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Environ Sci Technol ; 49(17): 10389-97, 2015 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-26161912


We use measurements made onboard the National Science Foundation's C-130 research aircraft during the 2013 Nitrogen, Oxidants, Mercury, and Aerosol Distributions, Sources, and Sinks (NOMADSS) experiment to examine total Hg (THg) emission ratios (EmRs) for six coal-fired power plants (CFPPs) in the southeastern U.S. We compare observed enhancement ratios (ERs) with EmRs calculated using Hg emissions data from two inventories: the National Emissions Inventory (NEI) and the Toxics Release Inventory (TRI). For four CFPPs, our measured ERs are strongly correlated with EmRs based on the 2011 NEI (r(2) = 0.97), although the inventory data exhibit a -39% low bias. Our measurements agree best (to within ±32%) with the NEI Hg data when the latter were derived from on-site emissions measurements. Conversely, the NEI underestimates by approximately 1 order of magnitude the ERs we measured for one previously untested CFPP. Measured ERs are uncorrelated with values based on the 2013 TRI, which also tends to be biased low. Our results suggest that the Hg inventories can be improved by targeting CFPPs for which the NEI- and TRI-based EmRs have significant disagreements. We recommend that future versions of the Hg inventories should provide greater traceability and uncertainty estimates.

Aerossóis/análise , Carvão Mineral/análise , Mercúrio/análise , Nitrogênio/análise , Oxidantes/química , Centrais Elétricas , Poluentes Atmosféricos/análise , Atmosfera/química , Dióxido de Carbono/análise , Modelos Lineares , Sudeste dos Estados Unidos , Dióxido de Enxofre/análise
Environ Sci Technol ; 47(13): 7285-94, 2013 Jul 02.
Artigo em Inglês | MEDLINE | ID: mdl-23425102


The Reno Atmospheric Mercury Intercomparison Experiment (RAMIX) was carried out from 22 August to 16 September, 2011 in Reno, NV to evaluate the performance of new and existing methods to measure atmospheric mercury (Hg). Measurements were made using a common sampling manifold to which controlled concentrations of Hg species, including gaseous elemental mercury (GEM) and HgBr2 (a surrogate gaseous oxidized mercury (GOM) compound), and potential interferents were added. We present an analysis of Hg measurements made using the University of Washington's Detector for Oxidized Hg Species (DOHGS), focusing on tests of GEM and HgBr2 spike recovery, the potential for interference from ozone (O3) and water vapor (WV), and temporal variability of ambient reactive mercury (RM). The mean GEM and HgBr2 spike recoveries measured with the DOHGS were 95% and 66%, respectively. The DOHGS responded linearly to HgBr2. We found no evidence that elevated O3 interfered in the DOHGS RM measurements. A reduction in RM collection and retention efficiencies at very high ambient WV mixing ratios is possible. Comparisons between the DOHGS and participating Hg instruments demonstrate good agreement for GEM and large discrepancies for RM. The results suggest that existing GOM measurements are biased low.

Poluentes Atmosféricos/análise , Brometos/análise , Compostos de Mercúrio/análise , Mercúrio/análise , Monitoramento Ambiental/instrumentação , Monitoramento Ambiental/métodos , Nevada , Oxirredução , Ozônio/análise , Reprodutibilidade dos Testes , Água/análise
Environ Sci Technol ; 47(13): 7295-306, 2013 Jul 02.
Artigo em Inglês | MEDLINE | ID: mdl-23305532


From August 22 to September 16, 2012, atmospheric mercury (Hg) was measured from a common manifold in the field during the Reno Atmospheric Mercury Intercomparison eXperiment. Data were collected using Tekran systems, laser induced fluorescence, and evolving new methods. The latter included the University of Washington-Detector for Oxidized Mercury, the University of Houston Mercury instrument, and a filter-based system under development by the University of Nevada-Reno. Good transmission of total Hg was found for the manifold. However, despite application of standard protocols and rigorous quality control, systematic differences in operationally defined forms of Hg were measured by the sampling systems. Concentrations of reactive Hg (RM) measured with new methods were at times 2-to-3-fold higher than that measured by Tekran system. The low RM recovery by the latter can be attributed to lack of collection as the system is currently configured. Concentrations measured by all instruments were influenced by their sampling location in-the-manifold and the instrument analytical configuration. On the basis of collective assessment of the data, we hypothesize that reactions forming RM were occurring in the manifold. Results provide a new framework for improved understanding of the atmospheric chemistry of Hg.

Poluentes Atmosféricos/análise , Mercúrio/análise , Poluentes Atmosféricos/química , Brometos/análise , Monóxido de Carbono/análise , Monitoramento Ambiental/instrumentação , Monitoramento Ambiental/métodos , Mercúrio/química , Compostos de Mercúrio/análise , Nevada , Ozônio/análise