SO2 over central China: Measurements, numerical simulations and the tropospheric sulfur budget

SO2in central China was measured in situ from an aircraft and remotely using the Ozone Monitoring Instrument (OMI) from the Aura satellite; results were used to develop a numerical tool for evaluating the tropospheric sulfur budget ‐ sources, sinks, transformation and transport. In April 2008, measured ambient SO2 concentrations decreased from ∼7 ppbv near the surface to ∼1 ppbv at 1800 m altitude (an effective scale height of ∼800 m), but distinct SO2 plumes were observed between 1800 and 4500 m, the aircraft's ceiling. These free tropospheric plumes play a major role in the export of SO2 and in the accuracy of OMI retrievals. The mean SO2 column contents from aircraft measurements (0.73 DU, Dobson Units) and operational OMI SO2 products (0.63 ± 0.26 DU) were close. The OMI retrievals were well correlated with in situ measurements (r = 0.84), but showed low bias (slope = 0.54). A new OMI retrieval algorithm was tested and showed improved agreement and bias (r = 0.87, slope = 0.86). The Community Multiscale Air Quality (CMAQ) model was used to simulate sulfur chemistry, exhibiting reasonable agreement (r = 0.62, slope = 1.33) with in situ SO2 columns. The mean CMAQ SO2 loading over central and eastern China was 54 kT, ∼30% more than the estimate from OMI SO2 products, 42 kT. These numerical simulations, constrained by observations, indicate that ∼50% (35 to 61%) of the anthropogenic sulfur emissions were transported downwind, and the overall lifetime of tropospheric SO2 was 38 ± 7 h. Key Points Tropospheric SO2 was measured by aircraft in spring 2008 over central China OMI SO2 products (BRD and ISF algorithm) were validated CMAQ model simulated and estimated export of sulfur compounds