燃煤电厂排放细颗粒物的水溶性无机离子特征综述

当前我国面临严重的大气细颗粒物(PM2.5)污染,燃煤电厂是大气中PM2.5的重要来源之一.为了实现国家"十一五"和"十二五"规划对二氧化硫(SO2)和氮氧化物(NOx)的总量减排目标,燃煤电厂大规模安装烟气脱硫和脱硝设施,这虽然减少了气态污染物转化生成的二次PM2.5,但另一方面也会对烟气中PM2.5的物理化学特征产生影响,有可能增加一次PM2.5的排放.本文综述了燃煤电厂排放PM2.5及其水溶性离子的粒径分布特征,重点介绍了脱硫和脱硝这两种烟气处理设施对燃煤电厂排放PM2.5的影响原理及相关研究结果,特别是对细颗粒物中水溶性离子(如SO2-4、Ca2+和NH+4)的影响.在目前我国PM2.5污染十分严重和燃煤电厂大量安装脱硫和脱硝装置的背景下,定量研究脱硫和脱硝对PM2.5排放特征的影响具有十分重要的意义.     

查干湖和新立城水库秋季水体悬浮颗粒物和CDOM吸收特性

分别于2012年9月对不同盐度水体的查干湖和新立城水进行水体野外采样和室内实验分析,通过测定颗粒物、CDOM等光学活性物质的吸收系数来对比分析两种水体的光学活性物质的吸收特性、来源及其在400~700 nm范围内对总吸收系数的贡献.结果表明,综合营养状态评价指数显示秋季查干湖、新立城水库水体属于中等富营养化,总悬浮颗粒物的吸收光谱表现均与色素类颗粒物吸收光谱相似.对于盐度较大的查干湖水体(EC=988.87μS·cm~(-1)),非藻类颗粒物占主导地位,各组分贡献率为非藻类颗粒物色素颗粒物CDOM;而盐度较低的新立城水库水体(EC=311.67μS·cm~(-1)),色素颗粒物贡献率略大于非藻类颗粒物贡献,各组分贡献率依次为:色素颗粒物非藻类颗粒物CDOM.查干湖总悬浮颗粒物吸收系数α_p(440)、α_p(675)和非藻类颗粒物吸收系数α_d(440)分别与TSM(总悬浮颗粒物)、ISM(无机悬浮颗粒物)和OSM(有机悬浮颗粒物)、Chl-a(叶绿素a)相关性均较好,相关系数在0.55以上;新立城水库α_p(440)、α_p(675)与Chl-a相关性较好(0.77和0.85,P0.05),α_d(440)与ISM具有相关性(0.74,P0.01),与OSM表现为负相关(-0.63,P0.05).查干湖CDOM吸收系数a_g(440)仅与OSM表现为负相关性(-0.54,P0.05),而新立城水库α_g(440)与其他参数均无相关性.通过对CDOM吸收曲线在250~400 nm的拟合所得到的S_g以及相对分子量M_r发现,查干湖的S_g[(0.021±0.001)m~(-1)]大于新立城的S_g[(0.017 6±0.001)m~(-1)],而CDOM的相对分子量M_r值分别为11.44±2.00(7.5~15.09)、7.53±0.79(6.17~8.89),查干湖M_r值高于新立城水库水体,表明查干湖CDOM组成较新立城水体中CDOM的分子量小,组成更趋向于小分子.查干湖受风速和湖岸坍塌的影响产生矿物悬浮、沉积微粒,水体颗粒物以非藻类为主,部分来自于浮游植物降解产物;新立城水库水体不仅有径流携带的陆源性无机物的输入,同时水体浮游植物生长减弱且微生物分解活动加强,降解有机颗粒物与非藻类吸收系数呈现负相关.     

Morphology, composition, and sources of individual aerosol particles at a regional background site of the YRD, China

Aerosol samples were collected at Lin'an, a background site of Yangtze River Delta(YRD).Morphology, size, composition, and mixing state of individual aerosol particles were characterized by transmission electron microscopy(TEM) coupled with energy dispersive X-ray spectroscopy(EDS), and the soluble ions of PM_(1.0) were studied by aerosol mass spectrometer(AMS). The daily average AMS mass concentrations of sulfate, nitrate, and ammonium were about 5.8, 8.6, and 5.6 μg/m~3, respectively. Individual aerosol particles were classified into seven types: S-rich, K-rich, organic matter(OM), soot, fly ash, metal, and mineral. S-rich particles were dominant in all size bins, and 51%(by number) of S-rich particles were internally mixed with other particles. The fraction of organic coating particles was 13.7% in morning, 25.2% in afternoon, and 11% in evening, suggesting that the strong photochemical process during afternoon produced more secondary organic aerosols(SOA) on the surface of inorganic particles. Fly ash and metal particles were abundant during the day, suggesting the influence of emissions from coal-fired power plants and steel plants. The results indicate that the intense industrial emissions in the YRD significantly transported to the background areas. PM_(2.5) concentration may be lower in background air than in urban air but complex mixing state of aerosol particles indicates that the long-range transported particles substantially influenced the background air quality.     

城市不同源雾霾颗粒物健康风险差异评估比较

通过研究不同来源霾颗粒物对大鼠气管上皮细胞（RTE cells）电阻抗变化和细胞自噬因子的影响,评价不同来源霾颗粒物对人体健康风险的差异性.分别将RTE暴露于从居民区（I）,高架交通源（Ⅱ）和化工园区（Ⅲ）采集的3种雾霾颗粒物中,统一暴露浓度和时间分别为100mg/L和24h.通过电子细胞基质阻抗检测（ECIS）细胞增长引起的阻抗变化和细胞电损伤恢复时间;通过蛋白免疫印迹测定p62,Atg5,Atg7,Beclin1,LC3B和mTOR蛋白表达量来分析比较不同来源雾霾颗粒物对RTE细胞自噬的影响.结果表明,与空白对照组相比,不同雾霾颗粒物处理组细胞电损伤恢复时间分别延长了34.6%,63.2%和78.0%;p62蛋白表达量差异显著性下降,Atg5,Atg7,Beclin1,LC3B蛋白表达量差异显著性上升.此外,mTOR相关蛋白表达量差异显著性下降,分别下降了4.38%,3.34%和2.36%;p-mTOR蛋白表达量与空白组相比,实验组I下降24.2%,实验组Ⅱ下降37.0%,实验组Ⅲ下降60.9%.由以上结果可知,不同来源雾霾颗粒物对RTE细胞均有一定的毒性损伤作用,能够减小细胞增长速度和削弱细胞修复能力,增强细胞自噬因子蛋白的表达,且化工园区采集的雾霾颗粒物毒性强于居民区和高架交通源.不同来源雾霾颗粒物的细胞毒性存在明显差异,基于细胞电损伤恢复时间的测定以及自噬相关蛋白的检测方法能够为雾霾颗粒物健康风险评价提供一种快速的生物学手段.     

西安冬季重污染过程PM2.5理化特征及来源解析

基于单颗粒气溶胶质谱仪（SPAMS）观测数据、颗粒物质量浓度数据和气象要素数据,研究了2017年11月西安市一次重污染过程中细颗粒物的化学组分特征及其成因,并使用正矩阵因子分析法（PMF）对细颗粒进行了来源解析.结果表明,西安市冬季重污染过程中细颗粒物主要类型为有机碳（OC）、元素碳（EC）、混合碳（ECOC）、富钾（K）、钠-钾（Na-K）、有机胺（amine）、矿尘（dust）和重金属（HM）,其主要来源为燃煤（24.9%）,二次（29.3%）,工业（19.3%）,交通（13.3%）,生物质燃烧（5.2%）和扬尘（1.9%）.通过对比分析不同污染过程细颗粒物的理化特征,发现高湿度,低风速的不利气象条件和供暖及工业生产导致的燃煤污染、二次污染,是此次重污染过程的主因.     

夏季持续高温天气对北京市大气细粒子(PM2.5)的影响

在1999-06-23北京市出现长达13d的持续高温期间对细粒子(PM_2.5)质量浓度进行了观测.数据表明,持续高温期间细粒子质量浓度比非高温期间要高出2～3倍.但是通过对持续高温期间的气象数据进行分析,发现还是很利于污染物扩散.进一步分析同步监测的O₃浓度、颗粒物中SO₄^2-的粒径范围及其含量等数据,发现夏季持续高温期间活跃的光化学反应应该是北京市细粒子的主要来源.     

北京市大气细粒子的来源分析

细粒子(空气动力学直径小于2.5μm的颗粒物)污染是许多城市重要的大气环境问题.从1999年至2000年对北京市细粒子展开了4次采样和化学分析,有效采样天数为40d.利用正定矩阵分解(PMF)方法对细粒子的来源进行了分析.化学成分包括EC(元素碳)、有机物、SO₄^2-、F^-、Cl^-、Fe、Ca、K、Mg、Al、Na、Zn、Mn、Ti、Pb、Ba和P等17种.发现主要来源有6类:地面扬尘、建筑源、生物质燃烧、二次源、机动车排放和燃煤.     

用核子微探针进行单个大气颗粒物的分析

本文对单个大气颗粒物进行了分析研究，用核子微探针对首钢地区单个大气颗粒物进行了扫描分析，用三维等高线法给出了各种元素在一群单个大气颗粒物中的二维分布。从一群单个大气颗粒物中各元素的二维分布可对首钢地区大气污染的特征及来源进行分析研究。     

Isomer distribution of nitrotriphenylenes in airborne particles, diesel exhaust particles, and the products of gas-phase radical-initiated nitration of triphenylene

The formation of mutagenic nitro-polycyclic aromatic hydrocarbons (NPAHs) 1- and 2-nitrotriphenylene (1- and 2-NTP) via gas-phase OH or NO₃ radical-initiated reactions of triphenylene was demonstrated for the first time using a flow reaction system. In contrast with the results of conventional electrophilic nitration, 2-NTP was formed in larger yield than 1-NTP, but this is consistent with the mechanism proposed for gas-phase radical-initiated nitration of PAH. In diesel exhaust particle (DEP) samples, both 1- and 2-NTP were identified and their concentrations determined, as well as 1-nitropyrene (1-NP), which is a representative combustion-derived NPAH: the mean concentrations of 1-NTP, 2-NTP, and 1-NP were 4.7, 1.9, and 32 pmol mg_DEP^–1, respectively. The mean 2-NTP/1-NTP, 1-NTP/1-NP, and 2-NTP/1-NP ratios in samples of airborne particles collected in a residential area in Osaka, Japan, were>1.55,<0.25, and 0.37, respectively; these values are much higher than those of the DEP samples. This finding indicates that there is another source for airborne NTPs, especially 2-NTP, apart from diesel exhaust. These results strongly suggest that airborne NTPs originate from atmospheric processes such as radical-initiated reactions of triphenylene, and this has a significant influence on the atmospheric occurrence of NTPs.     

Association of the mutagenicity of airborne particles with the direct emission from combustion processes investigated in Osaka, Japan

The association of the direct-acting mutagenicity of soluble organic fraction of airborne particles toward Salmonella typhimurium YG1024 strain with the direct emission was investigated at a roadside and at a residential area in Osaka, Japan. The direct-acting mutagenicity was evaluated as mutagenic activity per unit volume of ambient air (rev m⁻³) and/or that per airborne particulate weight collected on a filter (rev mg⁻¹). The annual or diurnal changes of the mutagenicity of airborne particles at the residential site showed similar patterns to those of some gaseous pollutants such as NO₂ and SO₂, which were emitted from combustion processes. This result indicates that the mutagenicity is mainly attributable to the primary emissions. From the analysis of the relationship between the wind sector and the mutagenic intensity, rev m⁻³ and rev mg⁻¹ values were strongly affected by the emissions from the fixed sources and from the mobile sources, respectively. The rev m⁻³ value and concentration of 1-nitropyrene (1-NP) in unit per m³ at the roadside were a factor of 2.6 and 2.8 higher than those at the residential site, respectively, but the rev mg⁻¹ value and concentration of 1-NP in unit per mg at the roadside were substantially comparable to those at the residential area. These observations suggest that the characteristics of the airborne particles can be attributed to the automotive emissions even at the suburban area.