School of Physics and Centre for Climate and Air Pollution Studies, Ryan Institute, National University of Ireland Galway, Galway, Ireland; Institut de Ciències del Mar, CSIC, Pg Marítim de la Barceloneta 37-49 Barcelona, Spain.
Department of Chemistry and Environmental Research Institute, University College Cork, Cork, Ireland; Laboratoire Chimie Environment, Aix Marseille Université, Marseille 13 331, France.
Sci Total Environ. 2014 Sep 15;493:197-208. doi: 10.1016/j.scitotenv.2014.05.027. Epub 2014 Jun 17.
The sources of ambient fine particulate matter (PM2.5) during wintertime at a background urban location in Cork city (Ireland) have been determined. Aerosol chemical analyses were performed by multiple techniques including on-line high resolution aerosol time-of-flight mass spectrometry (Aerodyne HR-ToF-AMS), on-line single particle aerosol time-of-flight mass spectrometry (TSI ATOFMS), on-line elemental carbon-organic carbon analysis (Sunset_EC-OC), and off-line gas chromatography/mass spectrometry and ion chromatography analysis of filter samples collected at 6-h resolution. Positive matrix factorization (PMF) has been carried out to better elucidate aerosol sources not clearly identified when analyzing results from individual aerosol techniques on their own. Two datasets have been considered: on-line measurements averaged over 2-h periods, and both on-line and off-line measurements averaged over 6-h periods. Five aerosol sources were identified by PMF in both datasets, with excellent agreement between the two solutions: (1) regional domestic solid fuel burning--"DSF_Regional," 24-27%; (2) local urban domestic solid fuel burning--"DSF_Urban," 22-23%; (3) road vehicle emissions--"Traffic," 15-20%; (4) secondary aerosols from regional anthropogenic sources--"SA_Regional" 9-13%; and (5) secondary aged/processed aerosols related to urban anthropogenic sources--"SA_Urban," 21-26%. The results indicate that, despite regulations for restricting the use of smoky fuels, solid fuel burning is the major source (46-50%) of PM2.5 in wintertime in Cork, and also likely other areas of Ireland. Whilst wood combustion is strongly associated with OC and EC, it was found that peat and coal combustion is linked mainly with OC and the aerosol from these latter sources appears to be more volatile than that produced by wood combustion. Ship emissions from the nearby port were found to be mixed with the SA_Regional factor. The PMF analysis allowed us to link the AMS cooking organic aerosol factor (AMS_PMF_COA) to oxidized organic aerosol, chloride and locally produced nitrate, indicating that AMS_PMF_COA cannot be attributed to primary cooking emissions only. Overall, there are clear benefits from factor analysis applied to results obtained from multiple techniques, which allows better association of aerosols with sources and atmospheric processes.
在科克市(爱尔兰)的一个背景城市位置,确定了冬季环境细颗粒物(PM2.5)的来源。气溶胶化学分析采用了多种技术,包括在线高分辨率气溶胶飞行时间质谱(Aerodyne HR-ToF-AMS)、在线单颗粒气溶胶飞行时间质谱(TSI ATOFMS)、在线元素碳-有机碳分析(Sunset_EC-OC)以及离线气相色谱/质谱和离子色谱分析以 6 小时分辨率采集的滤膜样品。采用正定矩阵因子分解(PMF)更好地阐明了在单独分析单个气溶胶技术的结果时未明确识别的气溶胶源。考虑了两个数据集:在线测量值,平均每 2 小时一次,以及在线和离线测量值,平均每 6 小时一次。PMF 在两个数据集中共识别出 5 个气溶胶源,两个解决方案之间具有极好的一致性:(1)区域家用固体燃料燃烧 - “DSF_Regional”,24-27%;(2)当地城市家用固体燃料燃烧 - “DSF_Urban”,22-23%;(3)道路车辆排放 - “Traffic”,15-20%;(4)区域人为源二次气溶胶 - “SA_Regional”,9-13%;以及(5)与城市人为源相关的二次老化/处理气溶胶 - “SA_Urban”,21-26%。结果表明,尽管有法规限制使用烟尘燃料,但在科克市冬季,固体燃料燃烧仍是 PM2.5 的主要来源(46-50%),并且可能也是爱尔兰其他地区的主要来源。虽然木材燃烧与 OC 和 EC 强烈相关,但发现泥炭和煤炭燃烧主要与 OC 有关,并且来自这些源的气溶胶似乎比木材燃烧产生的气溶胶更易挥发。附近港口的船舶排放物被发现与 SA_Regional 因子混合。PMF 分析使我们能够将 AMS 烹饪有机气溶胶因子(AMS_PMF_COA)与氧化有机气溶胶、氯化物和本地产生的硝酸盐联系起来,表明 AMS_PMF_COA 不能仅归因于初级烹饪排放。总体而言,对多种技术获得的结果进行因子分析有明显的好处,这可以更好地将气溶胶与源和大气过程联系起来。