Top-down constraints on atmospheric mercury emissions and implications for global biogeochemical cycling
We perform global-scale inverse modeling to constrain present-day atmospheric mercury emissions and relevant physiochemical parameters in the GEOS-Chem chemical transport model. We use Bayesian inversion methods combining simulations with GEOS-Chem and ground-based Hg[superscript 0] observations fro...
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| 语言: | en_US |
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Copernicus GmbH
2015
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| 在线阅读: | http://hdl.handle.net/1721.1/98104 https://orcid.org/0000-0002-6396-5622 https://orcid.org/0000-0001-6395-7422 |
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| author | Soerensen, A. L. Angot, H. Artz, R. Brooks, S. Brunke, E.-G. Conley, G. Dommergue, A. Ebinghaus, R. Holsen, T. M. Jaffe, D. A. Kang, S. Kelley, P. Luke, W. T. Magand, O. Marumoto, K. Pfaffhuber, K. A. Ren, X. Sheu, G.-R. Slemr, F. Warneke, T. Weigelt, A. Weiss-Penzias, P. Wip, D. C. Zhang, Q. Song, Shaojie Selin, Noelle E |
| author2 | Massachusetts Institute of Technology. Department of Earth, Atmospheric, and Planetary Sciences |
| author_facet | Massachusetts Institute of Technology. Department of Earth, Atmospheric, and Planetary Sciences Soerensen, A. L. Angot, H. Artz, R. Brooks, S. Brunke, E.-G. Conley, G. Dommergue, A. Ebinghaus, R. Holsen, T. M. Jaffe, D. A. Kang, S. Kelley, P. Luke, W. T. Magand, O. Marumoto, K. Pfaffhuber, K. A. Ren, X. Sheu, G.-R. Slemr, F. Warneke, T. Weigelt, A. Weiss-Penzias, P. Wip, D. C. Zhang, Q. Song, Shaojie Selin, Noelle E |
| author_sort | Soerensen, A. L. |
| collection | MIT |
| description | We perform global-scale inverse modeling to constrain present-day atmospheric mercury emissions and relevant physiochemical parameters in the GEOS-Chem chemical transport model. We use Bayesian inversion methods combining simulations with GEOS-Chem and ground-based Hg[superscript 0] observations from regional monitoring networks and individual sites in recent years. Using optimized emissions/parameters, GEOS-Chem better reproduces these ground-based observations and also matches regional over-water Hg[superscript 0] and wet deposition measurements. The optimized global mercury emission to the atmosphere is ~ 5.8 Gg yr[superscript −1]. The ocean accounts for 3.2 Gg yr[superscript −1] (55% of the total), and the terrestrial ecosystem is neither a net source nor a net sink of Hg[superscript 0]. The optimized Asian anthropogenic emission of Hg[superscript 0] (gas elemental mercury) is 650–1770 Mg yr[superscript −1], higher than its bottom-up estimates (550–800 Mg yr[superscript −1]). The ocean parameter inversions suggest that dark oxidation of aqueous elemental mercury is faster, and less mercury is removed from the mixed layer through particle sinking, when compared with current simulations. Parameter changes affect the simulated global ocean mercury budget, particularly mass exchange between the mixed layer and subsurface waters. Based on our inversion results, we re-evaluate the long-term global biogeochemical cycle of mercury, and show that legacy mercury becomes more likely to reside in the terrestrial ecosystem than in the ocean. We estimate that primary anthropogenic mercury contributes up to 23 % of present-day atmospheric deposition. |
| first_indexed | 2024-09-23T12:07:38Z |
| format | Article |
| id | mit-1721.1/98104 |
| institution | Massachusetts Institute of Technology |
| language | en_US |
| last_indexed | 2024-09-23T12:07:38Z |
| publishDate | 2015 |
| publisher | Copernicus GmbH |
| record_format | dspace |
| spelling | mit-1721.1/981042024-05-15T02:21:28Z Top-down constraints on atmospheric mercury emissions and implications for global biogeochemical cycling Soerensen, A. L. Angot, H. Artz, R. Brooks, S. Brunke, E.-G. Conley, G. Dommergue, A. Ebinghaus, R. Holsen, T. M. Jaffe, D. A. Kang, S. Kelley, P. Luke, W. T. Magand, O. Marumoto, K. Pfaffhuber, K. A. Ren, X. Sheu, G.-R. Slemr, F. Warneke, T. Weigelt, A. Weiss-Penzias, P. Wip, D. C. Zhang, Q. Song, Shaojie Selin, Noelle E Massachusetts Institute of Technology. Department of Earth, Atmospheric, and Planetary Sciences Massachusetts Institute of Technology. Engineering Systems Division Song, Shaojie Selin, Noelle Eckley We perform global-scale inverse modeling to constrain present-day atmospheric mercury emissions and relevant physiochemical parameters in the GEOS-Chem chemical transport model. We use Bayesian inversion methods combining simulations with GEOS-Chem and ground-based Hg[superscript 0] observations from regional monitoring networks and individual sites in recent years. Using optimized emissions/parameters, GEOS-Chem better reproduces these ground-based observations and also matches regional over-water Hg[superscript 0] and wet deposition measurements. The optimized global mercury emission to the atmosphere is ~ 5.8 Gg yr[superscript −1]. The ocean accounts for 3.2 Gg yr[superscript −1] (55% of the total), and the terrestrial ecosystem is neither a net source nor a net sink of Hg[superscript 0]. The optimized Asian anthropogenic emission of Hg[superscript 0] (gas elemental mercury) is 650–1770 Mg yr[superscript −1], higher than its bottom-up estimates (550–800 Mg yr[superscript −1]). The ocean parameter inversions suggest that dark oxidation of aqueous elemental mercury is faster, and less mercury is removed from the mixed layer through particle sinking, when compared with current simulations. Parameter changes affect the simulated global ocean mercury budget, particularly mass exchange between the mixed layer and subsurface waters. Based on our inversion results, we re-evaluate the long-term global biogeochemical cycle of mercury, and show that legacy mercury becomes more likely to reside in the terrestrial ecosystem than in the ocean. We estimate that primary anthropogenic mercury contributes up to 23 % of present-day atmospheric deposition. National Science Foundation (U.S.). Atmospheric Chemistry Program (1053648) 2015-08-19T17:34:01Z 2015-08-19T17:34:01Z 2015-06 2015-05 Article http://purl.org/eprint/type/JournalArticle 1680-7324 1680-7316 http://hdl.handle.net/1721.1/98104 Song, S., N. E. Selin, A. L. Soerensen, H. Angot, R. Artz, S. Brooks, E.-G. Brunke, et al. “Top-down Constraints on Atmospheric Mercury Emissions and Implications for Global Biogeochemical Cycling.” Atmos. Chem. Phys. 15, no. 12 (2015): 7103–7125. https://orcid.org/0000-0002-6396-5622 https://orcid.org/0000-0001-6395-7422 en_US http://dx.doi.org/10.5194/acp-15-7103-2015 Atmospheric Chemistry and Physics Creative Commons Attribution http://creativecommons.org/licenses/by/3.0/ application/pdf Copernicus GmbH Copernicus Publications |
| spellingShingle | Soerensen, A. L. Angot, H. Artz, R. Brooks, S. Brunke, E.-G. Conley, G. Dommergue, A. Ebinghaus, R. Holsen, T. M. Jaffe, D. A. Kang, S. Kelley, P. Luke, W. T. Magand, O. Marumoto, K. Pfaffhuber, K. A. Ren, X. Sheu, G.-R. Slemr, F. Warneke, T. Weigelt, A. Weiss-Penzias, P. Wip, D. C. Zhang, Q. Song, Shaojie Selin, Noelle E Top-down constraints on atmospheric mercury emissions and implications for global biogeochemical cycling |
| title | Top-down constraints on atmospheric mercury emissions and implications for global biogeochemical cycling |
| title_full | Top-down constraints on atmospheric mercury emissions and implications for global biogeochemical cycling |
| title_fullStr | Top-down constraints on atmospheric mercury emissions and implications for global biogeochemical cycling |
| title_full_unstemmed | Top-down constraints on atmospheric mercury emissions and implications for global biogeochemical cycling |
| title_short | Top-down constraints on atmospheric mercury emissions and implications for global biogeochemical cycling |
| title_sort | top down constraints on atmospheric mercury emissions and implications for global biogeochemical cycling |
| url | http://hdl.handle.net/1721.1/98104 https://orcid.org/0000-0002-6396-5622 https://orcid.org/0000-0001-6395-7422 |
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