PM 2:5 source attribution for Seoul in May from 2009 to 2013 using GEOS-Chem and its adjoint model * Hyung-Min Lee a, * , Rokjin J. Park b , Daven K. Henze c , Seungun Lee b , Changsub Shim d , Hye-Jung Shin e , Kwang-Joo Moon e , Jung-Hun Woo f a Department of Civil, Environmental, and Architectural Engineering, University of Colorado, Boulder, CO, USA b School of Earth and Environmental Sciences, Seoul National University, Seoul, Republic of Korea c Department of Mechanical Engineering, University of Colorado, Boulder, CO, USA d Korea Environment Institute, 370 Sicheong-daro, Sejong, Republic of Korea e National Institute of Environmental Research, Incheon, Republic of Korea f Department of New Technology and Fusion, Konkuk University, Seoul, Republic of Korea article info Article history: Received 16 July 2016 Received in revised form 23 November 2016 Accepted 30 November 2016 Available online 5 December 2016 Keywords: PM2.5 Seoul metropolitan area Adjoint modeling Source attribution Sensitivity analysis Atmospheric chemical transport model abstract Enforcement of an air quality standard for PM 2:5 in the Seoul metropolitan area (SMA) was enacted in 2015. From May to June of 2016, an international airborne and surface measurement campaign took place to investigate air pollution mechanisms in the SMA. The total and speciated PM 2:5 concentrations since 2008 have been measured at an intensive monitoring site for the SMA operated by the National Institute of Environmental Research (NIER). To gain insight on the trends and sources of PM 2:5 in the SMA in May, we analyze PM 2:5 concentrations from 2009 to 2013 using the measurements and simulations from a 3- dimensional global chemical transport model, GEOS-Chem and its adjoint. The model is updated here with the latest regional emission inventory and diurnally varying NH 3 emissions. Monthly average PM 2:5 concentration measured by b-ray attenuation ranges from 28 (2010) to 45 (2013) mg/m 3 , decreased from 2009 to 2010, and then continuously increased until 2013. The model shows good agreement with the measurements for the daily average PM 2:5 concentrations (R 0.5), and reproduces 10 out of 17 measured episodes exceeding the daily air quality standard (50 mg/m 3 ). Using the GEOS-Chem adjoint model, we nd that anthropogenic emissions from the Shandong region have the largest modeled in- uence on PM 2:5 in Seoul in May. Average contributions to the high PM 2:5 episodes simulated by the model are 39% from the Shandong region, 16% from the Shanghai region,14% from the Beijing region, and 15% from South Korea. Anthropogenic SO 2 emissions from South Korea are negligible with 90% of the total contribution originating from China. Findings from this study may guide interpretation of obser- vations obtained in the KORUS-AQ measurement campaign. © 2016 Elsevier Ltd. All rights reserved. 1. Introduction Particulate matter with aerodynamic diameter less than 2.5 mm (PM 2:5 ) is known to have detrimental impacts on human health, causing increased respiratory disease and stroke related mortalities (e.g., Burnett et al., 2000; Franklin et al., 2006; Bell et al., 2007). The Seoul metropolitan area (Seoul, Incheon, and Geonggi) is one of the most densely populated mega-cities worldwide, having more than 23 million residents (49% of national population) in about 12,000 km 2 (12% of the Korean peninsula) (KOSIS, 2010). Air quality standards for PM 2:5 , however, have recently been implemented in Seoul since 2015. The Korean Ministry of Environment devised a Special Act legislation for improving air quality in the Seoul metropolitan area in 2003 (enacted in 2005). The rst Seoul Metropolitan Air Quality Improvement Plan (2005e2014) aimed at reducing PM 10 and NO 2 concentrations. In the second master plan, formulated for 2015e2024, PM 2:5 and O 3 were added to the regu- lations. This plan includes PM 2:5 standards of 50 mg/m 3 for 24 h, and 25 mg/m 3 for a year. The goal of the second master plan is reducing annual PM 2:5 from 27 mg/m 3 in 2010 to 20 mg/m 3 in the Seoul metropolitan area by 2024 (ME, 2013). In order to help monitor and enforce these air quality * This paper has been recommended for acceptance by Dr. Hageman Kimberly Jill. * Corresponding author. E-mail address: hyungmin.lee@colorado.edu (H.-M. Lee). Contents lists available at ScienceDirect Environmental Pollution journal homepage: www.elsevier.com/locate/envpol http://dx.doi.org/10.1016/j.envpol.2016.11.088 0269-7491/© 2016 Elsevier Ltd. All rights reserved. Environmental Pollution 221 (2017) 377e384