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Nitryl chloride (ClNO2) has been reported as a critical species of chlorine chemistry. Its chemistry interrupts a nighttime sink of NOX and emits chlorine radical (Cl•) in the daytime, consequently altering gaseous and aerosol chemistry. Recent field studies have also measured considerable concentrations of ClNO2 in South Korea under the influences of natural and anthropogenic chlorine sources. However, the impacts of ClNO2 chemistry on air quality in South Korea have yet to be evaluated. We validate simulated ClNO2 and its chemistry in South Korea using observations and a 3-D chemical transport model (CTM) during the Korea-United States Air Quality field study. We implemented the latest Chinese and Korean anthropogenic chlorine emissions in the model. We found that the model reproduces the observed spatial and temporal variations of ClNO2, including its local and transboundary transport and precursors. We found that ClNO2 chemistry results in a more efficient conversion of NO to NO2 at night and daytime acceleration of the NOX-O3 cycle. It results in an increase of O3 (1.1%), NOX (3.1%), OH (2.0%), HO2 (0.8%), and Cl• (507.8%) and a decrease of TNO3(HNO3 + aerosol nitrate, 1.7%) on the campaign mean basis.

Despite the effort to control SO

High concentrations of PM2.5 have become a serious environmental issue in South Korea, which ranked 1st or 2nd among OECD countries in terms of population exposure to PM2.5. Quantitative understanding of PM2.5 source attribution is thus crucial for developing efficient air quality mitigation strategies. Here we use a suite of extensive observations of PM2.5 and its precursors concentrations during the international KORea-US cooperative Air Quality field study in Korea (KORUS-AQ) in May–June 2016 to investigate source contributions to PM2.5 in South Korea under various meteorological conditions. For the quantitative analysis, we updated a 3-D chemical transport model, GEOS-Chem, and its adjoint with the latest regional emission inventory and other recent findings. The updated model is evaluated by comparing against observed daily PM2.5 and its component concentrations from six ground sites (Bangnyung, Bulkwang, Olympic park, Gwangju, Ulsan, and Jeju). Overall, simulated concentrations of daily PM2.5 and its components are in a good agreement with observations over the peninsula. We conduct an adjoint sensitivity analysis for simulated surface level PM2.5 concentrations at five ground sites (except for Bangnyung because of its small population) under four different meteorological conditions: dynamic weather, stagnant, extreme pollution, and blocking periods. Source contributions by regions vary greatly depending on synoptic meteorological conditions. Chinese contribution accounts for almost 68% of PM2.5 in surface air in South Korea during the extreme pollution period of the campaign, whereas an enhanced contribution from domestic sources (57%) occurs for the blocking period. Results from our sensitivity analysis suggest that the reduction of domestic anthropogenic NH3 emissions could be most effective in reducing population exposure to PM2.5 in South Korea (effectiveness = 14%) followed by anthropogenic SO2 emissions from Shandong region (effectiveness = 11%), domestic anthropogenic NOx emissions (effectiveness = 10%), anthropogenic NH3 emissions from Shandong region (effectiveness = 8%), anthropogenic NOx emissions from Shandong region (effectiveness = 7%), domestic anthropogenic OC emissions (effectiveness = 7%), and domestic anthropogenic BC emissions (effectiveness = 5%).

Photolysis of nitrous acid (HONO) is recognized as an early-morning source of OH radicals in the urban air. During the Korea–US air quality (KORUS-AQ) campaign, HONO was measured using quantum cascade - tunable infrared laser differential absorption spectrometer (QC-TILDAS) at Olympic Park in Seoul from 17 May, 2016 to 14 June, 2016. The HONO concentration was in the range of 0.07–3.46 ppbv, with an average of 0.93 ppbv. Moreover, it remained high from 00:00–05:00 LST. During this time, the mean concentration was higher during the high-O(3) episodes (1.82 ppbv) than the non-episodes (1.20 ppbv). In the morning, the OH radicals that were produced from HONO photolysis were 50% higher (0.95 pptv) during the high-O(3) episodes than the non-episodes. Diurnal variations in HO(x) and O(3) concentrations were simulated by the F0AM model, which revealed a difference of ~20 ppbv in the daily maximum O(3) concentrations between the high-O(3) episodes and non-episodes. Furthermore, the HONO concentration increased with an increase in relative humidity (RH) up to 80%; the highest HONO was associated with the top 10% NO(2) in each RH group, confirming that NO(2) is one of the main precursors of HONO. At night, the conversion ratio of NO(2) to HONO was estimated to be 0.88×10(−2) h(−1); this ratio was found to increase with an increase in RH. The Aitken mode particles (30–120 nm), which act as catalyst surfaces, exhibited a similar tendency with a conversion ratio that increased along with RH, indicating the coupling of surfaces with HONO conversion. Using an artificial neural network (ANN) model, HONO concentrations were successfully simulated with measured variables (r(2) = 0.66 as an average of five models). Among these variables, NO(x), aerosol surface area, and RH were found to be the main factors affecting the ambient HONO concentrations. The results reveal that RH facilitates the conversion of NO(2) to HONO by constraining the availability of aerosol surfaces. This study demonstrates the coupling of HONO with the HO(x)-O(3) cycle in the Seoul Metropolitan Area (SMA) and provides practical evidence of the heterogeneous formation of HONO by employing the ANN model.

Despite its profound influence on air quality, the aerosol acidity, quantifiable by aerosol pH is poorly characterized in South Korea where high concentrations of fine particles have become a serious environmental issue. In this study, we estimated the pH values of PM2.5 using observations of inorganic species and precursor gases concentrations, ambient temperature and relative humidity (RH), measured at the Olympic Park in Seoul during the KORUS-AQ campaign (10 May to June 19, 2016). For the aerosol pH calculation, the ISORROPIA and E-AIM thermodynamic equilibrium models in forward mode were used, in which we found the phase state assumption, either stable (solid + liquid) or metastable (liquid only) had no significant impact on pH predictions. As reported previously, the unrealistic pH prediction of ∼7.6 by ISORROPIA, which largely misrepresents ammonia-rich aerosol contents in the Seoul atmosphere was mainly due to coding errors in the standard ISORROPIA model (i.e., forward mode with stable state assumption). Using the revised ISORROPIA, pH predictions obtained with stable assumption approached those obtained with the metastable state assumption. Following such amendment, fine particle samples were predicted to be acidic with pH values ranging from 1.5 to 4.0 as determined by both ISORROPIA and E-AIM calculations. These pH values were higher than those reported in the United States and Europe and lower than those reported in northern China. A comparison of ISORROPIA and E-AIM models revealed that the pH values obtained using ISORROPIA were consistently but only ∼0.4 pH unit higher than those obtained using E-AIM, demonstrating the precision and consistent utility of thermodynamic equilibrium model in the quantification of PM2.5 pH in Seoul.

Nitryl chloride (ClNO2) plays an important role as a night-time reservoir of NOX and the source of Cl radical during the daytime, which consequently affects the ozone photochemistry. Its impacts on regional air quality in East Asia, however, are not fully understood so far. We here use extensive observations during the international KORea-US cooperative Air Quality field study in Korea (KORUS-AQ), which occurred in May-June 2016, with a 3-D chemistry transport model to examine the impacts of ClNO2 chemistry on radical species and total nitrate concentrations in East Asia. We first update the model by implementing chlorine chemistry and latest anthropogenic chlorine emissions of China and South Korea. We conduct model simulations for May-June, 2016 and validate the model by comparing against the observations from the KORUS-AQ campaign. We find that the ClNO2 chemistry in the model results in an increase of ozone by ~1.4 ppbv (~2.5%), Cl radical by ~ 4.6x103 molec cm-3 (~3600%), OH ~8.2x104 molec cm-3 (~5.3%), HO2 ~6.6 molec cm-3 (~3.0%), a decrease of TNO3 (HNO3 + nitrate aerosol) concentrations by ~2 μg m-3 on a daily mean basis during the campaign. Overall, the enhanced conversion of NO to NO2 driven by ClNO2 chemistry contributes to higher oxidant concentrations in the model. As a result, the updated model shows a better agreement with the observations in Korea during the KORUS-AQ campaign.

Photolysis of nitrous acid (HONO) has long been recognized as an early morning source of OH radicals in urban air, but the detailed mechanism of its formation is still unclear. During the Korea-US Air Quality (KORUS-AQ) campaign, HONO was measured using Quantum Cascade Tunable Diode Laser Absorption Spectroscopy (QC-TDLAS) at Olympic Park in Seoul from 17 May to 10 June, 2016. HONO concentrations ranged from 0.07 ppbv to 3.46 ppbv with an average of 0.93 ppbv. HONO remained high at night from 1 am to 5 am, during which the mean concentration was higher in high-O3 episodes (1.82 ppbv) than non-episode (1.20 ppbv). In the morning, OH budget due to HONO photolysis were higher by 50 % (0.95 pptv) during high-O3 episodes compared to non-episode. Diurnal variations of HOx and O3 simulated by the F0AM model demonstrated a difference of ~ 20 ppbv in daily maximum O3 between the two periods. The HONO concentration increased with relative humidity (RH) until 80 %, of which the highest HONO was associated with the top 10 % NOx, confirming that NOx is a crucial precursor of HONO and its formation is facilitated by humidity. The conversion ratio of NOx to HONO was estimated to be 0.86 × 10−2 h−1 at night and also increased with RH. As surrogate for the catalyst surface, the mass concentrations of black carbon (eBC) and the surface areas of particles smaller than 120 nm showed a tendency for RH similar to conversion ratio. Using an Artificial Neuron Network (ANN) model, HONO concentrations were successfully simulated with measured variables (r = 0.8 for the best suite), among which NOx, surface area, and RH were found to be main factors affecting ambient HONO concentrations with weigh values of 26.2 %, 11.9 %, and 10.6 %, respectively. This study demonstrates the coupling of HONO with HOx-VOCs-O3 cycle in Seoul Metropolitan Areas (SMA) and provides practical evidence for heterogeneous formation of HONO by employing the ANN model to atmospheric chemistry.

Photolysis of nitrous acid (HONO) is recognized as an early-morning source of OH radicals in the urban air. During the Korea-US air quality (KORUS-AQ) campaign, HONO was measured using quantum cascade - tunable infrared laser differential absorption spectrometer (QC-TILDAS) at Olympic Park in Seoul from 17 May, 2016 to 14 June, 2016. The HONO concentration was in the range of 0.07-3.46 ppbv, with an average of 0.93 ppbv. Moreover, it remained high from 00:00-05:00 LST. During this time, the mean concentration was higher during the high-O3 episodes (1.82 ppbv) than the non-episodes (1.20 ppbv). In the morning, the OH radicals that were produced from HONO photolysis were 50% higher (0.95 pptv) during the high-O3 episodes than the non-episodes. Diurnal variations in HOx and O3 concentrations were simulated by the F0AM model, which revealed a difference of ~20 ppbv in the daily maximum O3 concentrations between the high-O3 episodes and non-episodes. Furthermore, the HONO concentration increased with an increase in relative humidity (RH) up to 80%; the highest HONO was associated with the top 10% NO2 in each RH group, confirming that NO2 is one of the main precursors of HONO. At night, the conversion ratio of NO2 to HONO was estimated to be 0.88×10-2 h-1; this ratio was found to increase with an increase in RH. The Aitken mode particles (30-120 nm), which act as catalyst surfaces, exhibited a similar tendency with a conversion ratio that increased along with RH, indicating the coupling of surfaces with HONO conversion. Using an artificial neural network (ANN) model, HONO concentrations were successfully simulated with measured variables (r2 = 0.66 as an average of five models). Among these variables, NOx, aerosol surface area, and RH were found to be the main factors affecting the ambient HONO concentrations. The results reveal that RH facilitates the conversion of NO2 to HONO by constraining the availability of aerosol surfaces. This study demonstrates the coupling of HONO with the HOx-O3 cycle in the Seoul Metropolitan Area (SMA) and provides practical evidence of the heterogeneous formation of HONO by employing the ANN model.

In this study, we simultaneously measured the PM10 and PM2.5 mass concentrations and their heavy metal content for three days at a subway station in Seoul to investigate the airborne PM flows. The average concentrations were 59 µg m–3, 37 µg m–3, 111 µg m–3, and 369 µg m–3 for the PM10 and 43 µg m–3, 28 µg m–3, 58 µg m–3, and 132 µg m–3 for the PM2.5 at the outdoor air inlet, in the concourse, on the platform, and in the tunnel, respectively. We also found strong correlations between the temporal variations at adjacent sampling locations for both fractions, although they were higher for the PM2.5. Additionally, of the airborne trace metals detected at the sampling locations inside the station (the concourse, platform, and tunnel), iron (Fe) displayed the highest concentration and was thus selected as a tracer of PM. Applying a simple mass balance model to the Fe concentrations and ventilation rates revealed that 78% of the PM10 and 62% of the PM2.5 on the platform emanated from the tunnel, whereas 84% of the PM10 and 87% of the PM2.5 in the concourse originated outdoors (and arrived in the filtered air). These results further confirm that reducing PM emission from the tunnel is the most effective strategy for improving air quality on the platform and achieving compliance with the national guideline.

The present study has determined the detection rate of norovirus (NoV) with acute gastroenteritis (AGE) in hospitalized children and describes the molecular epidemiology of NoV circulating in Seoul, Korea. Six hundred and eighty-three (9.8%) of samples were positive for NoV. Of these, the NoV GII genogroup was the most commonly found, with a prevalence of 96.2% (683 of 710). Only 27 samples were positive for the NoV GI genogroup. Ten kinds of GI genotype (GI/1, GI/2, GI/3, GI/4, GI/5, GI/6, GI/7, GI/9, GI/12, and GI/13) and eight kinds of GII genotype (GII/2, GII/3, GII/4, GII/8, GII/14, GII/15, GII/16, and GII/17) were identified in children with AGE during the years 2008-2011.

The present study has determined the detection rate of norovirus (NoV) with acute gastroenteritis (AGE) in hospitalized children and describes the molecular epidemiology of NoV circulating in Seoul, Korea. Six hundred and eighty-three (9.8%) of samples were positive for NoV. Of these, the NoV GII genogroup was the most commonly found, with a prevalence of 96.2% (683 of 710). Only 27 samples were positive for the NoV GI genogroup. Ten kinds of GI genotype (GI/1, GI/2, GI/3, GI/4, GI/5, GI/6, GI/7, GI/9, GI/12, and GI/13) and eight kinds of GII genotype (GII/2, GII/3, GII/4, GII/8, GII/14, GII/15, GII/16, and GII/17) were identified in children with AGE during the years 2008-2011.