基于太原市2013年5、6、12月和2014年1月大气中SO2、NO2及PM2.5中水溶性离子SO2-4 、NO-3 浓度,分析了大气中硫和氮的转化率( Fs、Fn ) ,并探讨了其影响因素.结果表明,大气中SO2、NO2的浓度夏季( 5、6月)分别为 89. 98、64. 73 μg·m-3 ,由于燃煤供热冬季( 12、1 月) SO2显著升高, SO2和 NO2分别为 119. 09、63.92 μg·m-3.PM2.5中水溶性离子SO2-4 、NO-3 夏季分别为16.54、6.87 μg·m-3,冬季显著降低,分别为12.79、5.53 μg·m-3.参照硫和氮气固两相转化模型,Fs夏季(0.13)高于冬季(0.07),Fn变化较小,夏、冬季分别为0.08、0.06,与南方城市相比,Fs较高,Fn较低.硫、氮转化受多种因素共同影响,且不同季节主导因素不同.温度和O3浓度对整个采样期间的硫转化起主要作用,冬季SO2-4 与PM2.5和湿度呈现一定的相关关系,显示SO2-4 主要来源于均相气相反应,冬季部分源于非均相反应.夏季相对湿度和O3浓度可明显促进氮转化,而冬季NO-3生成还与PM2.5和温度有关,说明夏季氮转化以均相液相反应为主,而冬季NO-3 主要源于非均相反应.此外, NH+4 与SO2-4 、NO-3 的线性分析表明,大气氨有助于气相中的硫、氮向颗粒相转移并转化.
The conversion ratios of sulfur and nitrogen ( F s and F n ) from air to particle in Taiyuan were discussed, based on the atmospheric SO2 and NO2 and the water soluble ions( SO2-4 and NO-3 ) in PM2.5 during two period of May—June 2013 ( summer ) and December 2013—January 2014 (winter).As the results showed, the SO2 and NO2 contents in summer were 89. 98 μg·m-3 and 64.73 μg·m-3 , respectively, while in winter NO2 level was constant, but SO2 increased to 119. 09μg·m-3 due to higher coal combustion for heating. The SO2-4 and NO-3 levels in PM2.5 were 16.54 and 6.87 μg·m-3 in summer, and decreased to 12.79 μg·m-3 and 5.53 μg·m-3 in winter, respectively. By using the modified forms of the gas-particle distribution, Fs and Fn were 0. 13 and 0. 08 in summer, and 0.07 and 0.06 in winter, respectively. Both Fs and Fn were affected by multiple factors simultaneously, and the main factors varied seasonally. Higher temperature and ozone ( O3 ) level contributed primarily to higher sulfur conversion, showing that SO2-4 mainly came from the homogeneous gas-phase reaction. However SO2-4 partially came from heterogeneous reactions in the winter because of a correlation between SO2-4 , PM2.5 and relative humidity ( RH,%) . Fn increased with relative humidity and O3 level in the summer, but in the winter NO-3 was partially affected by temperature and PM2.5 level. These indicated the homogeneous liquid-phase reaction played an important role in the process of nitrogen conversion in summer, but the heterogeneous reaction dominated in winter. Furthermore, NH+4 in PM2.5 was well correlated with SO2-4 and NO-3 , which indicated atmospheric NH3 may enhance the gas to particle sulfur and nitrogen migration and conversion.
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