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Abstract The Observation-Constrained Atmospheric BOX model (OCABOX) was used to analyze the formation of secondary inorganic PM species in the Seoul Metropolitan Area (SMA), South Korea. The measurement data of the ionic components of PM2.5 and their gaseous precursors made at the Olympic Park ground site (37.53°N, 127.12°E) during the Korea-United States Air Quality field campaign were used to run OCABOX in observation-based mode and compare the simulation results. The use of the HNO3 concentrations measured at a marine background site as the boundary conditions appeared to increase the accuracy of the model prediction of HNO3 and particulate NO3− concentrations. For the primary precursors emitted considerably throughout the SMA, such as NOx and NH3, using the data measured inside the SMA as the boundary conditions could lead to more accurate predictions. OCABOX was shown to be a reliable tool to analyze the formation of secondary inorganic aerosol in the SMA if used with appropriate regional background concentrations and observation-based constraints

Nitrous acid (HONO) is a main precursor of hydroxyl radicals (OH), which contribute to the formation of numerous secondary air pollutants in the troposphere. Despite its importance in atmospheric chemistry, HONO chemistry has not been fully incorporated into many chemical transport models (CTMs). Due to the lack of atmospheric HONO processes, CTM simulations often tend to underestimate atmospheric mixing ratios of HONO. This study was undertaken because simulations with current Community Multiscale Air Quality (CMAQ) model have a strong tendency to underestimate the HONO mixing ratio. In search of missing sources of atmospheric HONO, we attempted to sequentially incorporate the following potential HONO sources and processes into the CMAQ modeling framework: (i) gas-phase HONO reactions; (ii) traffic HONO emissions; (iii) soil HONO emissions; (iv) heterogeneous HONO production on the surfaces of aerosols; (v) heterogeneous HONO formation on tree leaf and building surfaces; (vi) photolysis reactions of particulates and deposited HNO3/nitrates called 'renoxification'. The simulation performances of the modified CMAQ models were then evaluated by comparing the modeled HONO mixing ratios with the HONO mixing ratios observed at the Olympic Park station in Seoul, South Korea. When HONO processes were fully added to the CMAQ model, average daily HONO mixing ratios increased from 0.06 ppb to 1.18 ppb. The daytime HONO mixing ratios produced from the CMAQ model run with a full account of atmospheric HONO processes were found to be in better agreement with observations than those from the original CMAQ model (CMAQv5.2.1) runs with improved statistical metrics (e.g., IOA increased from 0.59 to 0.68, while MB decreased dramatically from -0.57 ppb to -0.34 ppb). In addition, we investigated the contributions of individual atmospheric HONO processes to HONO mixing ratios, as well as the impacts of HONO atmospheric processes on the concentrations of other atmospheric species in South Korea. All these issues are also discussed in this manuscript. [ABSTRACT FROM AUTHOR]

In this study, the WRF-Chem v4.4 model was utilized to evaluate three bottom-up emission inventories (EDGAR-HTAP v2, v3, and KORUS v5) using surface and aircraft data in East Asia during the Korea-United States Air Quality (KORUS-AQ) campaign period in 2016. All emission inventories were found to reproduce the diurnal variations of O3 and NO2 as compared to the surface monitor data. However, the spatial distributions of the daily maximum 8-hour average (MDA8) O3 in the model do not completely align with the observations. The model MDA8 O3 had a negative (positive) bias north (south) of 30°N over China. All simulations underestimated the observed CO by 50-60% over China and South Korea. In the Seoul Metropolitan Area (SMA), EDGAR-HTAP v2, v3, and KORUS v5 simulated the vertical shapes and diurnal patterns of O3 and other precursors effectively, but the model underestimated the observed O3, CO and HCHO concentrations. Notably, the model aromatic VOCs were significantly underestimated with the three bottom-up emission inventories, although the KORUS v5 shows improvements. The model isoprene estimations had a positive bias relative to the observations, suggesting that the Model of Emissions of Gases and Aerosols from Nature (MEGAN) version 2.04 overestimated isoprene emissions. Additional model simulations were conducted by doubling CO and VOC emissions over China and South Korea to investigate the causes of the model O3 biases and the effects of the long-range transport on the O3 over South Korea. The doubled CO and VOC emission simulations improved the model O3 simulations for the local emission dominant case, but led to the model O3 overestimations for the transport dominant case, which emphasizes the need for accurate representations of the local VOC emissions over South Korea. [ABSTRACT FROM AUTHOR]