mechanism and source identification were analyzed. In this study, according to the comprehensive identidication of pollution sources, the methods and measures of emission inventory quantification were applied and revised for the key pollution plant, combining with the national pollution census and the innovative methods for verifying the emission sources of key national controlled enterprises. The quantitative changellenge for fugitive emission of VOCs in petrochemical industry was studied and practiced. Additionally, the air pollution emission inventory in shanghai was developed, which contained the criteria pollutants of PM, PM_(10), PM_(2.5), SO_2, NO_X, CO, VOCs and NH_3 aiming for aerosol pollution control. The grid resolution of this emission inventory is for 1km×1km and the height is 1km, including 33 kinds of industrial point sources (12896 industrial enterprises), 20 kinds of domestic and industrial point sources, as well as the mobile sources such as motor vehicles, ships, aircraft and trains.
As shown by emission inventory of 2006, the total mass of all kinds of emission sources are 582,000 tons for PM, 279000 tons for PM_(10), 111000 tons for PM_(2.5), 564000 tons for SO_2, 464000 tons for NO_X, 1417000 tons for CO, 574000 tons for VOC, 14000 tons for NH_3, which is the highest in the world. Area emission is the major sources for PM, PM_(10), PM_(2.5), VOC and NH3. Point emission is the major source for SO_2 and NO_X. Mobil emission is the major source for CO, which contributed 46% of the total. The road dust is the major source for primary pollutants such as PM, PM_(10) and PM_(2.5), which contributed 54%, 45% and 26% respectively. The power plant and the fuel-firing of industry, contributing 57% and 12% of the total and was the key source of SO_2 which would transform into the secondary aerosol pollutant. The major source for NO_X is power plant and vehicles, which contributed 36% and 18% of the total mass in shanghai. The major sources for VOCs pollutant are coatings, tank and motor vehicles production process, which contributed 28%, 23% and 16% respectively. The major source of NH3 pollutant is from the breeding of livestock feeding, poultry and industrial process, which contributed 66.7% and 19.7% of the total emission mass in Shanghai.
In this study, MODEL3-CMAQ was used to analyze the source of the pollution in winter in shanghai, the scenario simulation was developed to analyze the contribution of different emission sources to the fine particle pollution in shanghai. The results showed that the concentration of PM_(10), PM_(2.5) in Shanghai was mainly influenced by area emission which contributed 68.3% of the concentration, and the mobile emission as well as the non-power plant next. The power plant emission was the major factor caused the continual high concentration of SO_2, which contributed the 32.1%, secondly is mobile and non power plant emission. The contribution of sources outside Shanghai was 15.3%. The mobile source is the major factor caused the high concentration of NO_2, next is power plant and non power generating industrial plant.
In this study, a great number of PM_(10) and PM_(2.5) data from ambient air monitoring network and aerosol sampling was analyzed. The results showed that the temporal variation exhibited high concentration in winter and spring (Jan. Mar. April, Nov. and Dec), low concentration in summer and autumn (Jul, Aug and Sep). The diurnal variation showed two peaks. And the spatial variation showed that low concentration of PM_(10) in eastern coastal areas and high concentration in northwestern areas. The average concentration of PM25/PM10 was more than 0.5 in Shanghai. The variation of gaseous pollutants was different from that of particle matter in different pollution episode. The SO_2/PM_(10) (0.38) value in serious haze days was significantly lower than that in good or moderate days, while PM_(2.5)/PM_(10) value significantly increased to 61%. The proportion of water-soluble components in PM_(2.5) accounted for 59%. SOR and NOR was to 0.67 and 0.61, respectively, which meant the sulfate, nitrate and ammonium transformed from primary SO_2 and NO_X. It was the key mechanism for the high concentration of PM_(2.5) in Shanghai. In the high pollution days influenced by long distance transport of dust storm, the ratios of SO_2/PM_(10),NO_2/PM_(10),PM_(2.5)/PM_(10) in ambient air of Shanghai have decreased to 0.066, 0.073 and 0.155. The values of SO_2/PM_(10),NO_2/PM_(10) and PM_(2.5)/PM_(10) could be used as the important index to identify the dust day, non-dust day or haze day in Shanghai.
The results of this study revealed the fine particle aerosol characteristics and changes in Shanghai. The characteristics, source and formation mechanism of aerosol, especially under the typical serious haze pollution and its impact on air quality, impact by the long distance transport of dust storm was clarified.
引文
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