Jiaoyan Huang

Ambient mercury sources in Rochester, NY: results from Principle Components Analysis (PCA) of Mercury Monitoring Network Data.

Continuous atmospheric measurements of speciated mercury (Hg) (elemental mercury (Hg⁰), reactive gaseous mercury (RGM), and particulate mercury (Hgp)) were made in Rochester, NY from Dec 2007 to May 2009. Continuous measurements of ozone (O₃), sulfur dioxide (SO₂), carbonmonoxide (CO), particulate matter (PM₂.₅), and meteorological data were also available. A principle components analysis (PCA) of 3886 observations of 13 variables for the period identified six major factors. Melting snow was observed to be a source of Hg⁰in winters. Positive correlations between RGM and O₃ in the spring and summer may be indicative of Hg⁰ oxidation. RGM concentrations increased simultaneously with SO₂ suggesting the influence of coal fired power plants (CFPP). The fifth factor (F5) containing O₃ (high negative loading), CO (positive loading), Hg⁰ and Hg(p) (positive), and/or RGM (negative) was identified as a mobile source which was usually observed during morning rush hours (6:00-9:00 a.m.). The concentrations of the three mercury species from the direction of the CFPP were significantly reduced following the shutdown of this source.

Impacts of the Canadian Forest Fires on Atmospheric Mercury and Carbonaceous Particles in Northern New York

The impact of Canadian forest fires in Quebec on May 31, 2010 on PM(2.5), carbonaceous species, and atmospheric mercury species was observed at three rural sites in northern New York. The results were compared with previous studies during a 2002 Quebec forest fire episode. MODIS satellite images showed transport of forest fire smoke from southern Quebec, Canada to northern New York on May 31, 2010. Back-trajectories were consistent with this regional transport. During the forest fire event, as much as an 18-fold increase in PM(2.5) concentration was observed. The concentrations of episode-related OC, EC, BC, UVBC, and their difference (Delta-C), reactive gaseous mercury (RGM), and particle-bound mercury (PBM) were also significantly higher than those under normal conditions, suggesting a high impact of Canadian forest fire emissions on air quality in northern New York. PBM, RGM, and Delta-C are all emitted from forest fires. The correlation coefficient between Delta-C and other carbonaceous species may serve as an indicator of forest fire smoke. Given the marked changes in PBM, it may serve as a more useful tracer of forest fires over distances of several hundred kilometers relative to GEM. However, the Delta-C concentration changes are more readily measured.

Variation in concentrations of three mercury (Hg) forms at a rural and a suburban site in New York State

Tekran® Hg speciation systems were used at a rural site (Huntington Forest, NY; HF) and a suburban site (Rochester, NY; ROC) to measure gaseous elemental mercury (GEM), gaseous oxidized mercury (GOM), and fine particulate-bound mercury (PBM2.5) concentrations for two years (December 2007 to November 2009). Ancillary data were also available from the New York State Department of Environmental Conservation and the United States Environmental Protection Agency Clean Air Status and Trends Network. Seasonal GEM concentrations were similar at both sites and influenced by factors such as the planet boundary layer (PBL) height and mercury emissions from snow, soil, and point sources. In some seasons, O3 was negatively correlated with GEM at ROC and positively correlated with GEM at HF. At HF, O3 was correlated with GOM and was typically higher in the afternoon. The cause of this pattern may be photochemical reactions during the day, and the GOM diel pattern may also be due to deposition which is enhanced by dew formation during the night and early morning. PBM2.5 concentrations were higher in winter at both sites. This is indicative of local wood combustion for space heating in winter, increased sorption to particles at lower temperatures, and lower PBL in the winter. At the suburban site, 2 of 12 events with enhanced GEM/CO ratios were poorly correlated with SO2/GOM, implying that these two events were due either to long range transport or regional metallurgical industries in Canada.

An evaluation of direct measurement techniques for mercury dry deposition

In this project, several surrogate surfaces designed to directly measure Hg dry deposition were investigated. Static water surrogate surfaces (SWSS) containing deionized (DI), acidified water, or salt solutions, and a knife-edge surrogate surface (KSS) using quartz fiber filters (QFF), KCl-coated QFF and gold-coated QFF were evaluated as a means to directly measure mercury (Hg) dry deposition. The SWSS was hypothesized to collect deposited elemental mercury (Hg⁰), reactive gaseous/oxidized mercury (RGM), and mercury associated with particulate matter (Hg(p)) while the QFF, KCl-coated QFF, and gold-coated QFF on the KSS were hypothesized to collect Hg(p), RGM+Hg(p), and Hg⁰+RGM+Hg(p), respectively. The Hg flux measured by the DI water was significantly smaller than that captured by the acidified water, probably because Hg⁰ was oxidized to Hg²+ which stabilized the deposited Hg and decreased mass transfer resistance. Acidified BrCl, which efficiently oxidizes Hg⁰, captured significantly more Hg than other solutions. However, of all collection media, gold-coated QFFs captured 6 to 100 times greater Hg mass than the other surfaces, probably because there is no surface resistance for Hg⁰ deposition to gold surfaces. In addition, the Hg⁰ concentration is usually 100-1000 times higher than RGM and Hg(p). For all other media, co-located samples were not significantly different, and the combination of daytime plus nighttime results were comparable to 24-h samples, implying that Hg⁰, RGM and Hg(p) were not released after they deposited nor did the surfaces reach equilibrium with the atmosphere. Based on measured Hg ambient air concentrations and fluxes, dry deposition velocities of RGM and Hg⁰ to DI water and other surfaces were 5.6±5.4 and 0.005-0.68 cm s⁻¹ in this study, respectively. These results suggest surrogate surfaces can be used to measure Hg dry deposition; however, extrapolating the results to natural surface can be challenging.

Mercury (Hg) emissions from domestic biomass combustion for space heating

Three mercury (Hg) species (gaseous elemental mercury (GEM), gaseous oxidized mercury (GOM), and fine particulate-bound mercury (PBM(2.5))) were measured in the stack of a small scale wood combustion chamber at 400°C, in the stack of an advanced wood boiler, and in two areas influenced by wood combustion. The low temperature process (lab-scale) emitted mostly GEM (∼99% when burning wood pellets and ∼95% when burning unprocessed wood). The high temperature wood boiler emitted a greater proportion of oxidized Hg (approximately 65%) than the low temperature system. In field measurements, mean PBM(2.5) concentrations at the rural and urban sites in winter were statistically significantly higher than in warmer seasons and were well correlated with Delta-C concentrations, a wood combustion indictor measured by an aethalometer (UV-absorbable carbon minus black carbon). Overall the results suggest that wood combustion may be an important source of oxidized mercury (mostly in the particulate phase) in northern climates in winter.

Effect of the shutdown of a large coal-fired power plant on ambient mercury species

In the spring of 2008, a 260MWe coal-fired power plant (CFPP) located in Rochester, New York was closed over a 4month period. Using a 2-years data record, the impacts of the shutdown of the CFPP on nearby ambient concentrations of three Hg species were quantified. The arithmetic average ambient concentrations of gaseous elemental mercury (GEM), gaseous oxidized mercury (GOM), and particulate mercury (PBM) during December 2007-November 2009 were 1.6ngm(-3), 5.1pgm(-3), and 8.9pgm(-3), respectively. The median concentrations of GEM, GOM, and PBM significantly decreased by 12%, 73%, and 50% after the CFPP closed (Mann-Whitney test, p<0.001). Positive Matrix Factorization (EPA PMF v4.1) identified six factors including O3-rich, traffic, gas phase oxidation, wood combustion, nucleation, and CFPP. When the CFPP was closed, median concentrations of GEM, GOM, and PBM apportioned to the CFPP factor significantly decreased by 25%, 74%, and 67%, respectively, compared to those measured when the CFPP was still in operation (Mann-Whitney test, p<0.001). Conditional probability function (CPF) analysis showed the greatest reduction in all three Hg species was associated with northwesterly winds pointing toward the CFPP. These changes were clearly attributable to the closure of the CFPP.

Atmospheric mercury pollution at an urban site in central Taiwan: Mercury emission sources at ground level

Total gaseous mercury (Hg) (TGM), gaseous oxidized Hg (GOM), and particulate-bound Hg (PBM) concentrations and dry depositions were measured at an urban site in central Taiwan. The concentrations were 6.14±3.91 ng m(-3), 332±153, and 71.1±46.1 pg m(-3), respectively. These results demonstrate high Hg pollution at the ground level in Taiwan. A back trajectory plot shows the sources of the high TGM concentration were in the low atmosphere (<500 m) and approximately 50% of the air masses coming from upper troposphere (>500 m) were associated with low TGM concentrations. This finding implies that Hg is trapped in the low atmosphere and comes from local Hg emission sources. The conditional probability function (CPF) reveals that the plumes of high TGM concentrations come from the south and northwest of the site. The plume from the south comes from two municipal solid waste incinerators (MSWIs). However, no significant Hg point source is located to the northwest of the site; therefore, the plumes from the northwest are hypothesized to be related to the combustion of agricultural waste. Dry deposition fluxes of Hg measured at this site considerably exceeded those measured in North America. Overall, this area is regarded as a highly Hg contaminated area because of local Hg emission sources.