Diagnostic modeling of PAMS VOC observation

Sheng Po Chen, Tsun Hsien Liu, Tu Fu Chen, Chang Feng Ou Yang, Jia Lin Wang, Julius S. Chang

Research output: Contribution to journalArticlepeer-review

22 Scopus citations

Abstract

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 observation 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 other countries as well. A protocol, using PAMS-AQM for testing consistency between detailed VOC emissions and PAMS observations, has been developed and demonstrated.

Original languageEnglish
Pages (from-to)4635-4644
Number of pages10
JournalEnvironmental Science and Technology
Volume44
Issue number12
DOIs
StatePublished - 15 Jun 2010

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