Source attribution and process analysis for atmospheric mercury in eastern China simulated by CMAQ-Hg

Abstract

The contribution from different emission sources and atmospheric processes to gaseous elemental mercury (GEM), gaseous oxidized mercury (GOM), particulate bound mercury (PBM) and mercury deposition in eastern China were quantified using the Community Multi-scale Air Quality (CMAQ-Hg) modeling system run with a nested domain. Natural sources (NAT) and six categories of anthropogenic mercury sources (ANTH) including cement production (CEM), domestic life (DOM), industrial boilers (IND), metal production (MET), coal-fired power plants (PP) and traffic (TRA) were considered for source apportionment. NAT were responsible for 36.6 % of annual averaged GEM concentration, which was regarded as the most important source for GEM in spite of obvious seasonal variation. Among ANTH, the influence of MET and PP on GEM were most evident especially in winter. ANTH dominated the variations of GOM and PBM concentrations with contributions of 86.7 and 79.1 %, respectively. Among ANTH, IND were the largest contributor for GOM (57.5 %) and PBM (34.4 %) so that most mercury deposition came from IND. The effect of mercury emitted from out of China was indicated by a > 30 % contribution to GEM concentration and wet deposition. The contributions from nine processes – consisting of emissions (EMIS), gas-phase chemical production/loss (CHEM), horizontal advection (HADV), vertical advection (ZADV), horizontal advection (HDIF), vertical diffusion (VDIF), dry deposition (DDEP), cloud processes (CLDS) and aerosol processes (AERO) – were calculated for process analysis with their comparison in urban and non-urban regions of the Yangtze River delta (YRD). EMIS and VDIF affected surface GEM and PBM concentrations most and tended to compensate each other all the time in both urban and non-urban areas. However, DDEP was the most important removal process for GOM with 7.3 and 2.9 ng m−3 reduced in the surface of urban and non-urban areas, respectively, in 1 day. The diurnal profile variation of processes revealed the transportation of GOM from urban area to non-urban areas and the importance of CHEM/AERO in higher altitudes which partly caused diffusion of GOM downwards to non-urban areas. Most of the anthropogenic mercury was transported and diffused away from urban areas by HADV and VDIF and increased mercury concentrations in non-urban areas by HADV. Natural emissions only influenced CHEM and AERO more significantly than anthropogenic. Local emissions in the YRD contributed 8.5 % more to GEM and ~ 30 % more to GOM and PBM in urban areas compared to non-urban areas.