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© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 11 Sep 2019

Submitted as: research article | 11 Sep 2019

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This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

Mapping the drivers of uncertainty in atmospheric selenium deposition with global sensitivity analysis

Aryeh Feinberg1,2,3, Moustapha Maliki4, Andrea Stenke1, Bruno Sudret4, Thomas Peter1, and Lenny H. E. Winkel2,3 Aryeh Feinberg et al.
  • 1Institute for Atmospheric and Climate Science, ETH Zurich, Zurich, Switzerland
  • 2Institute of Biogeochemistry and Pollutant Dynamics, ETH Zurich, Zurich, Switzerland
  • 3Eawag, Swiss Federal Institute of Aquatic Science and Technology, Dübendorf, Switzerland
  • 4Chair of Risk, Safety and Uncertainty Quantification, ETH Zurich, Zurich, Switzerland

Abstract. An estimated 0.5–1 billion people globally have inadequate intakes of selenium (Se), due to a lack of bioavailable Se in agricultural soils. Deposition from the atmosphere, especially through precipitation, is an important source of Se to soils. However, very little is known about the atmospheric cycling of Se. It has therefore been difficult to predict how far Se travels in the atmosphere and where it deposits. To answer these questions, we have built the first global atmospheric Se model by implementing Se chemistry into an aerosol–chemistry–climate model, SOCOL-AER. In the model, we include information from the literature about the emissions, speciation, and chemical transformation of atmospheric Se. Natural processes and anthropogenic activities emit volatile Se compounds, which oxidize quickly and partition to the particulate phase. Our model tracks the transport and deposition of Se in 7 gas-phase species and 41 aerosol tracers. However, there are large uncertainties associated with many of the model's input parameters. In order to identify which model uncertainties are the most important for understanding the atmospheric Se cycle, we conducted a global sensitivity analysis with 34 input parameters related to Se chemistry, Se emissions, and the interaction of Se with aerosols. In the first bottom-up estimate of its kind, we have calculated a median global atmospheric lifetime of 4.4 d (days), ranging from 2.9–6.4 d (2nd–98th percentile) given the uncertainties of the input parameters. The uncertainty in the Se lifetime is mainly driven by the uncertainty in the carbonyl selenide (OCSe) oxidation rate and the lack of tropospheric aerosol species other than sulfate aerosols in SOCOL-AER. In contrast to uncertainties in Se lifetime, the uncertainty in deposition flux maps are governed by Se emission factors, with all four Se sources (volcanic, marine biosphere, terrestrial biosphere, and anthropogenic emissions) contributing equally to the uncertainty in deposition over agricultural areas. We evaluated the simulated Se wet deposition fluxes from SOCOL-AER with a compiled database of rainwater Se measurements, since wet deposition contributes around 80 % of total Se deposition. Despite difficulties in comparing a global, coarse resolution model with local measurements from a range of time periods, past Se wet deposition measurements are within the range of the model's 2nd–98th percentile at 79 % of background sites. This agreement validates the application of the SOCOL-AER model to identifying regions which are at risk of low atmospheric Se inputs. In order to constrain the uncertainty in Se deposition fluxes over agricultural soils we should prioritize field campaigns measuring Se emissions, rather than laboratory measurements of Se rate constants.

Aryeh Feinberg et al.
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Status: open (until 06 Nov 2019)
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Aryeh Feinberg et al.
Data sets

Simulation data used for sensitivity analysis of atmospheric selenium in SOCOL-AER A. Feinberg, M. Maliki, A. Stenke, B. Sudret, T. Peter, and L. H. E. Winkel

Aryeh Feinberg et al.
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Short summary
The amount of the micronutrient selenium in food largely depends on the amount and form of selenium in soil. The atmosphere acts as a source of selenium to soils through deposition, yet little information is available about atmospheric selenium cycling. Therefore, we built the first global atmospheric selenium model. Through sensitivity and uncertainty analysis we determine that selenium can be transported thousands of kilometres and that measurements of selenium emissions should be prioritized.
The amount of the micronutrient selenium in food largely depends on the amount and form of...