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Diagnostic Modeling of PAMS VOC Observation

机译：PAMS VOC观察的诊断建模

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Although a number of gas-phase chemical mechanisms, such as CBM-IV, RADM2, and SAPRC have been successful in studying gas-phase atmospheric chemical processes, they all used different combinations of lumped organic species to describe the role of organics in gas-phase chemical processes. Photochemical Assessment Monitoring Stations (PAMS) have been in use for over a decade and yet it is not clear how the detailed organic species measured by PAMS compare to the lumped modeled species. By developing a detailed mechanism specifically for the PAMS organics and embedding this diagnostic model within a regional-scale transport and chemistry model, one can then directly compare PAMS observation with regional-scale model simulations. By means of this comparison one can perhaps better evaluate model performance. The Taiwan Air Quality Model (TAQM)was modified by adding a submodel with transport processes and chemical mechanism for interactions of the 56 species observed by PAMS. It is assumed that TAQM can simulate the overall regional-scale environment including time evolution of oxidants and radicals; these results are then used to simulate the evolution of PAMS organics with species-specific source functions, meteorological transport, and chemical interactions. Model simulations of each PAMS organic were compared with PAMS hourly surface measurements. A case study with data collected at three sites in central Taiwan showed that when meteorological simulations were comparable with observations, diurnal patterns of most organics performed well with PAMS data after emissions were corrected. It is found emissions of over half of the PAMS species require correction, some by surprisingly large factors. With such correlation, simulated time evolution of ratios of ethylbenzene/m,p-xylenes and ethane/ n-butane showed similar behaviors as shown by obseivation data. From the results of PAMS organics diurnal variations as well as indicator ratios, one can conclude that PAMS Air Quality Model (PAMS-AQM) has been successfully developed and can be applied to the study of evolution of PAMS organics in regional and urban environments. Further, one finds that an existing VOC emissions estimation procedure heavily dependent on U.S.-data based emissions speciation factors is suspect in application in Taiwan and perhaps in otherrncountries as well. A protocol, using PAMS-AQM for testing consistency between detailed VOC emissions and PAMS observations, has been developed and demonstrated.
机译：尽管许多气相化学机理（例如CBM-IV，RADM2和SAPRC）已成功地研究了气相大气化学过程，但他们都使用了不同的集总有机物组合来描述有机物在气相中的作用。相化学过程。光化学评估监测站（PAMS）已经使用了十多年，但尚不清楚通过PAMS测量的详细有机物与集总模型物的比较。通过开发一种专门针对PAMS有机物的详细机制并将此诊断模型嵌入区域规模的运输和化学模型中，可以将PAMS观测结果与区域规模的模型模拟直接进行比较。通过这种比较，也许可以更好地评估模型性能。通过添加具有运输过程和化学机制的子模型来修改台湾空气质量模型（TAQM），以通过PAMS观察到56种物种之间的相互作用。假定TAQM可以模拟整个区域规模的环境，包括氧化剂和自由基的时间演化。然后将这些结果用于模拟具有特定物种来源功能，气象传输和化学相互作用的PAMS有机物的演化。将每种PAMS有机物的模型模拟与PAMS每小时表面测量值进行了比较。一项对台湾中部三个地点收集的数据进行的案例研究表明，当气象模拟与观察结果相当时，在校正排放后，PAMS数据能使大多数有机物的昼夜模式表现良好。发现超过一半的PAMS物质的排放需要校正，其中一些因素出乎意料的大。通过这种相关性，乙苯/ m，对二甲苯和乙烷/正丁烷之比的模拟时间演化显示出相似的行为，如增磁数据所示。从PAMS有机物的日变化以及指标比率的结果可以得出结论，PAMS空气质量模型（PAMS-AQM）已成功开发，可用于研究区域和城市环境中PAMS有机物的演变。此外，人们发现在台湾甚至在其他国家也可能采用现有的VOC排放估算程序，该程序严重依赖基于美国数据的排放形成因子。已经开发并演示了使用PAMS-AQM来测试详细VOC排放量与PAMS观测值之间一致性的协议。

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  • 来源
    《Environmental Science & Technology》 |2010年第12期|P.4635-4644|共10页
  • 作者

    SHENG-PO CHEN; rnTSUN-HSIEN LIU; rnTU-FU CHEN; rnCHANG-FENG OU YANG; rnJIA-LIN WANG; rnJULIUS S. CHANG;

  • 作者单位

    Institute of Atmospheric Physics, National Central University, Taiwan;

    rnInstitute of Atmospheric Physics, National Central University, Taiwan;

    rnInstitute of Atmospheric Physics, National Central University, Taiwan;

    rnDepartment of Chemistry, National Central University, Taiwan;

    rnDepartment of Chemistry, National Central University, Taiwan;

    rnInstitute of Atmospheric Physics, National Central University, Taiwan;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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