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Photochemical oxidation and dispersion of gaseous sulfur compounds from natural and anthropogenic sources around a coastal location
Authors:Sang-Keun Song  Zang-Ho Shon  Ki-Hyun Kim
Institution:1. Division of Earth Environmental System, Pusan National University, 30 Jang Jeon Dong, Geum Jeong Gu, Busan 609-735, Republic of Korea;2. Department of Environmental Engineering, Dong-Eui University, 995 Eom Gwang No, Busan Jin Gu, Busan 614-714, Republic of Korea;3. Department of Earth & Environmental Sciences, Sejong University, 98 Goon Ja Dong, Gwang Jin Gu, Seoul 143-747, Republic of Korea;1. State Key Laboratory of Fine Chemicals, PSU-DUT Joint Center for Energy Research, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, P. R. China;2. EMS Energy Institute, PSU-DUT Joint Center for Energy Research and Department of Energy & Mineral Engineering, Pennsylvania State University, University Park, Pennsylvania 16802, United States;1. Key Laboratory of Condition Monitoring and Control for Power Plant Equipment, Ministry of Education, North China Electric Power University, Beijing 102206, PR China;2. Institute of Combustion Science and Environmental Technology, Western Kentucky University, Bowling Green, KY 42101, USA;1. Air Conditioning and Refrigeration Center, Department of Mechanical Science and Engineering, University of Illinois at Urbana-Champaign, 1206 West Green Street, Urbana, IL 61801, USA;2. Creative Thermal Solutions, 2209 North Willow Road, Urbana, IL 61802, USA
Abstract:The photochemical oxidation and dispersion of reduced sulfur compounds (RSCs: H2S, CH3SH, DMS, CS2, and DMDS) emitted from anthropogenic (A) and natural (N) sources were evaluated based on a numerical modeling approach. The anthropogenic emission concentrations of RSCs were measured from several sampling sites at the Donghae landfill (D-LF) (i.e., source type A) in South Korea during a series of field campaigns (May through December 2004). The emissions of natural RSCs in a coastal study area near the D-LF (i.e., source type N) were estimated from sea surface DMS concentrations and transfer velocity during the same study period. These emission data were then used as input to the CALPUFF dispersion model, revised with 34 chemical reactions for RSCs. A significant fraction of sulfur dioxide (SO2) was produced photochemically during the summer (about 34% of total SO2 concentrations) followed by fall (21%), spring (15%), and winter (5%). Photochemical production of SO2 was dominated by H2S (about 55% of total contributions) and DMS (24%). The largest impact of RSCs from source type A on SO2 concentrations occurred around the D-LF during summer. The total SO2 concentrations produced from source type N around the D-LF during the summer (a mean SO2 concentration of 7.4 ppbv) were significantly higher than those (≤0.3 ppbv) during the other seasons. This may be because of the high RSC and SO2 emissions and their photochemistry along with the wind convergence.
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