Passive water sampling and air–water diffusive exchange of long-range transported semi-volatile organic pollutants in high-mountain lakes
The concentrations of legacy and currently emitted organic pollutants were determined in the freely dissolved phase of water from six high-mountain lakes in the Pyrenees (1619–2453 m) by passive water sampling. Low-density polyethylene (LDPE) and silicone rubber (SR) sheets were exposed for three co...
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| Published in | The Science of the total environment Vol. 860; p. 160509 |
|---|---|
| Main Authors | , , , |
| Format | Journal Article |
| Language | English |
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Netherlands
Elsevier B.V
20.02.2023
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| Abstract | The concentrations of legacy and currently emitted organic pollutants were determined in the freely dissolved phase of water from six high-mountain lakes in the Pyrenees (1619–2453 m) by passive water sampling. Low-density polyethylene (LDPE) and silicone rubber (SR) sheets were exposed for three consecutive periods lasting each one year between 2017 and 2020 for the study of polychlorinated biphenyls (PCBs), organophosphate esters (OPEs), polycyclic aromatic hydrocarbons (PAHs), and other organochlorine compounds (e.g., hexachlorobenzene, HCB). HCB concentrations (1.0–14 pg L−1) remained essentially the same as those measured with pumping systems over two decades ago in the same area. ƩPAHs (35–920 pg L−1) were around half of those observed in the past, which agrees with reductions in European atmospheric emissions. ƩPCB concentrations (1.2–2.2 pg L−1) were substantially lower, although unexpectedly large differences could be due to comparing yearly averages from the present study to seasonally variable (i.e., affected by snowmelt, stratification, and colloidal organic matter) episodic pumping measurements from previous studies. ƩOPEs (139–2849 pg L−1) were measured for the first time in this area and were found at high concentrations in some sites. Concentrations of most compounds obtained with LDPE and SR samplers agreed with each other by ratios generally lower than three or four times, except for a few PAHs and OPEs. Diffusive exchange flux calculations between the atmospheric gas phase and the freely dissolved water phase revealed net deposition of pollutants from air to water, except for some OPEs and PCBs presenting equilibrium conditions, and HCB with volatilization fluxes. Atmospheric degradation fluxes of PAHs and OPEs pointed at competing removal mechanisms that support the air-to-water direction of their diffusive exchange, while PCBs and organochlorines were not affected by photodegradation. In their current state, these remote lakes accumulate many emerging and legacy pollutants subject to long-range atmospheric transport.
[Display omitted]
•LDPE and SR passive water samplers were used to analyze HOCs in high-mountain lakes.•PCB concentrations were lower than 20 years ago, while HCB remained the same.•PAH concentrations were reduced by half, as did atmospheric emissions in Europe.•OPEs were detected for the first time in these lakes at environmentally relevant levels.•Air–water diffusive fluxes revealed generalized deposition or near-equilibrium conditions. |
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| AbstractList | The concentrations of legacy and currently emitted organic pollutants were determined in the freely dissolved phase of water from six high-mountain lakes in the Pyrenees (1619-2453 m) by passive water sampling. Low-density polyethylene (LDPE) and silicone rubber (SR) sheets were exposed for three consecutive periods lasting each one year between 2017 and 2020 for the study of polychlorinated biphenyls (PCBs), organophosphate esters (OPEs), polycyclic aromatic hydrocarbons (PAHs), and other organochlorine compounds (e.g., hexachlorobenzene, HCB). HCB concentrations (1.0-14 pg L
) remained essentially the same as those measured with pumping systems over two decades ago in the same area. ƩPAHs (35-920 pg L
) were around half of those observed in the past, which agrees with reductions in European atmospheric emissions. ƩPCB concentrations (1.2-2.2 pg L
) were substantially lower, although unexpectedly large differences could be due to comparing yearly averages from the present study to seasonally variable (i.e., affected by snowmelt, stratification, and colloidal organic matter) episodic pumping measurements from previous studies. ƩOPEs (139-2849 pg L
) were measured for the first time in this area and were found at high concentrations in some sites. Concentrations of most compounds obtained with LDPE and SR samplers agreed with each other by ratios generally lower than three or four times, except for a few PAHs and OPEs. Diffusive exchange flux calculations between the atmospheric gas phase and the freely dissolved water phase revealed net deposition of pollutants from air to water, except for some OPEs and PCBs presenting equilibrium conditions, and HCB with volatilization fluxes. Atmospheric degradation fluxes of PAHs and OPEs pointed at competing removal mechanisms that support the air-to-water direction of their diffusive exchange, while PCBs and organochlorines were not affected by photodegradation. In their current state, these remote lakes accumulate many emerging and legacy pollutants subject to long-range atmospheric transport. The concentrations of legacy and currently emitted organic pollutants were determined in the freely dissolved phase of water from six high-mountain lakes in the Pyrenees (1619-2453 m) by passive water sampling. Low-density polyethylene (LDPE) and silicone rubber (SR) sheets were exposed for three consecutive periods lasting each one year between 2017 and 2020 for the study of polychlorinated biphenyls (PCBs), organophosphate esters (OPEs), polycyclic aromatic hydrocarbons (PAHs), and other organochlorine compounds (e.g., hexachlorobenzene, HCB). HCB concentrations (1.0-14 pg L-1) remained essentially the same as those measured with pumping systems over two decades ago in the same area. ƩPAHs (35-920 pg L-1) were around half of those observed in the past, which agrees with reductions in European atmospheric emissions. ƩPCB concentrations (1.2-2.2 pg L-1) were substantially lower, although unexpectedly large differences could be due to comparing yearly averages from the present study to seasonally variable (i.e., affected by snowmelt, stratification, and colloidal organic matter) episodic pumping measurements from previous studies. ƩOPEs (139-2849 pg L-1) were measured for the first time in this area and were found at high concentrations in some sites. Concentrations of most compounds obtained with LDPE and SR samplers agreed with each other by ratios generally lower than three or four times, except for a few PAHs and OPEs. Diffusive exchange flux calculations between the atmospheric gas phase and the freely dissolved water phase revealed net deposition of pollutants from air to water, except for some OPEs and PCBs presenting equilibrium conditions, and HCB with volatilization fluxes. Atmospheric degradation fluxes of PAHs and OPEs pointed at competing removal mechanisms that support the air-to-water direction of their diffusive exchange, while PCBs and organochlorines were not affected by photodegradation. In their current state, these remote lakes accumulate many emerging and legacy pollutants subject to long-range atmospheric transport.The concentrations of legacy and currently emitted organic pollutants were determined in the freely dissolved phase of water from six high-mountain lakes in the Pyrenees (1619-2453 m) by passive water sampling. Low-density polyethylene (LDPE) and silicone rubber (SR) sheets were exposed for three consecutive periods lasting each one year between 2017 and 2020 for the study of polychlorinated biphenyls (PCBs), organophosphate esters (OPEs), polycyclic aromatic hydrocarbons (PAHs), and other organochlorine compounds (e.g., hexachlorobenzene, HCB). HCB concentrations (1.0-14 pg L-1) remained essentially the same as those measured with pumping systems over two decades ago in the same area. ƩPAHs (35-920 pg L-1) were around half of those observed in the past, which agrees with reductions in European atmospheric emissions. ƩPCB concentrations (1.2-2.2 pg L-1) were substantially lower, although unexpectedly large differences could be due to comparing yearly averages from the present study to seasonally variable (i.e., affected by snowmelt, stratification, and colloidal organic matter) episodic pumping measurements from previous studies. ƩOPEs (139-2849 pg L-1) were measured for the first time in this area and were found at high concentrations in some sites. Concentrations of most compounds obtained with LDPE and SR samplers agreed with each other by ratios generally lower than three or four times, except for a few PAHs and OPEs. Diffusive exchange flux calculations between the atmospheric gas phase and the freely dissolved water phase revealed net deposition of pollutants from air to water, except for some OPEs and PCBs presenting equilibrium conditions, and HCB with volatilization fluxes. Atmospheric degradation fluxes of PAHs and OPEs pointed at competing removal mechanisms that support the air-to-water direction of their diffusive exchange, while PCBs and organochlorines were not affected by photodegradation. In their current state, these remote lakes accumulate many emerging and legacy pollutants subject to long-range atmospheric transport. The concentrations of legacy and currently emitted organic pollutants were determined in the freely dissolved phase of water from six high-mountain lakes in the Pyrenees (1619–2453 m) by passive water sampling. Low-density polyethylene (LDPE) and silicone rubber (SR) sheets were exposed for three consecutive periods lasting each one year between 2017 and 2020 for the study of polychlorinated biphenyls (PCBs), organophosphate esters (OPEs), polycyclic aromatic hydrocarbons (PAHs), and other organochlorine compounds (e.g., hexachlorobenzene, HCB). HCB concentrations (1.0–14 pg L⁻¹) remained essentially the same as those measured with pumping systems over two decades ago in the same area. ƩPAHs (35–920 pg L⁻¹) were around half of those observed in the past, which agrees with reductions in European atmospheric emissions. ƩPCB concentrations (1.2–2.2 pg L⁻¹) were substantially lower, although unexpectedly large differences could be due to comparing yearly averages from the present study to seasonally variable (i.e., affected by snowmelt, stratification, and colloidal organic matter) episodic pumping measurements from previous studies. ƩOPEs (139–2849 pg L⁻¹) were measured for the first time in this area and were found at high concentrations in some sites. Concentrations of most compounds obtained with LDPE and SR samplers agreed with each other by ratios generally lower than three or four times, except for a few PAHs and OPEs. Diffusive exchange flux calculations between the atmospheric gas phase and the freely dissolved water phase revealed net deposition of pollutants from air to water, except for some OPEs and PCBs presenting equilibrium conditions, and HCB with volatilization fluxes. Atmospheric degradation fluxes of PAHs and OPEs pointed at competing removal mechanisms that support the air-to-water direction of their diffusive exchange, while PCBs and organochlorines were not affected by photodegradation. In their current state, these remote lakes accumulate many emerging and legacy pollutants subject to long-range atmospheric transport. The concentrations of legacy and currently emitted organic pollutants were determined in the freely dissolved phase of water from six high-mountain lakes in the Pyrenees (1619–2453 m) by passive water sampling. Low-density polyethylene (LDPE) and silicone rubber (SR) sheets were exposed for three consecutive periods lasting each one year between 2017 and 2020 for the study of polychlorinated biphenyls (PCBs), organophosphate esters (OPEs), polycyclic aromatic hydrocarbons (PAHs), and other organochlorine compounds (e.g., hexachlorobenzene, HCB). HCB concentrations (1.0–14 pg L−1) remained essentially the same as those measured with pumping systems over two decades ago in the same area. ƩPAHs (35–920 pg L−1) were around half of those observed in the past, which agrees with reductions in European atmospheric emissions. ƩPCB concentrations (1.2–2.2 pg L−1) were substantially lower, although unexpectedly large differences could be due to comparing yearly averages from the present study to seasonally variable (i.e., affected by snowmelt, stratification, and colloidal organic matter) episodic pumping measurements from previous studies. ƩOPEs (139–2849 pg L−1) were measured for the first time in this area and were found at high concentrations in some sites. Concentrations of most compounds obtained with LDPE and SR samplers agreed with each other by ratios generally lower than three or four times, except for a few PAHs and OPEs. Diffusive exchange flux calculations between the atmospheric gas phase and the freely dissolved water phase revealed net deposition of pollutants from air to water, except for some OPEs and PCBs presenting equilibrium conditions, and HCB with volatilization fluxes. Atmospheric degradation fluxes of PAHs and OPEs pointed at competing removal mechanisms that support the air-to-water direction of their diffusive exchange, while PCBs and organochlorines were not affected by photodegradation. In their current state, these remote lakes accumulate many emerging and legacy pollutants subject to long-range atmospheric transport. [Display omitted] •LDPE and SR passive water samplers were used to analyze HOCs in high-mountain lakes.•PCB concentrations were lower than 20 years ago, while HCB remained the same.•PAH concentrations were reduced by half, as did atmospheric emissions in Europe.•OPEs were detected for the first time in these lakes at environmentally relevant levels.•Air–water diffusive fluxes revealed generalized deposition or near-equilibrium conditions. |
| ArticleNumber | 160509 |
| Author | van Drooge, Barend L. Grimalt, Joan O. Prats, Raimon M. Fernández, Pilar |
| Author_xml | – sequence: 1 givenname: Raimon M. surname: Prats fullname: Prats, Raimon M. email: raimon.martinez@idaea.csic.es – sequence: 2 givenname: Barend L. surname: van Drooge fullname: van Drooge, Barend L. – sequence: 3 givenname: Pilar surname: Fernández fullname: Fernández, Pilar – sequence: 4 givenname: Joan O. surname: Grimalt fullname: Grimalt, Joan O. |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/36436648$$D View this record in MEDLINE/PubMed |
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| CitedBy_id | crossref_primary_10_1021_acs_est_4c03099 crossref_primary_10_1016_j_scitotenv_2023_164566 crossref_primary_10_1016_j_clwat_2023_100002 crossref_primary_10_1016_j_enmm_2023_100888 crossref_primary_10_1016_j_scitotenv_2024_177981 crossref_primary_10_3390_app14177892 crossref_primary_10_3390_su17062493 crossref_primary_10_1021_acs_est_3c01866 crossref_primary_10_56530_lcgc_na_rn2885a5 |
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| Keywords | Organophosphate esters Polychlorinated biphenyls Polycyclic aromatic hydrocarbons Passive sampling Freely dissolved |
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| SubjectTerms | air Air Pollutants - analysis environment Environmental Monitoring Environmental Pollutants - analysis Freely dissolved hexachlorobenzene Hexachlorobenzene - analysis Hydrocarbons, Chlorinated Lakes organic matter Organophosphate esters organophosphorus compounds Passive sampling photolysis Polychlorinated biphenyls Polychlorinated Biphenyls - analysis Polycyclic aromatic hydrocarbons Polycyclic Aromatic Hydrocarbons - analysis Polyethylene rubber silicone snowmelt volatile organic compounds volatilization Water Water Pollutants, Chemical - analysis |
| Title | Passive water sampling and air–water diffusive exchange of long-range transported semi-volatile organic pollutants in high-mountain lakes |
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