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These processes may be responsible of the higher atmospheric concentrations over ocean than over land, but further research is needed on landocean interactions affecting persistent organic pollutants occurrence

Oceanic biogeochemical controls on global dynamics of persistent organic pollutants.

Environmental science & technology, no. 20 (2002): 4229-4237

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摘要

Understanding and quantifying the global dynamics and sinks of persistent organic pollutants (POPs) is important to assess their environmental impact and fate. Air-surface exchange processes, where temperature plays a central role in controlling volatilization and deposition, are of key importance in controlling global POP dynamics. The p...更多

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  • The long-range transport, persistence, and global dynamics of persistent organic pollutants (POPs) have been issues of increasing concern during the past decade, because they are key to understanding the potential impact of POPs on ecosystems, human health, and their ultimate fate [1,2,3,4,5,6,7,8,9].
  • The low concentrations of dissolved POPs in the mixed layer of high primary productivity regions are driven by enhanced sinking fluxes of particle associated POPs that cannot be supported by the air-water diffusive inputs from the atmosphere.
重点内容
  • The long-range transport, persistence, and global dynamics of persistent organic pollutants (POPs) have been issues of increasing concern during the past decade, because they are key to understanding the potential impact of POPs on ecosystems, human health, and their ultimate fate [1,2,3,4,5,6,7,8,9]
  • Experimental evidence for global fractionation and cold condensation has been observed in terrestrial and limnic systems but is scarce in the marine environment [6, 15, 16,17,18]. These limited data suggest that these processes may be of relatively minor importance, compared to other processes affecting the fate of POPs, such as sorption to organic matter, sequestration in deep waters, etc. [18,19,20]
  • The gas-phase polychlorinated biphenyls (PCBs) concentrations measured in the Atlantic ocean transect ranged from 54 to 1290 pg m-3 and averaged 501 pg m-3
  • Gas-phase concentrations measured over land may not be representative of what is occurring over the oceans since gas-phase concentrations are influenced by air-vegetation, air-soil, and air-water exchange [19, 31]
  • These processes may be responsible of the higher atmospheric concentrations over ocean than over land, but further research is needed on landocean interactions affecting POP occurrence
  • In upwelling regions where the dissolved phase of the mixed layer is depleted in POPs, enhanced sinking fluxes are observed, due to higher fluxes of organic matter driven by the higher primary productivity
结果
  • The predicted sinking fluxes, which are equal to the airwater exchange fluxes, due to the assumption of steadystate conditions, show the influence of the biogeochemical processes of phytoplankton uptake and sinking fluxes of particle associated POPs. In upwelling regions where the dissolved phase of the mixed layer is depleted in POPs, enhanced sinking fluxes are observed, due to higher fluxes of organic matter driven by the higher primary productivity.
  • For chemicals with low to moderate hydrophobicities, such as PCB52, air-water exchange is faster than sinking of particle associated POPs. the air-water exchange will keep surface water concentrations in conditions close to equilibrium with the atmospheric gas-phase, except in areas with very high primary productivity.
  • Airwater exchange is not fast enough to compensate the depletion of POPs in the surface mixed layer, due to vertical fluxes of particle-associated POPs. The analysis of fugacity ratios (Figure 5) show strong disequilibria at mid-high latitudes, due to depletion of water column concentrations.
  • The relative importance of air-water exchange and vertical fluxes as controlling processes of the global dynamics of POPs are, to a certain extent, independent of the magnitude of gas-phase concentrations of POPs. the rate-limiting process depends on the values of the mass transfer coefficients and the fugacity ratio can be derived from these mass transfer coefficients if steady state is assumed (Annex II).
结论
  • Biogeochemical processes and phytoplankton uptake and the subsequent sinking to deep waters play a major role determining air-water fluxes and the ultimate sink of POPs. For chemicals with low hydrophobicities, this is due to higher values of kADW, while for very hydrophobic chemicals, enhanced fluxes are found at mid-high latitudes due to depletion of water column concentrations and increased concentration gradients.
  • The present work suggests that the influence of biogeochemical processes controlling water column concentrations and vertical fluxes of particle associated POPs may be as important as temperature as factors driving the global fate, transport, and sinks of POPs. The authors thank Dr Watson Gregg (GSFC-NASA) for providing chlorophyll estimations from the SEAWIFFS satellite and Dr Rafel Simo (CMIMA-CSIC) for many insightful discussions and coordination of the AMIGOS project.
总结
  • The long-range transport, persistence, and global dynamics of persistent organic pollutants (POPs) have been issues of increasing concern during the past decade, because they are key to understanding the potential impact of POPs on ecosystems, human health, and their ultimate fate [1,2,3,4,5,6,7,8,9].
  • The low concentrations of dissolved POPs in the mixed layer of high primary productivity regions are driven by enhanced sinking fluxes of particle associated POPs that cannot be supported by the air-water diffusive inputs from the atmosphere.
  • The predicted sinking fluxes, which are equal to the airwater exchange fluxes, due to the assumption of steadystate conditions, show the influence of the biogeochemical processes of phytoplankton uptake and sinking fluxes of particle associated POPs. In upwelling regions where the dissolved phase of the mixed layer is depleted in POPs, enhanced sinking fluxes are observed, due to higher fluxes of organic matter driven by the higher primary productivity.
  • For chemicals with low to moderate hydrophobicities, such as PCB52, air-water exchange is faster than sinking of particle associated POPs. the air-water exchange will keep surface water concentrations in conditions close to equilibrium with the atmospheric gas-phase, except in areas with very high primary productivity.
  • Airwater exchange is not fast enough to compensate the depletion of POPs in the surface mixed layer, due to vertical fluxes of particle-associated POPs. The analysis of fugacity ratios (Figure 5) show strong disequilibria at mid-high latitudes, due to depletion of water column concentrations.
  • The relative importance of air-water exchange and vertical fluxes as controlling processes of the global dynamics of POPs are, to a certain extent, independent of the magnitude of gas-phase concentrations of POPs. the rate-limiting process depends on the values of the mass transfer coefficients and the fugacity ratio can be derived from these mass transfer coefficients if steady state is assumed (Annex II).
  • Biogeochemical processes and phytoplankton uptake and the subsequent sinking to deep waters play a major role determining air-water fluxes and the ultimate sink of POPs. For chemicals with low hydrophobicities, this is due to higher values of kADW, while for very hydrophobic chemicals, enhanced fluxes are found at mid-high latitudes due to depletion of water column concentrations and increased concentration gradients.
  • The present work suggests that the influence of biogeochemical processes controlling water column concentrations and vertical fluxes of particle associated POPs may be as important as temperature as factors driving the global fate, transport, and sinks of POPs. The authors thank Dr Watson Gregg (GSFC-NASA) for providing chlorophyll estimations from the SEAWIFFS satellite and Dr Rafel Simo (CMIMA-CSIC) for many insightful discussions and coordination of the AMIGOS project.
表格
  • Table1: Latitudinal Variability of Temperature (T), Wind Speed (U10), Chlorophyll Concentrations (Chl), Mixed Layer Depths (MLD), and Sinking Fluxes of Organic Carbon (FOC) during the Fall of 1998a
Download tables as Excel
基金
  • The modeling part of this work has been funded by the Spanish Ministry of Science and Technology through the AMIGOS project (REN2001-3462/CLI), while the field measurements were done as part of the GLOBALSOC project coordinated by Drs J
  • Broman (Stockholm University) with financial support from the European Union (ENV4 CT97 0638). Supporting Information Available The procedure to obtain eq 14 (Annex I) and the arithmetics leading to eq 17 (Annex II)
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