The impact of anthropogenic emissions on atmospheric sulfate production pathways, oxidants, and ice core Δ 17 O(SO 4 2– )
We use a global three-dimensional chemical transport model to quantify the influence of anthropogenic emissions on atmospheric sulfate production mechanisms and oxidant concentrations constrained by observations of the oxygen isotopic composition (Δ 17 O = &delta 17 O–0.52 × &delta 18 O) of...
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ftdoajarticles:oai:doaj.org/article:afda79d225c0497697e19c1c1813110e 2023-05-15T13:53:56+02:00 The impact of anthropogenic emissions on atmospheric sulfate production pathways, oxidants, and ice core Δ 17 O(SO 4 2– ) S. A. Kunasek B. Alexander E. D. Sofen 2011-04-01T00:00:00Z https://doi.org/10.5194/acp-11-3565-2011 https://doaj.org/article/afda79d225c0497697e19c1c1813110e EN eng Copernicus Publications http://www.atmos-chem-phys.net/11/3565/2011/acp-11-3565-2011.pdf https://doaj.org/toc/1680-7316 https://doaj.org/toc/1680-7324 doi:10.5194/acp-11-3565-2011 1680-7316 1680-7324 https://doaj.org/article/afda79d225c0497697e19c1c1813110e Atmospheric Chemistry and Physics, Vol 11, Iss 7, Pp 3565-3578 (2011) Physics QC1-999 Chemistry QD1-999 article 2011 ftdoajarticles https://doi.org/10.5194/acp-11-3565-2011 2022-12-31T10:44:43Z We use a global three-dimensional chemical transport model to quantify the influence of anthropogenic emissions on atmospheric sulfate production mechanisms and oxidant concentrations constrained by observations of the oxygen isotopic composition (Δ 17 O = &delta 17 O–0.52 × &delta 18 O) of sulfate in Greenland and Antarctic ice cores and aerosols. The oxygen isotopic composition of non-sea salt sulfate (Δ 17 O(SO 4 2– )) is a function of the relative importance of each oxidant (e.g. O 3 , OH, H 2 O 2 , and O 2 ) during sulfate formation, and can be used to quantify sulfate production pathways. Due to its dependence on oxidant concentrations, Δ 17 O(SO 4 2– ) has been suggested as a proxy for paleo-oxidant levels. However, the oxygen isotopic composition of sulfate from both Greenland and Antarctic ice cores shows a trend opposite to that expected from the known increase in the concentration of tropospheric O 3 since the preindustrial period. The model simulates a significant increase in the fraction of sulfate formed via oxidation by O 2 catalyzed by transition metals in the present-day Northern Hemisphere troposphere (from 11% to 22%), offset by decreases in the fractions of sulfate formed by O 3 and H 2 O 2 . There is little change, globally, in the fraction of tropospheric sulfate produced by gas-phase oxidation (from 23% to 27%). The model-calculated change in Δ 17 O(SO 4 2– ) since preindustrial times (1850 CE) is consistent with Arctic and Antarctic observations. The model simulates a 42% increase in the concentration of global mean tropospheric O 3 , a 10% decrease in OH, and a 58% increase in H 2 O 2 between the preindustrial period and present. Model results indicate that the observed decrease in the Arctic Δ 17 O(SO 4 2– ) – in spite of increasing tropospheric O 3 concentrations – can be explained by the combined effects of increased sulfate formation by O 2 catalyzed by anthropogenic transition metals and increased cloud water acidity, rendering Δ 17 O(SO 4 2– ) insensitive to changing ... Article in Journal/Newspaper Antarc* Antarctic Arctic Greenland ice core Directory of Open Access Journals: DOAJ Articles Arctic Antarctic Greenland Atmospheric Chemistry and Physics 11 7 3565 3578 |
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Directory of Open Access Journals: DOAJ Articles |
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English |
topic |
Physics QC1-999 Chemistry QD1-999 |
spellingShingle |
Physics QC1-999 Chemistry QD1-999 S. A. Kunasek B. Alexander E. D. Sofen The impact of anthropogenic emissions on atmospheric sulfate production pathways, oxidants, and ice core Δ 17 O(SO 4 2– ) |
topic_facet |
Physics QC1-999 Chemistry QD1-999 |
description |
We use a global three-dimensional chemical transport model to quantify the influence of anthropogenic emissions on atmospheric sulfate production mechanisms and oxidant concentrations constrained by observations of the oxygen isotopic composition (Δ 17 O = &delta 17 O–0.52 × &delta 18 O) of sulfate in Greenland and Antarctic ice cores and aerosols. The oxygen isotopic composition of non-sea salt sulfate (Δ 17 O(SO 4 2– )) is a function of the relative importance of each oxidant (e.g. O 3 , OH, H 2 O 2 , and O 2 ) during sulfate formation, and can be used to quantify sulfate production pathways. Due to its dependence on oxidant concentrations, Δ 17 O(SO 4 2– ) has been suggested as a proxy for paleo-oxidant levels. However, the oxygen isotopic composition of sulfate from both Greenland and Antarctic ice cores shows a trend opposite to that expected from the known increase in the concentration of tropospheric O 3 since the preindustrial period. The model simulates a significant increase in the fraction of sulfate formed via oxidation by O 2 catalyzed by transition metals in the present-day Northern Hemisphere troposphere (from 11% to 22%), offset by decreases in the fractions of sulfate formed by O 3 and H 2 O 2 . There is little change, globally, in the fraction of tropospheric sulfate produced by gas-phase oxidation (from 23% to 27%). The model-calculated change in Δ 17 O(SO 4 2– ) since preindustrial times (1850 CE) is consistent with Arctic and Antarctic observations. The model simulates a 42% increase in the concentration of global mean tropospheric O 3 , a 10% decrease in OH, and a 58% increase in H 2 O 2 between the preindustrial period and present. Model results indicate that the observed decrease in the Arctic Δ 17 O(SO 4 2– ) – in spite of increasing tropospheric O 3 concentrations – can be explained by the combined effects of increased sulfate formation by O 2 catalyzed by anthropogenic transition metals and increased cloud water acidity, rendering Δ 17 O(SO 4 2– ) insensitive to changing ... |
format |
Article in Journal/Newspaper |
author |
S. A. Kunasek B. Alexander E. D. Sofen |
author_facet |
S. A. Kunasek B. Alexander E. D. Sofen |
author_sort |
S. A. Kunasek |
title |
The impact of anthropogenic emissions on atmospheric sulfate production pathways, oxidants, and ice core Δ 17 O(SO 4 2– ) |
title_short |
The impact of anthropogenic emissions on atmospheric sulfate production pathways, oxidants, and ice core Δ 17 O(SO 4 2– ) |
title_full |
The impact of anthropogenic emissions on atmospheric sulfate production pathways, oxidants, and ice core Δ 17 O(SO 4 2– ) |
title_fullStr |
The impact of anthropogenic emissions on atmospheric sulfate production pathways, oxidants, and ice core Δ 17 O(SO 4 2– ) |
title_full_unstemmed |
The impact of anthropogenic emissions on atmospheric sulfate production pathways, oxidants, and ice core Δ 17 O(SO 4 2– ) |
title_sort |
impact of anthropogenic emissions on atmospheric sulfate production pathways, oxidants, and ice core δ 17 o(so 4 2– ) |
publisher |
Copernicus Publications |
publishDate |
2011 |
url |
https://doi.org/10.5194/acp-11-3565-2011 https://doaj.org/article/afda79d225c0497697e19c1c1813110e |
geographic |
Arctic Antarctic Greenland |
geographic_facet |
Arctic Antarctic Greenland |
genre |
Antarc* Antarctic Arctic Greenland ice core |
genre_facet |
Antarc* Antarctic Arctic Greenland ice core |
op_source |
Atmospheric Chemistry and Physics, Vol 11, Iss 7, Pp 3565-3578 (2011) |
op_relation |
http://www.atmos-chem-phys.net/11/3565/2011/acp-11-3565-2011.pdf https://doaj.org/toc/1680-7316 https://doaj.org/toc/1680-7324 doi:10.5194/acp-11-3565-2011 1680-7316 1680-7324 https://doaj.org/article/afda79d225c0497697e19c1c1813110e |
op_doi |
https://doi.org/10.5194/acp-11-3565-2011 |
container_title |
Atmospheric Chemistry and Physics |
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11 |
container_issue |
7 |
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3565 |
op_container_end_page |
3578 |
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1766259411716669440 |