Seasonal dependence of the oxidation capacity of the city of Santiago de Chile |
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| Authors: | YF Elshorbany J Kleffmann R Kurtenbach E Lissi M Rubio G Villena E Gramsch AR Rickard MJ Pilling P Wiesen |
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| Institution: | 1. CNR - Institute of Atmospheric Pollution Research, Via Salaria Km 29.3, CP10, 00015 Monterotondo S., Rome, Italy;2. Research Consortium CORAM, Via Cristoforo Colombo 37/E, 441000 Ferrara, Italy;3. State Key Joint Laboratory for Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, No.5 Yiheyuan Road Haidian District, 100871, Beijing, China;1. Emissions, Measurements and Modeling of the Atmosphere Laboratory, EGFEM Unit, Center for Analysis and Research, Faculty of Sciences, Saint Joseph University, Beirut, Lebanon;2. Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA), UMR7583, CNRS, Université Paris-Est-Créteil (UPEC) et Université Paris Diderot (UPD), Institut Pierre Simon Laplace (IPSL), Créteil, France;3. Institut de Combustion, Aérothermique, Réactivité et Environnement, CNRS, Orléans, France;1. State Key Laboratory for Structural Chemistry of Unstable and Stable Species, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, PR China;2. University of Chinese Academy of Sciences, Beijing 100049, PR China;3. Center for Excellence in Regional Atmospheric Environment, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, PR China;4. State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry (LAPC), Institute of Atmospheric Physics (IAP), Chinese Academy of Sciences, Beijing 100029, PR China;5. School of Geography Earth and Environmental Sciences, University of Birmingham, Birmingham B15 2TT, United Kingdom;6. Beijing Urban Ecosystem Research Station, State Key Laboratory of Urban and Regional Ecology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, PR China;7. State Key Joint Laboratory of Environment Simulation and Pollution Control, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, PR China;1. State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Beijing National Laboratory for Molecular Sciences (BNLMS), CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China;2. School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing 100049, China;3. Center for Excellence in Regional Atmospheric Environment, Institute of Urban Environment, Chinese Academy of Science, Xiamen 361021, China;1. State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing, China;2. Institute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Juelich GmbH, Juelich, Germany;3. International Joint laboratory for Regional pollution Control (IJRC), Peking University, Beijing, China;4. Beijing Innovation Center for Engineering Sciences and Advanced Technology, Peking University, Beijing, China;5. CAS Center for Excellence in Regional Atmospheric Environment, Chinese Academy of Science, Xiamen, China |
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| Abstract: | The oxidation capacity of the highly polluted urban area of Santiago de Chile has been evaluated during a winter measurement campaign from May 25 to June 07, 2005, with the results compared and contrasted with those previously evaluated during a summer campaign from March 8 to 20, 2005. The OH radical budget was evaluated in both campaigns employing a simple quasi-photostationary state model (PSS) constrained with simultaneous measurements of HONO, HCHO, O3, NO, NO2, j(O1D), j(NO2), 13 alkenes and meteorological parameters. In addition, a zero dimensional photochemical box model based on the Master Chemical Mechanism (MCMv3.1) has been used for the analysis of the radical budgets and concentrations of OH, HO2 and RO2. Besides the above parameters, the MCM model has been constrained by the measured CO and other volatile organic compounds (VOCs) including alkanes and aromatics. Total production and destruction rates of OH and HO2 in winter are about two times lower than that during summer. Simulated OH levels by both PSS and MCM models are similar during the daytime for both winter and summer indicating that the primary OH sources and sinks included in the simple PSS model are predominant. On a 24 h basis, HONO photolysis was shown to be the most important primary OH radical source comprising 81% and 52% of the OH initiation rate during winter and summer, respectively followed by alkene ozonolysis (12.5% and 29%), photolysis of HCHO (6.1% and 15%), and photolysis of O3 (<1% and 4%), respectively. During both winter and summer, there was a balance between the OH secondary production (HO2 + NO) and destruction (OH + VOCs) showing that initiation sources of RO2 and HO2 are no net OH initiation sources. This result was found to be fulfilled also for all other studies investigated. Seasonal impacts on the radical budgets are also discussed. |
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