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青岛大气中酸碱气体及PM2.5中水溶性离子的浓度特征和气粒平衡关系
摘要点击 2634  全文点击 1453  投稿时间:2015-02-01  修订日期:2015-04-02
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中文关键词  酸性气体  氨气  水溶性无机离子  PM2.5  气粒平衡  ISORROPIA Ⅱ模型
英文关键词  acidic gases  ammonia  water-soluble inorganic ions  PM2.5  gas-particle equilibrium  ISORROPIA Ⅱ model
作者单位E-mail
周佳佳 中国海洋大学环境科学与工程学院, 青岛 266100 zjj910123@163.com 
石金辉 中国海洋大学环境科学与工程学院, 青岛 266100
中国海洋大学海洋环境与生态教育部重点实验室, 青岛 266100 
engroup@ouc.edu.cn 
李丽平 中国海洋大学环境科学与工程学院, 青岛 266100  
姚小红 中国海洋大学环境科学与工程学院, 青岛 266100
中国海洋大学海洋环境与生态教育部重点实验室, 青岛 266100 
 
高会旺 中国海洋大学环境科学与工程学院, 青岛 266100
中国海洋大学海洋环境与生态教育部重点实验室, 青岛 266100 
 
中文摘要
      2012年11~12月在青岛采集58套denuder和PM2.5样品,分析了其中酸碱气体及相应的颗粒态组分浓度,探讨了它们的浓度特征和气粒平衡关系. 青岛大气中HNO3、HNO2、HCl、SO2和NH3平均浓度分别为1.36、1.64、1.46、27.58和2.95 μg ·m-3. PM2.5中NO3-、NO2-、Cl-、SO42-和NH4+浓度分别为6.49、0.12、1.95、9.36和6.04 μg ·m-3. 霾天大气中酸碱气体浓度较之晴天时的增幅明显低于PM2.5中相应离子浓度的增幅; 雾天时,除HNO2外其他气体浓度均低于晴天,但PM2.5中相应离子浓度较之晴天时均有明显增加. 采样期间青岛大气为富氨环境,PM2.5中NH4+主要以(NH4)2SO4的形式存在,NO3-生成主要受HNO3的限制. 利用ISORROPIA Ⅱ模型探讨了青岛PM2.5中二次离子的控制因子,通过敏感性实验发现NH4+对总NH3(TNH3)变化响应不敏感,但对总H2SO4(TSO4)和总HNO3(TNO3)变化响应敏感; NO3-和SO42-则分别仅对TNO3和TSO4变化响应敏感,这暗示了减少TNO3和TSO4而不是TNH3的排放对降低青岛大气中PM2.5浓度更有效.
英文摘要
      Fifty-eight samples were collected in Qingdao from November to December 2012 using a PM2.5 sampler. Concentrations of acidic gases, ammonia and their partner ions in PM2.5were determined, and the correlation between concentrations and the gas-particle partitioning were analyzed. The averaged concentrations of HNO3, HNO2, HCl, SO2 and NH3 in atmosphere samples of Qingdao were 1.36, 1.64, 1.46, 27.58 and 2.95 μg ·m-3, respectively, for the concentrations of NO3-, NO2-, Cl-, SO42- and NH4+ in PM2.5 were 6.49, 0.12, 1.95, 9.36 and 6.04 μg ·m-3, respectively. When the measurements made in haze days, compared to those made in clear days, the concentration of these ions in PM2.5increased more than those of acidic gases and ammonia; In foggy days, the concentrations of gases were lower than those in clear days except HNO2, while the reverse was true for the concentrations of all particulate species in PM2.5. During whole study period, the NH3 level was high and the NH4+ in PM2.5 in Qingdao was mainly present as (NH4)2SO4. The analysis results suggested that formation of NO3- were mainly determined by HNO3. To further explore the control factors of these species in PM2.5, the thermodynamic equilibrium model of ISORROPIA Ⅱ was employed. Our sensitivity tests showed that the formation of NH4+ was less sensitive to the change of total NH3 (TNH3), but sensitive to the changes of total H2SO4 (TSO4) and total HNO3 (TNO3). The formation of NO3- and SO42- was sensitive to the changes of TNO3 and TSO4, respectively. Taken together, our findings implied that the reduction of TNO3 and TSO4 rather than TNH3 appears to be more effective in lowering mass concentrations of PM2.5 in Qingdao.

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