Gas-particle partitioning of atmospheric Hg(II) and its effect on global mercury deposition

被引:329
作者
Amos, H. M. [1 ]
Jacob, D. J. [1 ,2 ]
Holmes, C. D. [3 ]
Fisher, J. A. [1 ]
Wang, Q. [2 ]
Yantosca, R. M. [2 ]
Corbitt, E. S. [1 ]
Galarneau, E. [4 ]
Rutter, A. P. [5 ]
Gustin, M. S. [6 ]
Steffen, A. [4 ]
Schauer, J. J. [7 ]
Graydon, J. A. [8 ]
St Louis, V. L. [8 ]
Talbot, R. W. [9 ]
Edgerton, E. S. [10 ]
Zhang, Y. [11 ]
Sunderland, E. M. [2 ,12 ]
机构
[1] Harvard Univ, Dept Earth & Planetary Sci, Cambridge, MA 02138 USA
[2] Harvard Univ, Sch Engn & Appl Sci, Boston, MA 02115 USA
[3] Univ Calif Irvine, Dept Earth Syst Sci, Irvine, CA USA
[4] Environm Canada, Air Qual Res Div, Toronto, ON, Canada
[5] Rice Univ, Dept Civil & Environm Engn, Houston, TX USA
[6] Univ Nevada, Dept Nat Resources & Environm Sci, Reno, NV 89557 USA
[7] Univ Wisconsin, Dept Civil & Environm Engn, Madison, WI 53706 USA
[8] Univ Alberta, Dept Biol Sci, Edmonton, AB, Canada
[9] Univ Houston, Dept Earth & Atmospher Sci, Houston, TX USA
[10] Atmospher Res & Anal Inc, Cary, NC USA
[11] Univ Washington, Dept Atmospher Sci, Seattle, WA 98195 USA
[12] Harvard Univ, Dept Environm Hlth, Boston, MA 02115 USA
基金
美国国家科学基金会; 加拿大自然科学与工程研究理事会;
关键词
REACTIVE GASEOUS MERCURY; SECONDARY ORGANIC AEROSOL; SOUTHERN NEW-HAMPSHIRE; CHEMICAL TRACER MODEL; POWER-PLANT PLUMES; DRY DEPOSITION; WET DEPOSITION; PARTICULATE MERCURY; UNITED-STATES; SCIENTIFIC UNCERTAINTIES;
D O I
10.5194/acp-12-591-2012
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Atmospheric deposition of Hg(II) represents a major input of mercury to surface environments. The phase of Hg(II) (gas or particle) has important implications for deposition. We use long-term observations of reactive gaseous mercury (RGM, the gaseous component of Hg(II)), particle-bound mercury (PBM, the particulate component of Hg(II)), fine particulate matter (PM2.5), and temperature (T) at five sites in North America to derive an empirical gas-particle partitioning relationship log(10)(K-1) = (10 +/- 1)-(2500 +/- 300)/T where K = (PBM/PM2.5)/RGM with PBM and RGM in common mixing ratio units, PM2.5 in mu g m(-3), and T in K. This relationship is within the range of previous work but is based on far more extensive data from multiple sites. We implement this empirical relationship in the GEOS-Chem global 3-D Hg model to partition Hg(II) between the gas and particle phases. The resulting gas-phase fraction of Hg(II) ranges from over 90% in warm air with little aerosol to less than 10% in cold air with high aerosol. Hg deposition to high latitudes increases because of more efficient scavenging of particulate Hg(II) by precipitating snow. Model comparison to Hg observations at the North American surface sites suggests that subsidence from the free troposphere (warm air, low aerosol) is a major factor driving the seasonality of RGM, while elevated PBM is mostly associated with high aerosol loads. Simulation of RGM and PBM at these sites is improved by including fast in-plume reduction of Hg(II) emitted from coal combustion and by assuming that anthropogenic particulate Hg(p) behaves as semivolatile Hg(II) rather than as a refractory particulate component. We improve the simulation of Hg wet deposition fluxes in the US relative to a previous version of GEOS-Chem; this largely reflects independent improvement of the washout algorithm. The observed wintertime minimum in wet deposition fluxes is attributed to inefficient snow scavenging of gas-phase Hg(II).
引用
收藏
页码:591 / 603
页数:13
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