苏州市大气中汞的形态分布特征及来源分析

针对苏州市大气中汞的分布特征和污染来源,自2018年1月1日至2018年12月31日对苏州市大气中的气态元素汞(GEM)、气态氧化汞(GOM)和颗粒态汞(PBM)进行1 a的连续监测,并基于浓度权重轨迹分析法(CWT)和浓度玫瑰图法,研究2018年大气汞来源和浓度变化规律.结果表明,监测期间苏州市大气中GEM、GOM和PBM浓度分别在0～53.3 ng·m~(-3)、 0～256 pg·m~(-3)和0～5 208 pg·m~(-3),年均浓度分别为(2.57±2.09)ng·m~(-3)、(5.27±15.7)pg·m~(-3)和(16.0±157)pg·m~(-3).其中,GEM是苏州市大气汞的主要成分,约占99.2%.监测期间,苏州市大气中GEM季节平均浓度表现出冬季(3.17 ng·m~(-3))春季(3.09 ng·m~(-3))秋季(2.30 ng·m~(-3))夏季(1.98 ng·m~(-3))的规律.根据CWT分析结果,苏州大气中汞迁移具有季节性差异:春季和冬季的含汞气团主要来自于内陆,夏季主要来自于苏州本地、黄海和东海,秋季的含汞气团来自于内陆、黄海和渤海.同时研究发现西北方向来自内陆的大气汞浓度较高,东方向来自海洋的大气汞浓度较低.苏州市大气中GEM和PBM平均浓度表现为昼间低夜间高,与大气参数进行相关性拟合,得出大气中GEM日变化规律与太阳总辐射亦呈显著的相关性(r=-0.664,P0.001),与湿度呈显著的相关性(r=0.859,P0.001),与气温呈显著的相关性(r=-0.866,P0.001); PBM与太阳总辐射呈一般相关性(r=-0.554,P0.01),与湿度呈显著的相关性(r=0.835,P0.001),与气温呈显著的相关性(r=-0.831,P0.001).苏州市大气中GOM平均浓度在1 d内出现多次峰值(05:00、 12:00、 18:00和23:00)和谷值(02:00、 10:00、 15:00和19:00).GOM浓度升高与早晚高峰燃料油燃烧排放正相关,亦与O_3浓度升高导致GEM氧化生成GOM正相关.

Distribution Characteristics and Source Analysis of Atmospheric Mercury Speciation in Suzhou

To explore the variation of mercury in the atmosphere in Suzhou, continuous monitoring of gaseous element mercury (GEM), gaseous oxidized mercury (GOM), and particulate bound mercury (PBM) was conducted from January 1 to December 31, 2018, in Suzhou. The weights trajectory analysis method (CWT) and concentration rose were used to analyze the atmospheric mercury sources and concentration variation. The results showed that during the monitoring period, the concentration ranges of GEM, GOM, and PBM in Suzhou were 0-53.3 ng·m^-3, 0-256 pg·m^-3, and 0-5208 pg·m^-3, respectively. The corresponding annual average concentrations of the three mercury species were (2.57±2.09) ng·m^-3, (5.27±15.7) pg·m^-3, and (16.0±157) pg·m^-3, respectively. GEM was the main component of atmospheric mercury in Suzhou. During the monitoring period, the average concentration of GEM in Suzhou was highest in winter, higher in spring than in autumn, and lowest in summer. According to the CWT, the mercury-containing air mass in spring and winter predominantly originated from inland; in summer, it mainly originated from the local area, the Yellow Sea, and the East China Sea, and in autumn from inland, the Yellow Sea, and the Bohai Sea. The wind and mercury rose charts showed that atmospheric mercury concentrations were higher from inland and lower from the ocean. During the monitoring period, the average concentrations of GEM and PBM in Suzhou were lower during the day than the night. The diurnal variation of GEM and PBM was significantly and strongly correlated with solar radiation, humidity, and air temperature. The average concentration of GOM showed multiple peaks and valleys in one day. Some peaks were caused by fuel oil combustion emissions, and some by O₃ oxidation with GEM.