Atmospheric Wet Deposition in Remote Regions: Benchmarks for Environmental Change

William C. Keene Department of Environmental Sciences, University of Virginia, Charlottesville, Virginia

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James N. Galloway Department of Environmental Sciences, University of Virginia, Charlottesville, Virginia

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Gene E. Likens Cary Institute of Ecosystem Studies, Millbrook, New York, and Department of Ecology and Evolutionary Biology, University of Connecticut, Storrs, Connecticut

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Frank A. Deviney Department of Environmental Sciences, University of Virginia, Charlottesville, Virginia

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Kerri N. Mikkelsen Department of Environmental Sciences, University of Virginia, Charlottesville, Virginia

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Jennie L. Moody Department of Environmental Sciences, University of Virginia, Charlottesville, Virginia

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John R. Maben Department of Environmental Sciences, University of Virginia, Charlottesville, Virginia

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Abstract

Precipitation composition was characterized at 14 remote sites between 65°N and 51°S. Anthropogenic sources contributed to non-sea-salt (nss) SO42−, NO3, and NH4+ in North Atlantic precipitation. Biogenic sources accounted for 0.4–3.3 μeq L−1 of volume-weighted-average (VWA) nss SO42− in marine precipitation. SO42− at the continental sites (2.9–7.7 μeq L−1) was generally higher. VWA NO3 (0.5–1.3 μeq L−1) and NH4+ (0.5–2.6 μeq L−1) at marine-influenced, Southern Hemispheric sites were generally less than those at continental sites (1.4–4.8 μeq L−1 and 2.3–4.2 μeq L−1, respectively). VWA pH ranged from 4.69 to 5.25. Excluding the North Atlantic, nss SO42−, NO3, and NH4+ wet depositions were factors of 4–47, 5–61, and 3–39, respectively, less than those in the eastern United States during 2002–04. HCOOHt (HCOOHaq + HCOO) and CH3COOHt (CH3COOHaq + CH3COO) concentrations and depositions at marine sites overlapped, implying spatially similar source strengths from marine-derived precursors. Greater variability at continental sites suggests heterogeneity in terrestrial source strengths. Seasonality in deposition was driven by variability in precipitation amount, wind velocity, transport, and emissions. Between 1980 and 2009, nss SO42− at Bermuda decreased by 85% in response to decreasing U.S. SO2 emissions; trends in NO3 and NH4+ were inconsequential. Corresponding decreases in acidity, as reflected in the significant 30% decline in VWA H+, impacted pH-dependent chemical processes. Comparisons between measurements and models indicate that current predictive capabilities are uncertain by factors of 2 or more.

Current affiliation: Commonwealth Computer Research, Inc., Charlottesville, Virginia.

Current affiliation: FirstCarbon Solutions, San Bernardino, California.

Corresponding author address: William C. Keene, Environmental Sciences, University of Virginia, Clark Hall, 291 McCormick Road, P.O. Box 400123, Charlottesville, VA 22904-4123. E-mail: wck@virginia.edu

Abstract

Precipitation composition was characterized at 14 remote sites between 65°N and 51°S. Anthropogenic sources contributed to non-sea-salt (nss) SO42−, NO3, and NH4+ in North Atlantic precipitation. Biogenic sources accounted for 0.4–3.3 μeq L−1 of volume-weighted-average (VWA) nss SO42− in marine precipitation. SO42− at the continental sites (2.9–7.7 μeq L−1) was generally higher. VWA NO3 (0.5–1.3 μeq L−1) and NH4+ (0.5–2.6 μeq L−1) at marine-influenced, Southern Hemispheric sites were generally less than those at continental sites (1.4–4.8 μeq L−1 and 2.3–4.2 μeq L−1, respectively). VWA pH ranged from 4.69 to 5.25. Excluding the North Atlantic, nss SO42−, NO3, and NH4+ wet depositions were factors of 4–47, 5–61, and 3–39, respectively, less than those in the eastern United States during 2002–04. HCOOHt (HCOOHaq + HCOO) and CH3COOHt (CH3COOHaq + CH3COO) concentrations and depositions at marine sites overlapped, implying spatially similar source strengths from marine-derived precursors. Greater variability at continental sites suggests heterogeneity in terrestrial source strengths. Seasonality in deposition was driven by variability in precipitation amount, wind velocity, transport, and emissions. Between 1980 and 2009, nss SO42− at Bermuda decreased by 85% in response to decreasing U.S. SO2 emissions; trends in NO3 and NH4+ were inconsequential. Corresponding decreases in acidity, as reflected in the significant 30% decline in VWA H+, impacted pH-dependent chemical processes. Comparisons between measurements and models indicate that current predictive capabilities are uncertain by factors of 2 or more.

Current affiliation: Commonwealth Computer Research, Inc., Charlottesville, Virginia.

Current affiliation: FirstCarbon Solutions, San Bernardino, California.

Corresponding author address: William C. Keene, Environmental Sciences, University of Virginia, Clark Hall, 291 McCormick Road, P.O. Box 400123, Charlottesville, VA 22904-4123. E-mail: wck@virginia.edu
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