Seasonal air concentration variability, gas–particle partitioning, precipitation scavenging, and air–water equilibrium of organophosphate esters in southern Canada
<p>In response to increasing production and application volumes, organophosphate esters (OPEs) have emerged as pervasively detected contaminants in various environmental media, with concentrations often exceeding those of traditional organic contaminants. Despite the recognition of the atmosph...
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Copernicus Publications
2025-01-01
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| Series: | Atmospheric Chemistry and Physics |
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| author | Y. Li F. Zhan C. Shunthirasingham Y. D. Lei J. Oh J. Oh A. Ben Chaaben Z. Lu K. Lee F. A. P. C. Gobas H. Hung F. Wania F. Wania |
| author_facet | Y. Li F. Zhan C. Shunthirasingham Y. D. Lei J. Oh J. Oh A. Ben Chaaben Z. Lu K. Lee F. A. P. C. Gobas H. Hung F. Wania F. Wania |
| author_sort | Y. Li |
| collection | DOAJ |
| description | <p>In response to increasing production and application volumes, organophosphate esters (OPEs) have emerged as pervasively detected contaminants in various environmental media, with concentrations often exceeding those of traditional organic contaminants. Despite the recognition of the atmosphere's important role in dispersing OPEs and a substantial number of studies quantifying OPEs in air, investigations into atmospheric phase distribution processes are rare. Using measurements of OPEs in the atmospheric gas and particle phase, in precipitation, and in surface water collected in southern Canada, we explored the seasonal concentration variability, gas–particle partitioning behaviour, precipitation scavenging, and air–water equilibrium status of OPEs. Whereas consistent seasonal trends were not observed for OPE concentrations in precipitation or atmospheric particles, gas phase concentrations of several OPEs were elevated during the summer in suburban Toronto and at two remote sites on Canada's eastern and western coast. Apparent enthalpies of air–surface exchange fell mainly within or slightly above the range of air–water and air–octanol enthalpies of exchange, indicating the influence of local air–surface exchange processes and/or seasonally variable source strength. While many OPEs were present with a notable fraction in both the gas and particle phase, no clear relationship with compound volatility was apparent, although there was a tendency for higher particle-bound fractions at a lower temperature. High precipitation scavenging ratios for OPEs measured at the two coastal sites are consistent with low air–water partitioning ratios and the association with particles. Although beset by large uncertainties, air–water equilibrium calculations suggest net deposition of gaseous OPEs from the atmosphere to the Salish Sea and the St. Lawrence River and St. Lawrence Estuary. The measured seasonal concentration variability is likely less a reflection of temperature-driven air–surface exchange and instead indicates that more OPEs enter or are formed in the atmosphere in summer. More research is needed to better understand the atmospheric gas–particle partitioning behaviour of the OPEs and how it may be influenced by transformation reactions.</p> |
| format | Article |
| id | doaj-art-f8f2f8fe8ea34172a8041dcee1463e36 |
| institution | Kabale University |
| issn | 1680-7316 1680-7324 |
| language | English |
| publishDate | 2025-01-01 |
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| series | Atmospheric Chemistry and Physics |
| spelling | doaj-art-f8f2f8fe8ea34172a8041dcee1463e362025-01-15T10:33:10ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242025-01-012545947210.5194/acp-25-459-2025Seasonal air concentration variability, gas–particle partitioning, precipitation scavenging, and air–water equilibrium of organophosphate esters in southern CanadaY. Li0F. Zhan1C. Shunthirasingham2Y. D. Lei3J. Oh4J. Oh5A. Ben Chaaben6Z. Lu7K. Lee8F. A. P. C. Gobas9H. Hung10F. Wania11F. Wania12Department of Physical & Environmental Sciences, University of Toronto Scarborough, 1265 Military Trail, Toronto, Ontario, M1C 1A4, CanadaDepartment of Physical & Environmental Sciences, University of Toronto Scarborough, 1265 Military Trail, Toronto, Ontario, M1C 1A4, CanadaEnvironment and Climate Change Canada, Downsview, 4905 Dufferin St, North York, Ontario, M3H 5T4, CanadaDepartment of Physical & Environmental Sciences, University of Toronto Scarborough, 1265 Military Trail, Toronto, Ontario, M1C 1A4, CanadaDepartment of Physical & Environmental Sciences, University of Toronto Scarborough, 1265 Military Trail, Toronto, Ontario, M1C 1A4, CanadaDepartment of Chemistry, University of Toronto Scarborough, 1265 Military Trail, Toronto, Ontario, M1C 1A4, CanadaInstitut des Sciences de la Mer, Université du Québec à Rimouski, 300 allée des Ursulines, Rimouski, Quebec, G5L 3A1, CanadaInstitut des Sciences de la Mer, Université du Québec à Rimouski, 300 allée des Ursulines, Rimouski, Quebec, G5L 3A1, CanadaSchool of Resource and Environmental Management, Simon Fraser University, 8888 University Dr, Burnaby, British Columbia, V5A 1S6, CanadaSchool of Resource and Environmental Management, Simon Fraser University, 8888 University Dr, Burnaby, British Columbia, V5A 1S6, CanadaEnvironment and Climate Change Canada, Downsview, 4905 Dufferin St, North York, Ontario, M3H 5T4, CanadaDepartment of Physical & Environmental Sciences, University of Toronto Scarborough, 1265 Military Trail, Toronto, Ontario, M1C 1A4, CanadaDepartment of Chemistry, University of Toronto Scarborough, 1265 Military Trail, Toronto, Ontario, M1C 1A4, Canada<p>In response to increasing production and application volumes, organophosphate esters (OPEs) have emerged as pervasively detected contaminants in various environmental media, with concentrations often exceeding those of traditional organic contaminants. Despite the recognition of the atmosphere's important role in dispersing OPEs and a substantial number of studies quantifying OPEs in air, investigations into atmospheric phase distribution processes are rare. Using measurements of OPEs in the atmospheric gas and particle phase, in precipitation, and in surface water collected in southern Canada, we explored the seasonal concentration variability, gas–particle partitioning behaviour, precipitation scavenging, and air–water equilibrium status of OPEs. Whereas consistent seasonal trends were not observed for OPE concentrations in precipitation or atmospheric particles, gas phase concentrations of several OPEs were elevated during the summer in suburban Toronto and at two remote sites on Canada's eastern and western coast. Apparent enthalpies of air–surface exchange fell mainly within or slightly above the range of air–water and air–octanol enthalpies of exchange, indicating the influence of local air–surface exchange processes and/or seasonally variable source strength. While many OPEs were present with a notable fraction in both the gas and particle phase, no clear relationship with compound volatility was apparent, although there was a tendency for higher particle-bound fractions at a lower temperature. High precipitation scavenging ratios for OPEs measured at the two coastal sites are consistent with low air–water partitioning ratios and the association with particles. Although beset by large uncertainties, air–water equilibrium calculations suggest net deposition of gaseous OPEs from the atmosphere to the Salish Sea and the St. Lawrence River and St. Lawrence Estuary. The measured seasonal concentration variability is likely less a reflection of temperature-driven air–surface exchange and instead indicates that more OPEs enter or are formed in the atmosphere in summer. More research is needed to better understand the atmospheric gas–particle partitioning behaviour of the OPEs and how it may be influenced by transformation reactions.</p>https://acp.copernicus.org/articles/25/459/2025/acp-25-459-2025.pdf |
| spellingShingle | Y. Li F. Zhan C. Shunthirasingham Y. D. Lei J. Oh J. Oh A. Ben Chaaben Z. Lu K. Lee F. A. P. C. Gobas H. Hung F. Wania F. Wania Seasonal air concentration variability, gas–particle partitioning, precipitation scavenging, and air–water equilibrium of organophosphate esters in southern Canada Atmospheric Chemistry and Physics |
| title | Seasonal air concentration variability, gas–particle partitioning, precipitation scavenging, and air–water equilibrium of organophosphate esters in southern Canada |
| title_full | Seasonal air concentration variability, gas–particle partitioning, precipitation scavenging, and air–water equilibrium of organophosphate esters in southern Canada |
| title_fullStr | Seasonal air concentration variability, gas–particle partitioning, precipitation scavenging, and air–water equilibrium of organophosphate esters in southern Canada |
| title_full_unstemmed | Seasonal air concentration variability, gas–particle partitioning, precipitation scavenging, and air–water equilibrium of organophosphate esters in southern Canada |
| title_short | Seasonal air concentration variability, gas–particle partitioning, precipitation scavenging, and air–water equilibrium of organophosphate esters in southern Canada |
| title_sort | seasonal air concentration variability gas particle partitioning precipitation scavenging and air water equilibrium of organophosphate esters in southern canada |
| url | https://acp.copernicus.org/articles/25/459/2025/acp-25-459-2025.pdf |
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