Assessment of transboundary ozone contribution toward South Korea using multiple source–receptor modeling techniques

Abstract

Ozone concentrations in East Asia were simulated using the Community Multi-scale Air Quality (CMAQ) model, and its source contributions were estimated by multiple source–receptor modeling techniques. To study relationships between ozone concentrations and precursor emission sources, three approaches were applied to four months (January, April, July, and October 2009) to represent seasonal characteristics and compare results, with a particular focus on South Korea. Brute force (BF) is a traditional sensitivity analysis method used to estimate model output response to an input change. The high-order decoupled direct method (HDDM), a computational method, is an efficient and accurate alternative to the BF method for sensitivity. The Ozone and Particulate Precursor Tagging Methodology (OPTM) provides contribution information quantified by tracking emissions from selected sources throughout the simulation period. The approaches generally show that most of the receptor regions were substantially influenced by emissions from central China, which is the largest anthropogenic emissions source region in East Asia. Local emissions were still major contributors, especially South Korea and Japan during July 2009. On the other hand, a case study of maximum 8-h ozone concentrations derived from CMAQ–OPTM on April 9 in South Korea shows that the NOx and VOCs emissions from China contributed approximately 82% and 91%, respectively, to maximum 8-h ozone in Region 4 (South Korea) without boundary inflow, which indicates that Chinese emissions are the dominant contributor in this episode. A comparison study of the three approaches shows that HDDM tends to estimate biogenic source contributions lower than that from OPTM in China but similar to OPTM in South Korea and Japan. When comparing the BF method and HDDM, the sensitivity results show a reasonably good agreement during a given period. The location- and time-dependent maximum 8-h ozone isopleths over South Korea as a receptor region created by HDDM suggest that most ozone was being transported from central China, whereas almost no ozone was formed locally during April 2009, and local conditions were heavily VOC limited. On the other hand, local emissions were the dominant contributor during July 2009, and every source region showed a NOx-limited regime, which indicates that ozone concentrations in South Korea strongly depend on NOx emissions during this month.