Effects of uncertainty in the reaction of the hydroxyl radical with nitrogen dioxide on model-simulated ozone control strategies |
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| Institution: | 1. Department of Physics, Università degli Studi di Milano and INFN Milan, Italy;2. Department of Chemistry, Università degli Studi di Milano, Milano, Italy;1. Research Center for Environmental Changes, Academia Sinica, Taipei 11529, Taiwan;2. Earth System Science Program, Taiwan International Graduate Program, Academia Sinica, Taiwan;3. College of Earth Science, National Central University, Taoyuan, Taiwan;1. Institute of Low Temperature Science, Hokkaido University, N19, W8, Kita-Ku, Sapporo 060-0819, Japan;2. Chubu Institute for Advanced Studies, Chubu University, 1200 Motsumoto-cho, Kasugai 487-8501, Japan;3. Research Institute for Global Change, Japan Agency for Marine-Earth Science and Technology, Yokohama, Japan;4. LAPC, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing, China;1. Lublin University of Technology, 38D, Nadbystrzycka Str., 20-618, Lublin, Poland;2. Sumy State University, 2, Rymskyi-Korsakov Str., 40007, Sumy, Ukraine |
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| Abstract: | We evaluated the effect of a 20% reduction in the rate constant of the reaction of the hydroxyl radical with nitrogen dioxide to produce nitric acid (OH+NO2→HNO3) on model predictions of ozone mixing ratios (O3]) and the effectiveness of reductions in emissions of volatile organic compounds (VOC) and nitrogen oxides (NOx) for reducing O3]. By comparing a model simulation with the new rate constant to a base case scenario, we found that the O3] increase was between 2 and 6% for typical rural conditions and between 6 and 16% for typical urban conditions. The increases in O3] were less than proportional to the reduction in the OH+NO2 rate constant because of negative feedbacks in the photochemical mechanism. Next, we used two different approaches to evaluate how the new OH+NO2 rate constant changed the effectiveness of reductions in emissions of VOC and NOx: first, we evaluated the effect on O3] sensitivity to small changes in emissions of VOC (dO3]/dEVOC) and NOx (dO3]/dENOx); and secondly, we used the empirical kinetic modeling approach to evaluate the effect on the level of emissions reduction necessary to reduce O3] to a specified level. Both methods showed that reducing the OH+NO2 rate constant caused control strategies for VOC to become less effective relative to NOx control strategies. We found, however, that dO3]/dEVOC and dO3]/dENOx did not quantitatively predict the magnitude of the change in the control strategy because the O3] response was nonlinear with respect to the size of the emissions reduction. We conclude that model sensitivity analyses calculated using small emissions changes do not accurately characterize the effect of uncertainty in model inputs (in this case, the OH+NO2 rate constant) on O3 attainment strategies. Instead, the effects of changes in model inputs should be studied using large changes in precursor emissions to approximate realistic attainment scenarios. |
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