成都冬季PM_(2.5)化学组分污染特征及来源解析
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摘要
2017年1月1~20日在成都地区分昼夜对PM_(2.5)进行连续膜样品采集,并在实验室测定了其主要化学组分(水溶性离子和碳质组分)的质量浓度.观测期间,PM_(2.5)的平均质量浓度为(127.1±59.9)μg·m~(-3);总水溶性离子的质量浓度为(56.5±25.7)μg·m~(-3),其中SO2-4、NO-3和NH+4是最主要的离子,质量浓度分别为(13.6±5.5)、(21.4±12.0)和(13.3±5.7)μg·m~(-3),一共占到了水溶性离子的85.6%;有机碳(OC)和元素碳(EC)的平均质量浓度分别为34.0μg·m~(-3)和6.1μg·m~(-3),分别占PM_(2.5)质量浓度的26.8%和4.8%.昼夜污染对比显示,PM_(2.5)白天和夜晚质量浓度分别为(120.4±56.4)μg·m~(-3)和(133.8±64.0)μg·m~(-3),夜间污染更为严重.SO2-4、NO-3和NH+4白天浓度高于夜间,这与白天光照促进了二次离子的形成有关;而Cl-、K+、OC和EC浓度夜间明显升高,可能是受夜间煤和生物质燃烧排放增加的影响.通过对近年来成都冬季PM_(2.5)化学组分的研究进行文献总结和比较后发现,SO2-4浓度显著降低,从2010年的50.6μg·m~(-3)降低到2017年的13.6μg·m~(-3);而NO-3浓度变化不大,维持在20μg·m~(-3)左右.PM_(2.5)中离子酸碱平衡分析表明,成都冬季PM_(2.5)由于NH+4的相对过剩而呈现出碱性,与以往呈偏酸性结果存在差异.对成都冬季NO-3/SO2-4的比值进行计算,NO-3/SO2-4平均值为1.57,表明移动源对PM_(2.5)污染影响更大.OC与EC的相关性表明,白天和夜间OC与EC的相关系数分别为0.82和0.90(P<0.01),OC与EC来源具有一致性.SOC估算结果显示,白天和夜间SOC浓度分别为8.5μg·m~(-3)和11.9μg·m~(-3),占到OC的28.1%和31.8%.K+/EC平均值为0.31,并且K+与OC之间相关系数为0.87(P<0.01),说明生物质燃烧对成都冬季碳质气溶胶有一定影响.主成分分析表明,成都冬季PM_(2.5)主要来源于燃烧源(燃煤、生物质燃烧等)、二次无机污染源以及土壤和扬尘源,其贡献率分别为32.8%、34.5%和21.5%.
Day-night PM_(2.5) samples were continuously collected in Chengdu from January 1 to 20,2017,and the concentrations of major chemical components(water-soluble ions and carbonaceous components) were measured in the laboratory.During the observation period,the average mass concentration of PM_(2.5) was(127.1 ± 59.9) μg·m~(-3).The mass concentration of water-soluble ions was(56.5 ± 25.7) μg·m~(-3) and SO2-4,NO-3,and NH+4 were the most dominant ions with a concentration of(13.6 ± 5.5),(21.4 ± 12.0),and(13.3 ± 5.7) μg·m~(-3),respectively,accounting for 85.6% of the water-soluble ions.The average mass concentrations of organic carbon(OC) and elemental carbon(EC) were 34.0 and 6.1 μg·m~(-3),respectively,accounting for 26.8%and 4.8% of the PM_(2.5) mass concentration,respectively.The comparison of the average day-night concentration shows that the daytime and nighttime mass concentrations of PM_(2.5) are(120.4 ± 56.4) and(133.8 ± 64.0) μg·m~(-3),respectively,and that the nighttime pollution is more serious.The SO2-4,NO-3,and NH+4 concentrations are higher during the day than at night,which is related to daytime light,which promotes the formation of secondary ions.The Cl-,K+,OC,and EC concentrations increase significantly,which may be affected by increased emissions from coal and material combustion.Based on the literature review and comparison of thewinter chemical composition of PM_(2.5) in Chengdu in recent years,the SO2-4 concentration significantly decreases from 50.6 μg·m~(-3) in2010 to 13.6 μg·m~(-3) in 2017.The NO-3 concentration changes little;it is maintained at ~ 20 μg·m~(-3).The analysis of the acid-alkali ion balance shows that PM_(2.5) in Chengdu is alkaline due to the relative overgrowth of NH+4,which is different from previous partially acidic results.The average value of NO-3/SO2-4 is 1.57.Mobile sources have a greater impact on the PM_(2.5) pollution in Chengdu in winter.The correlation coefficients of OC and EC between daytime and nighttime are 0.82 and 0.90,respectively(P<0.01),which indicates that the OC and EC sources are consistent.The SOC estimation shows that the SOC concentrations during the day and night are 8.5 μg·m~(-3) and 11.9 μg·m~(-3),respectively,accounting for 28.1% and 30.8% of the OC,respectively.The K+/EC average value is 0.31 and the correlation coefficient between K+and OC is 0.87(P<0.01),indicating that biomass combustion has a certain influence on the carbonaceous aerosol in Chengdu in winter.The principal component analysis shows that the winter PM_(2.5) in Chengdu mainly originates from combustion sources(coal burning,biomass burning,etc.),secondary inorganic sources,and soil and dust sources.The contribution rates are 32.8%,34.5%,and 21.5%,respectively.
Day-night PM_(2.5) samples were continuously collected in Chengdu from January 1 to 20,2017,and the concentrations of major chemical components(water-soluble ions and carbonaceous components) were measured in the laboratory.During the observation period,the average mass concentration of PM_(2.5) was(127.1 ± 59.9) μg·m~(-3).The mass concentration of water-soluble ions was(56.5 ± 25.7) μg·m~(-3) and SO2-4,NO-3,and NH+4 were the most dominant ions with a concentration of(13.6 ± 5.5),(21.4 ± 12.0),and(13.3 ± 5.7) μg·m~(-3),respectively,accounting for 85.6% of the water-soluble ions.The average mass concentrations of organic carbon(OC) and elemental carbon(EC) were 34.0 and 6.1 μg·m~(-3),respectively,accounting for 26.8%and 4.8% of the PM_(2.5) mass concentration,respectively.The comparison of the average day-night concentration shows that the daytime and nighttime mass concentrations of PM_(2.5) are(120.4 ± 56.4) and(133.8 ± 64.0) μg·m~(-3),respectively,and that the nighttime pollution is more serious.The SO2-4,NO-3,and NH+4 concentrations are higher during the day than at night,which is related to daytime light,which promotes the formation of secondary ions.The Cl-,K+,OC,and EC concentrations increase significantly,which may be affected by increased emissions from coal and material combustion.Based on the literature review and comparison of thewinter chemical composition of PM_(2.5) in Chengdu in recent years,the SO2-4 concentration significantly decreases from 50.6 μg·m~(-3) in2010 to 13.6 μg·m~(-3) in 2017.The NO-3 concentration changes little;it is maintained at ~ 20 μg·m~(-3).The analysis of the acid-alkali ion balance shows that PM_(2.5) in Chengdu is alkaline due to the relative overgrowth of NH+4,which is different from previous partially acidic results.The average value of NO-3/SO2-4 is 1.57.Mobile sources have a greater impact on the PM_(2.5) pollution in Chengdu in winter.The correlation coefficients of OC and EC between daytime and nighttime are 0.82 and 0.90,respectively(P<0.01),which indicates that the OC and EC sources are consistent.The SOC estimation shows that the SOC concentrations during the day and night are 8.5 μg·m~(-3) and 11.9 μg·m~(-3),respectively,accounting for 28.1% and 30.8% of the OC,respectively.The K+/EC average value is 0.31 and the correlation coefficient between K+and OC is 0.87(P<0.01),indicating that biomass combustion has a certain influence on the carbonaceous aerosol in Chengdu in winter.The principal component analysis shows that the winter PM_(2.5) in Chengdu mainly originates from combustion sources(coal burning,biomass burning,etc.),secondary inorganic sources,and soil and dust sources.The contribution rates are 32.8%,34.5%,and 21.5%,respectively.
引文
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