基于观测与模型模拟的济南市大气羰基化合物污染特征及生成机制

Observational and modeling insights into pollution characteristics and formation mechanisms of atmospheric carbonyl compounds in Jinan City

  • 摘要: 为探究济南市夏季羰基化合物的污染特征及生成机制,于2022年6月在典型居民区开展大气观测,结合基于观测的模型(OBM)解析其来源与光化学反应路径。结果表明,羰基化合物平均浓度为(12.08±4.26)×10−9,甲醛〔(5.33±2.23)×10−9〕、乙醛〔(4.08±1.00)×10−9〕和丙酮〔(1.59±0.51)×10−9〕占主导,占比分别为44.12%、33.77%和13.16%。羰基化合物日变化呈现早间(机动车排放)、午后(光化学反应)及夜间(柴油车与烧烤排放)三峰模式,受人为活动与气象条件共同驱动。模型模拟显示,甲醛净生成速率为0.23×10−9~0.94×10−9 h−1,烷烃和烯烃对其生成贡献显著(相对增量反应活性最高达3.3),乙醛则因剧烈光化学反应呈现净消耗特征。敏感性实验表明,控制烷烃和烯烃排放可有效降低甲醛和乙醛浓度。

     

    Abstract: To investigate the pollution characteristics and formation mechanisms of carbonyl compounds in Jinan City during summer, this study conducted atmospheric observations in a typical residential area in June 2022, combined with an observation-based model (OBM) to analyze their sources and photochemical pathways. Results showed that the average concentration of carbonyl compounds was (12.08±4.26)×10−9, dominated by formaldehyde (5.33±2.23)×10−9, acetaldehyde (4.08±1.00) ×10−9, and acetone (1.59±0.51)×10−9, accounting for 44.12%, 33.77%, and 13.16%, respectively. Diurnal variations exhibited a tri-modal pattern: morning peaks (vehicle emissions), afternoon peaks (photochemical processes), and nighttime peaks (diesel vehicle and barbecue emissions), driven by anthropogenic activities and meteorological conditions. Model simulations revealed a net formaldehyde formation rate of 0.23×10−9-0.94×10−9 h−1, with significant contributions from alkanes and alkenes (highest Relative Incremental Reactivity, RIR=3.3), while acetaldehyde showed net consumption due to intense photochemical reactions. Sensitivity experiments demonstrated that controlling alkane and alkene emissions could effectively reduce formaldehyde and acetaldehyde concentrations.

     

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