Top-down estimate of mercury emissions in China using four-dimensional variational data assimilation

An inverse modeling method using the four-dimensional variational data assimilation approach is developed to provide a top-down estimate of mercury emission inventory in China. The mercury observations on board the C130 aircraft during the Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia) campaign in April 2001 are assimilated into a regional chemical transport model, STEM. Using a 340 Mg of elemental mercury emitted in 1999, the assimilation results in an increase in Hg⁰ emissions for China to 1140 Mg in 2001. This is an upper limit amount of the elemental mercury required in China. The average emission-scaling factor is ～3.4 in China. The spatial changes in the mercury emissions after the assimilation are also evaluated. The largest changes are estimated on the China north-east coastal areas and the areas of north-center China. The influences of the observation and inventory uncertainties and the initial and boundary conditions on the emission estimates are discussed. Increasing the boundary conditions of Hg from 1.2 to 1.5 ng m^?3, results in a top-down estimate of Hg⁰ emissions for China of 718 Mg, and leads the average scaling factor from 3.4 to 2.1.