Particulate chloride (Cl) can be transformed to nitryl chloride (ClNO) via heterogeneous reaction with nitrogen pentoxide (NO) at night. Photolysis of ClNO and subsequent reactions of chlorine radical with other gases can significantly affect the atmospheric photochemistry. In China, the only available integrated anthropogenic chloride emission inventory was compiled in the 1990s with low spatial resolution, which hinders assessment of impact of ClNO on current air quality. In this study, we developed an up-to-date and high-resolution anthropogenic inventory of hydrogen chloride (HCl) and fine particulate Cl emissions in China for 2014 with 0.1° × 0.1° resolution. Detailed local data and county-level activity data were collected and complied. The anthropogenic emissions of HCl and fine particulate Cl in 2014 were estimated to be 458 and 486 Gg, respectively. Biomass burning was the largest contributor, accounting for 75% of fine particulate Cl emission and 32% of HCl emission. Northeast China and North China Plain were the largest chloride emitters. The monthly distribution varied in different regions, due to different agricultural activities and climate conditions. This work updates the chloride emission information and improves its spatial and temporal resolution, which enables better quantification of the ClNO production and its impact over China.
Abstract. Mercury transformation mechanisms and speciation profiles are reviewed for mercury formed in and released from flue gases of coal-fired boilers, non-ferrous metal smelters, cement plants, iron and steel plants, waste incinerators, biomass burning and so on. Mercury in coal, ores, and other raw materials is released to flue gases in the form of Hg 0 during combustion or smelting in boilers, kilns or furnaces. Decreasing temperature from over 800 • C to below 300 • C in flue gases leaving boilers, kilns or furnaces promotes homogeneous and heterogeneous oxidation of Hg 0 to gaseous divalent mercury (Hg 2+ ), with a portion of Hg 2+ adsorbed onto fly ash to form particulate-bound mercury (Hg p ). Halogen is the primary oxidizer for Hg 0 in flue gases, and active components (e.g., TiO 2 , Fe 2 O 3 , etc.) on fly ash promote heterogeneous oxidation and adsorption processes. In addition to mercury removal, mercury transformation also occurs when passing through air pollution control devices (APCDs), affecting the mercury speciation in flue gases. In coal-fired power plants, selective catalytic reduction (SCR) system promotes mercury oxidation by 34-85 %, electrostatic precipitator (ESP) and fabric filter (FF) remove over 99 % of Hg p , and wet flue gas desulfurization system (WFGD) captures 60-95 % of Hg 2+ . In non-ferrous metal smelters, most Hg 0 is converted to Hg 2+ and removed in acid plants (APs). For cement clinker production, mercury cycling and operational conditions promote heterogeneous mercury oxidation and adsorption. The mercury speciation profiles in flue gases emitted to the atmosphere are determined by transformation mechanisms and mercury removal efficiencies by various APCDs. For all the sectors reviewed in this study, Hg p accounts for less than 5 % in flue gases. In China, mercury emission has a higher Hg 0 fraction (66-82 % of total mercury) in flue gases from coal combustion, in contrast to a greater Hg 2+ fraction (29-90 %) from non-ferrous metal smelting, cement and iron and/or steel production. The higher Hg 2+ fractions shown here than previous estimates may imply stronger local environmental impacts than previously thought, caused by mercury emissions in East Asia. Future research should focus on determining mercury speciation in flue gases from iron and steel plants, waste incineration and biomass burning, and on elucidating the mechanisms of mercury oxidation and adsorption in flue gases.
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