Source Attribution, Physicochemical Properties and Spatial Distribution of Wet Deposited Mercury to the Ohio River Valley

Abstract

Mercury (Hg) is a bioaccumulative neurotoxin that is emitted from anthropogenic sources through fossil fuel combustion. The spatial scale of atmospheric transport prior to deposition is dependent on the chemical and physical form of Hg emissions, and has yet to be quantitatively defined. A five-year comprehensive Hg monitoring and source apportionment study was conducted in Steubenville, Ohio to investigate atmospheric Hg deposition to the highly industrialized Ohio River Valley region. Long-term event-precipitation measurements revealed a significant 30% to three-fold enrichment of Hg concentrations and total Hg deposition flux to the Steubenville site over other Great Lakes regional sites. Multivariate receptor models attributed ~70% of Hg wet deposition to local coal combustion sources. While local stagnant atmospheric conditions led to moderately high volume-weighted mean Hg concentrations and the majority of Hg wet deposition flux, regional transport from the Chicago/Gary and Detroit/Windsor urban areas also led to elevated precipitation Hg concentrations, but did not contribute significantly to the overall Hg deposition. The degree of local source influence was established during a summertime field intensive study in which a local scale network of concurrently collected rain samples revealed that 42% of Hg wet deposition measured less than one km from the base of coal fired utilities could be attributed to the adjacent source, corresponding to 170% Hg concentration enhancement over regionally representative precipitation collected concurrently. In addition, 69±37% of the Hg collected in rain was in a soluble form, entering the precipitation as reactive gas phase or fine particle associated Hg. The Hg scavenging coefficient (rate of concentration reduction throughout a single precipitation event) was particularly low when compared to other trace elements. Furthermore, when compared to an upwind but non-locally source impacted site, the scavenging coefficient for Hg in the locally source influenced precipitation was significantly lower. These results indicate that a continuous source of soluble gaseous Hg may be the reason for the low scavenging coefficient. Therefore, this work revealed through measurements that the chemical forms of Hg in coal combustion emissions, and the physicochemical properties therein, explain the locally elevated Hg wet deposition observed.