Chemistry plays an indispensable role in investigations of the atmosphere; however, many climate models either ignore or greatly simplify atmospheric chemistry, limiting both their accuracy and their scope. We present the development and evaluation of the online global atmospheric chemical model BCC-GEOS-Chem v1.0, coupling the GEOS-Chem chemical transport model (CTM) as an atmospheric chemistry component in the Beijing Climate Center atmospheric general circulation model (BCC-AGCM). The GEOS-Chem atmospheric chemistry component includes detailed troposphericHO_x–NO_x–volatile organic compounds–ozone–bromine–aerosol chemistry and online dry and wet deposition schemes. We then demonstrate the new capabilities of BCC-GEOS-Chem v1.0 relative to the base BCC-AGCM model through a 3-year (2012–2014) simulation with anthropogenic emissions from the Community Emissions Data System (CEDS) used in the Coupled Model Intercomparison Project Phase 6 (CMIP6). The model captures well the spatial distributions and seasonal variations in tropospheric ozone, with seasonal mean biases of 0.4–2.2 ppbv at 700–400 hPa compared to satellite observations and within 10 ppbv at the surface to 500 hPa compared to global ozonesonde observations. The model has larger high-ozone biases over the tropics which we attribute to an overestimate of ozone chemical production. It underestimates ozone in the upper troposphere which is likely due either to the use of a simplified stratospheric ozone scheme or to biases in estimated stratosphere–troposphere exchange dynamics. The model diagnoses the global tropospheric ozone burden, OH concentration, and methane chemical lifetime to be 336 Tg, 1.16×10⁶ molecule cm⁻³, and 8.3 years, respectively, which is consistent with recent multimodel assessments. The spatiotemporal distributions of NO₂, CO, SO₂, CH₂O, and aerosol optical depth are generally in agreement with satellite observations. The development of BCC-GEOS-Chem v1.0 represents an important step for the development of fully coupled earth system models (ESMs) in China.

Nitrate and sulfate are two key components of airborne particulate matter (PM). While multiple formation mechanisms have been proposed for sulfate, current air quality models commonly underestimate its concentrations and mass fractions during northern China winter haze events. On the other hand, current models usually overestimate the mass fractions of nitrate. Very recently, laboratory studies have proposed that nitrous acid (N(III)) produced by particulate nitrate photolysis can oxidize sulfur dioxide to produce sulfate. Here, for the first time, we parameterize this heterogeneous mechanism into the state-of-the-art Community Multi-scale Air Quality (CMAQ) model and quantify its contributions to sulfate formation. We find that the significance of this mechanism mainly depends on the enhancement effects (by 1–3 orders of magnitude as suggested by the available experimental studies) of nitrate photolysis rate constants in aerosol liquid water compared to that in the gas phase. Comparisons between model simulations and in-situ observations in Beijing suggest that this pathway can explain about 15% (assuming an enhancement factor (EF) of 10) to 65% (assuming EF = 100) of the model–observation gaps in sulfate concentrations during winter haze. Our study strongly calls for future research on reducing the uncertainty in EF.

A regional fully coupled meteorology–chemistry model, Weather Research and Forecasting model with Chemistry (WRF-Chem), was employed to study the seasonality of ozone (O₃) pollution and its sources in both China and India. Observations and model results suggest that O₃ in the North China Plain (NCP), Yangtze River Delta (YRD), Pearl River Delta (PRD), and India exhibit distinctive seasonal features, which are linked to the influence of summer monsoons. Through a factor separation approach, we examined the sensitivity of O₃ to individual anthropogenic, biogenic, and biomass burning emissions. We found that summer O₃ formation in China is more sensitive to industrial and biogenic sources than to other source sectors, while the transportation and biogenic sources are more important in all seasons for India. Tagged simulations suggest that local sources play an important role in the formation of the summer O₃ peak in the NCP, but sources from Northwest China should not be neglected to control summer O₃ in the NCP. For the YRD region, prevailing winds and cleaner air from the ocean in summer lead to reduced transport from polluted regions, and the major source region in addition to local sources is Southeast China. For the PRD region, the upwind region is replaced by contributions from polluted PRD as autumn approaches, leading to an autumn peak. The major upwind regions in autumn for the PRD are YRD (11 %) and Southeast China (10 %). For India, sources in North India are more important than sources in the south. These analyses emphasize the relative importance of source sectors and regions as they change with seasons, providing important implications for O₃ control strategies.