南京市工业和商业区域可吸入颗粒物的污染特征及控制研究
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摘要
在南京市大厂地区和山西路两个采样点,用大流量采样器及PM_(10)切割器,逐月采集一年内大气环境中的可吸入颗粒物(PM_(10))样品。采用扫描电镜(SEM)和X射线能谱分析(EDX)等现代测试手段研究大气颗粒物的微观特征(形态、矿物成分、元素组成)。同时,研究南京市区不同功能分区、不同季节PM_(10)的污染变化规律。选择EPA指定的优先控制的16种PAHs作为待测物质,采用高效液相色谱技术,分析PM_(10)中PAHs的污染水平和浓度特征以及季节变化规律,并主要针对烹调源、交通源、焦化源、燃煤源等几种典型污染源排放的PM_(10)中的PAHs进行定性、定量分析。通过实验找出并比较各个污染源PAHs的组成及分布特征,建立源成分谱,在此基础上,运用CMB受体模型对PM_(10)上PAHs的来源进行解析。在“静电一颗粒层过滤复合技术”的基础上,设计形成了一种用于PM_(10)脱除的新型“静电—带电颗粒层过滤复合除尘技术”,通过理论分析阐明了其除尘机理和主要影响因素,并在自制带电颗粒的基础上,研究了PM_(10)脱除的最佳工艺条件。
(1)研究了南京大厂、山西路地区可吸入颗粒物物理特性及时空动态变化规律。
南京市两典型地区大气颗粒物非常复杂,大厂地区(典型工业区)多以规则的形态出现,块状、柱状、针状、层状、球状集合体为最常见,其成分以碳酸盐、硫酸盐、铝硅酸盐为主。山西路地区(典型商业区)多以不规则形态出现,常见烟尘集合体、生物质、不规则矿物等。从PM_(10)的月变化规律来看,南京市整年的PM10浓度均超过1996年《环境空气质量标准》规定的国家二级标准0.15mg·m~(-3),四个季度的PM10的浓度大小顺序为：春季>冬季>秋季>夏季,与当地的气候有一定的关系。从PM_(10)的空间变化来看,大厂地区(工业区)的PM_(10)浓度明显高于山西路(商业区)。PM_(10)污染比较严重,全年均超过了1996年颁布的《环境空气质量标准》中规定的PM_(10)的二级标准浓度,山西路地区有部分时间达到二级标准。
(2)南京大厂、山西路地区可吸入颗粒物中金属元素的组成特征及来源分析。
采用全谱直读等离子体发射光谱仪、流动注射-氢化物发生-原子吸收法、离子印迹壳聚糖／凹土有机-无机杂化材料分离富集-火焰原子吸收光谱法测定样品中15种金属元素的含量。应用富集因子法对金属元素的来源进行解析,在大厂地区PM10样品中Cr、Ni、Cu、Zn、Pb、Cd、As元素富集程度大,主要来源于人为源。山西路地区PM10样品中Ni、Cu、Zn、Pb、Cd、As元素富集程度大,主要来源于人为源。汽车尾气标记性元素Pb在山西路地区比大厂地区富集程度高,说明山西路地区受汽车尾气影响较大；Zn在大厂地区的富集程度较高,因Zn主要来自于金属冶炼,与大厂地区处于工业区有关。
(3)南京大厂、山西路地区可吸入颗粒物中PAHs的时空动态变化规律研究。
南京市大厂地区春、夏、秋、冬的PAHs平均浓度分别为107.256ng·m-3、21.890ng·m-3、111.839ng·m-3和88.605ng·m~(-3),山西路地区分别为76.276ng·m-3、52.904ng·m-342.561ng·m-3和75.815ng·m~(-3),大厂地区四季度PAHs平均浓度明显高于山西路地区,分别是山西路地区的1.406、2.304、2.628、1.169倍。大厂地区PHAs总量受季节影响不大,山西路地区浓度与季节呈一定的相关性,即春季>冬季>夏季>秋季,两地区PHAs中蒽、荧蒽、苯并[b]荧葸、苯并[g,h,i]苝含量相对都较高,表明燃煤和交通是南京市的主要污染源,大厂区燃煤污染更为明显。两地区PAHs的浓度变化与PM10的浓度变化没有相关性,各自的浓度变化也没有规律性。
(4)南京大厂、山西路地区可吸入颗粒物源解析研究。
建立大厂和山西路地区化学质量平衡(CMB)受体源解析模型,并对模型进行求解,从而确定大厂和山西路地区各污染源的贡献值。各污染源对大厂地区PAHs的贡献率分别为：燃煤源12.48%,交通源25.61%,焦化源52.16%,烹调源9.75%。这表明大厂地区PAHs的主要污染源是焦化源、其次是交通源,两者占总量的77.79%。各污染源对山西路PAHs的贡献率为：燃煤源9.65%,交通源25.55%,焦化源52.83%,烹调源11.97%；这表明山西路PAHs的主要污染源是交通源和焦化源,两者占总量的78.38%。
(5)静电—带电颗粒层过滤复合除尘技术对PM1o的控制。
采用“静电—带电颗粒层过滤复合除尘技术”,使静电除尘器除尘后荷电的PM10进入带电颗粒层过滤器,通过颗粒层过滤的方式去除。壳聚糖／凹土为带电颗粒较理想的制备材料,壳聚糖／凹土改性的最优条件是：壳聚糖溶胶与凹土的比例(质量比)为1.5：1,反应温度为50℃,反应时间为3.5h。在该最优条件下,壳聚糖在凹土上的负载率(%)为40.26%,改性操作的工艺稳定性良好。通过XRD、FTIR和热分析证实壳聚糖在凹土表面已成功负载,经测定壳聚糖／凹土的Zeta电位为：+46.28mV,带正电。带电颗粒层过滤器对PM1o脱除的最佳工艺条件是：过滤时间为70min,过滤风速为0.42m·s-1,过滤层厚度为30mm,过滤颗粒粒径为0.756mm、颗粒均一性为1.32,PM10浓度为600μg·m~(-3)。工艺稳定性良好,易于工业化放大使用。
Dachang and Shanxi Road region were selected as inspected spots in Nanjing. Samples of inhalable particles(PM10) in ambient air were gathered month by month for one year, using big flux sampling equipment and PM10incision equipment. Scanning Electron Microscope and X-ray energy dispersive spectrometer were used to analyze the morphology and chemical composition of inhalable particles. At the same time, the PM10pollution change laws of different functional partition, different season of Nanjing city was studied.16PAHs were selected as the EPA designated materials with priority control. The PAHs level of pollution, concentration characteristics and seasonal change law was analyzed by using high performance liquid chromatography. The PAHs in the PM10of several typical pollution sources (coal combustion, coke plant, motor vehicle and dining hall) were analysed qualitatively and quantitatively. The composition and distribution of PAHs of different pollution sources were compared to each other, and, the source components spectrum were collected. Then, The CMB receptor model was used to analyse the sources of PAHs in the PM10. Baesd on the "electrostatic-granular layer filtration composite technology", a new type of "electrostatic-charged particle layer filtration compound dust removal technology" has been designed in this research for removing PM10. Theoretical analysis illustrated the dust removal mechanism and the main influence factors. Homemade charged particles were used to study the best removing process conditions of the PM10.
(1) Study on the PM10physical characteristics and space-time dynamic change rule of Dachang area and Shanxi Road in Nanjing
Atmospheric particulates in two typical areas of Nanjing are very complex, Dachang area (a typical industrial zone) shows a more inerratic pattern, such as massive, the columnar, needle, layer, globular aggregation are commonly inspected, with carbonate, sulfate, aluminum silicate as ingredients primarily. But, Shanxi Road (a typical business district) shows a irregular pattern, such as smoke, biomass, common collection of irregular minerals, etc., PM10concentration in Nanjing is higher than the secondary standard in1996national environmental air quality standards. The order of the concentration of PM10of four different seasons is:spring> summer> autumn> winter, which is relative to the local climate. PM10concentration of Dachang is significantly higher than Shanxi Road from a region of view, and the PM10concentration in Shanxi Road is beyond the secondary standard sometimes. Overall, the PM10pollution is heavy, which exceeds the secondary standard in1996national environmental air quality standards.
(2) The composition characteristics and source analysis of the metal elements in PM10in Nanjing
15metal elements are determined by ICP-AES, Hydrogenation method and ions imprinted method. Analysis shows that enrichment factor of Cr、Ni、Cu、Zn、Pb、Cd、As of Dachang and Ni、Cu、Zn、Pb、Cd、As of Shanxi Road are greater than10, the results indicate that these elements mainly come from anthropogenie Pollution. PM10of Shanxi Road mainly come from vehicle exhausts, and Dachang was mainly sourced from industrial pollution.
(3) The space-time dynamic change regulation research of PAHs in PM10in Nanjing
The average PAHs concentration of Spring, Summer, Autumn, Winter in Dachang area is107.256ng·m-3、121.890ng·m-3、111.839ng·m-3and88.605ng·m-3, respectively, and in Shanxi Road is76.276ng·m-3、52.904ng·m-3、42.561ng·m-3and75.815ng·m-3, respectively. The average PAHs concentration of four seasons in Dachang was significantly higher than that of Shanxi Road, and the proportion is1.406,2.304,2.628,1.169times respectively. Seasonal condition had a slight influence on the total amount of PAHs in Dachang area, while the seasonal variation are found in the concentration of PAHs in Shanxi road. The highest concentration was observed in spring with the lowest level in Autumn, and the value in winter was higher than that in summer. The contents of Anthracene, Fluoranthene, Benzo [b] fluoranthene, and Benzo [g,h,i] perylene in the two locations are petty high, exhibiting that coal combustion and traffic were the predominant sources for the pollution of Nanjin city, and the pollution from coal combustion was more severe in Dachang area.
(4) Source assignment of PM10in Dachang area and Shanxi Road region
Chemical Mass Balance (CMB) receptor models is established to simulate the pollution of Dachang area and Shanxi Road region, so as to determine the contribution of the pollution sources. The PAHs contribution rates of coal combustion, motor vehicle, coke-source and dining hall were obtained, with12.48%,25.61%,52.16%and9.75%in Dachang and9.65%,25.55%,52.83%and11.97%in Shanxi Road, respectively. This suggests that the main sources of PAHs are coke-source and traffic source in both areas.
(5). Control of PM10with electrostatic-charged particle layer filtration compound dust removal technology
According to the "Electrostatic-charged particle layer filtration compound dust removal technology", passing through the electrostatic precipitator, the PM10is charged. Then the charged PM10was removed by the charged particle layer filter. Chitosan/attapulgite is an ideal charged particle material. The optimal condition for chitosan/attapulgite composition is that mix chitosan sol and attapulgite at1.5:1mass ration, and react3.5h at50℃. In the optimal conditions, the load rate(%) of chitosan in attapulgite is40.26%, with good modification stability. XRD, FT-IR and thermal analysis confirmed that the chitosan is successful loaded on the attapulgite surface. Chitosan/attapulgite Zeta potential is+46.28mV, and carrys positive electricity. The best removing process condition of charged particle filter of PM10is filtering time is70min, filter wind speed is0.42m·s-1, filter layer thickness is30mm, filtering particle diameter is0.756mm, particle uniformity is1.32, concentration of PM10is600μg·m-3. This process is very steady and good for industrialization amplification.
(1)研究了南京大厂、山西路地区可吸入颗粒物物理特性及时空动态变化规律。
南京市两典型地区大气颗粒物非常复杂,大厂地区(典型工业区)多以规则的形态出现,块状、柱状、针状、层状、球状集合体为最常见,其成分以碳酸盐、硫酸盐、铝硅酸盐为主。山西路地区(典型商业区)多以不规则形态出现,常见烟尘集合体、生物质、不规则矿物等。从PM_(10)的月变化规律来看,南京市整年的PM10浓度均超过1996年《环境空气质量标准》规定的国家二级标准0.15mg·m~(-3),四个季度的PM10的浓度大小顺序为：春季>冬季>秋季>夏季,与当地的气候有一定的关系。从PM_(10)的空间变化来看,大厂地区(工业区)的PM_(10)浓度明显高于山西路(商业区)。PM_(10)污染比较严重,全年均超过了1996年颁布的《环境空气质量标准》中规定的PM_(10)的二级标准浓度,山西路地区有部分时间达到二级标准。
(2)南京大厂、山西路地区可吸入颗粒物中金属元素的组成特征及来源分析。
采用全谱直读等离子体发射光谱仪、流动注射-氢化物发生-原子吸收法、离子印迹壳聚糖／凹土有机-无机杂化材料分离富集-火焰原子吸收光谱法测定样品中15种金属元素的含量。应用富集因子法对金属元素的来源进行解析,在大厂地区PM10样品中Cr、Ni、Cu、Zn、Pb、Cd、As元素富集程度大,主要来源于人为源。山西路地区PM10样品中Ni、Cu、Zn、Pb、Cd、As元素富集程度大,主要来源于人为源。汽车尾气标记性元素Pb在山西路地区比大厂地区富集程度高,说明山西路地区受汽车尾气影响较大；Zn在大厂地区的富集程度较高,因Zn主要来自于金属冶炼,与大厂地区处于工业区有关。
(3)南京大厂、山西路地区可吸入颗粒物中PAHs的时空动态变化规律研究。
南京市大厂地区春、夏、秋、冬的PAHs平均浓度分别为107.256ng·m-3、21.890ng·m-3、111.839ng·m-3和88.605ng·m~(-3),山西路地区分别为76.276ng·m-3、52.904ng·m-342.561ng·m-3和75.815ng·m~(-3),大厂地区四季度PAHs平均浓度明显高于山西路地区,分别是山西路地区的1.406、2.304、2.628、1.169倍。大厂地区PHAs总量受季节影响不大,山西路地区浓度与季节呈一定的相关性,即春季>冬季>夏季>秋季,两地区PHAs中蒽、荧蒽、苯并[b]荧葸、苯并[g,h,i]苝含量相对都较高,表明燃煤和交通是南京市的主要污染源,大厂区燃煤污染更为明显。两地区PAHs的浓度变化与PM10的浓度变化没有相关性,各自的浓度变化也没有规律性。
(4)南京大厂、山西路地区可吸入颗粒物源解析研究。
建立大厂和山西路地区化学质量平衡(CMB)受体源解析模型,并对模型进行求解,从而确定大厂和山西路地区各污染源的贡献值。各污染源对大厂地区PAHs的贡献率分别为：燃煤源12.48%,交通源25.61%,焦化源52.16%,烹调源9.75%。这表明大厂地区PAHs的主要污染源是焦化源、其次是交通源,两者占总量的77.79%。各污染源对山西路PAHs的贡献率为：燃煤源9.65%,交通源25.55%,焦化源52.83%,烹调源11.97%；这表明山西路PAHs的主要污染源是交通源和焦化源,两者占总量的78.38%。
(5)静电—带电颗粒层过滤复合除尘技术对PM1o的控制。
采用“静电—带电颗粒层过滤复合除尘技术”,使静电除尘器除尘后荷电的PM10进入带电颗粒层过滤器,通过颗粒层过滤的方式去除。壳聚糖／凹土为带电颗粒较理想的制备材料,壳聚糖／凹土改性的最优条件是：壳聚糖溶胶与凹土的比例(质量比)为1.5：1,反应温度为50℃,反应时间为3.5h。在该最优条件下,壳聚糖在凹土上的负载率(%)为40.26%,改性操作的工艺稳定性良好。通过XRD、FTIR和热分析证实壳聚糖在凹土表面已成功负载,经测定壳聚糖／凹土的Zeta电位为：+46.28mV,带正电。带电颗粒层过滤器对PM1o脱除的最佳工艺条件是：过滤时间为70min,过滤风速为0.42m·s-1,过滤层厚度为30mm,过滤颗粒粒径为0.756mm、颗粒均一性为1.32,PM10浓度为600μg·m~(-3)。工艺稳定性良好,易于工业化放大使用。
Dachang and Shanxi Road region were selected as inspected spots in Nanjing. Samples of inhalable particles(PM10) in ambient air were gathered month by month for one year, using big flux sampling equipment and PM10incision equipment. Scanning Electron Microscope and X-ray energy dispersive spectrometer were used to analyze the morphology and chemical composition of inhalable particles. At the same time, the PM10pollution change laws of different functional partition, different season of Nanjing city was studied.16PAHs were selected as the EPA designated materials with priority control. The PAHs level of pollution, concentration characteristics and seasonal change law was analyzed by using high performance liquid chromatography. The PAHs in the PM10of several typical pollution sources (coal combustion, coke plant, motor vehicle and dining hall) were analysed qualitatively and quantitatively. The composition and distribution of PAHs of different pollution sources were compared to each other, and, the source components spectrum were collected. Then, The CMB receptor model was used to analyse the sources of PAHs in the PM10. Baesd on the "electrostatic-granular layer filtration composite technology", a new type of "electrostatic-charged particle layer filtration compound dust removal technology" has been designed in this research for removing PM10. Theoretical analysis illustrated the dust removal mechanism and the main influence factors. Homemade charged particles were used to study the best removing process conditions of the PM10.
(1) Study on the PM10physical characteristics and space-time dynamic change rule of Dachang area and Shanxi Road in Nanjing
Atmospheric particulates in two typical areas of Nanjing are very complex, Dachang area (a typical industrial zone) shows a more inerratic pattern, such as massive, the columnar, needle, layer, globular aggregation are commonly inspected, with carbonate, sulfate, aluminum silicate as ingredients primarily. But, Shanxi Road (a typical business district) shows a irregular pattern, such as smoke, biomass, common collection of irregular minerals, etc., PM10concentration in Nanjing is higher than the secondary standard in1996national environmental air quality standards. The order of the concentration of PM10of four different seasons is:spring> summer> autumn> winter, which is relative to the local climate. PM10concentration of Dachang is significantly higher than Shanxi Road from a region of view, and the PM10concentration in Shanxi Road is beyond the secondary standard sometimes. Overall, the PM10pollution is heavy, which exceeds the secondary standard in1996national environmental air quality standards.
(2) The composition characteristics and source analysis of the metal elements in PM10in Nanjing
15metal elements are determined by ICP-AES, Hydrogenation method and ions imprinted method. Analysis shows that enrichment factor of Cr、Ni、Cu、Zn、Pb、Cd、As of Dachang and Ni、Cu、Zn、Pb、Cd、As of Shanxi Road are greater than10, the results indicate that these elements mainly come from anthropogenie Pollution. PM10of Shanxi Road mainly come from vehicle exhausts, and Dachang was mainly sourced from industrial pollution.
(3) The space-time dynamic change regulation research of PAHs in PM10in Nanjing
The average PAHs concentration of Spring, Summer, Autumn, Winter in Dachang area is107.256ng·m-3、121.890ng·m-3、111.839ng·m-3and88.605ng·m-3, respectively, and in Shanxi Road is76.276ng·m-3、52.904ng·m-3、42.561ng·m-3and75.815ng·m-3, respectively. The average PAHs concentration of four seasons in Dachang was significantly higher than that of Shanxi Road, and the proportion is1.406,2.304,2.628,1.169times respectively. Seasonal condition had a slight influence on the total amount of PAHs in Dachang area, while the seasonal variation are found in the concentration of PAHs in Shanxi road. The highest concentration was observed in spring with the lowest level in Autumn, and the value in winter was higher than that in summer. The contents of Anthracene, Fluoranthene, Benzo [b] fluoranthene, and Benzo [g,h,i] perylene in the two locations are petty high, exhibiting that coal combustion and traffic were the predominant sources for the pollution of Nanjin city, and the pollution from coal combustion was more severe in Dachang area.
(4) Source assignment of PM10in Dachang area and Shanxi Road region
Chemical Mass Balance (CMB) receptor models is established to simulate the pollution of Dachang area and Shanxi Road region, so as to determine the contribution of the pollution sources. The PAHs contribution rates of coal combustion, motor vehicle, coke-source and dining hall were obtained, with12.48%,25.61%,52.16%and9.75%in Dachang and9.65%,25.55%,52.83%and11.97%in Shanxi Road, respectively. This suggests that the main sources of PAHs are coke-source and traffic source in both areas.
(5). Control of PM10with electrostatic-charged particle layer filtration compound dust removal technology
According to the "Electrostatic-charged particle layer filtration compound dust removal technology", passing through the electrostatic precipitator, the PM10is charged. Then the charged PM10was removed by the charged particle layer filter. Chitosan/attapulgite is an ideal charged particle material. The optimal condition for chitosan/attapulgite composition is that mix chitosan sol and attapulgite at1.5:1mass ration, and react3.5h at50℃. In the optimal conditions, the load rate(%) of chitosan in attapulgite is40.26%, with good modification stability. XRD, FT-IR and thermal analysis confirmed that the chitosan is successful loaded on the attapulgite surface. Chitosan/attapulgite Zeta potential is+46.28mV, and carrys positive electricity. The best removing process condition of charged particle filter of PM10is filtering time is70min, filter wind speed is0.42m·s-1, filter layer thickness is30mm, filtering particle diameter is0.756mm, particle uniformity is1.32, concentration of PM10is600μg·m-3. This process is very steady and good for industrialization amplification.
引文
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