The partition of fluoranthene and pyrene between suspended particles and dissolved phase in the Humber Estuary: a study of the controlling factors

Particle–water interactions are one of the most important mechanisms controlling the distribution and movement of hydrophobic organic chemicals such as polycyclic aromatic hydrocarbons (PAHs) in aquatic environments (e.g. estuaries and oceans). To accurately predict the transport and fates of hydrop...

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Published inThe Science of the total environment Vol. 243; pp. 305 - 321
Main Authors Zhou, J.L, Fileman, T.W, Evans, S, Donkin, P, Readman, J.W, Mantoura, R.F.C, Rowland, S
Format Journal Article
LanguageEnglish
Published Elsevier B.V 15.12.1999
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ISSN0048-9697
1879-1026
DOI10.1016/S0048-9697(99)00404-0

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Abstract Particle–water interactions are one of the most important mechanisms controlling the distribution and movement of hydrophobic organic chemicals such as polycyclic aromatic hydrocarbons (PAHs) in aquatic environments (e.g. estuaries and oceans). To accurately predict the transport and fates of hydrophobic contaminants in estuarine and coastal marine environments, the partition coefficient ( K p) and organic carbon normalised partition coefficient ( K oc) are widely used in various biogeochemical models. Such partition coefficients may be calculated from the so-called linear free energy relationships between K p, K oc and more easily measured parameters such as the octanol-water partition coefficient ( K ow). However K p and K oc values measured for real environmental samples of water and particles obtained from seasonal field surveys in the Humber Estuary, UK deviated from such ideals. For example, K P values showed no correlation with the fraction organic carbon content of particles ( f oc) and instead of being constant, K oc, values varied with f oc. Both K p and K oc were 1–3 orders of magnitude higher than those predicted from the simple equilibrium–partitioning model, but were in good agreement with several other recently published field studies. To improve our understanding of PAH partitioning, the soot carbon (SC) content of particulate samples was measured so that the simple partition model can be extended to incorporate SC. The partition coefficients derived from the extended partition model are very close to the field K ps. The results suggest that PAHs associated with particles are in fact present in the form of soot and soot-like particles that are not subject to particle–water equilibrations. In other words, the PAHs on soot-like particles are extremely strongly bound and not influenced by further partitioning between the particles and water. However, there are still limitations with the extended partition model as it failed to simulate the field K oc values. No correlation was found between the partition coefficients and salinity, which again we attribute to the non-equilibrium nature of the PAHs. However both K p and K oc generally decreased with increasing suspended solids concentrations (SSC) in the estuary. Such a relationship is probably due to the mixing of soot-like permanently suspended particles with resuspended estuarine sedimentary particles at the higher SSC values, and to the increased concentrations of dissolved organic carbon (DOC) associated with increase in SSC. However, it has been shown that DOC concentrations are not a suitable tool for correcting the SSC effect. There is therefore an urgent need to harmonise the laboratory and field approaches for K p measurements.
AbstractList Particle-water interactions predicting the transport and fates of hydrophobic contaminants rely on partition coefficient (K p), the organic carbon normalized partition coefficient (K oc) and the octanol-water partition coefficient (K ow). Values for real environment samples of water and particles obtained from field surveys in the Humber estuary deviated from predictions. To improve the understanding of partitioning this study measured the soot carbon (SC) content of particulate samples to extend the simple partition model. Partition coefficients from this new model very closely fitted field values resulting in the suggestion that PAH associated with particles were present in the form of soot-like particles that were not subject to particle-water equilibrations. PAH were extremely strongly bound and not influenced by further partitioning. No correlation was found between the partition coefficients and salinity. K p and K oc generally decreased with increasing suspended solids concentrations in the estuary.
Particle–water interactions are one of the most important mechanisms controlling the distribution and movement of hydrophobic organic chemicals such as polycyclic aromatic hydrocarbons (PAHs) in aquatic environments (e.g. estuaries and oceans). To accurately predict the transport and fates of hydrophobic contaminants in estuarine and coastal marine environments, the partition coefficient ( K p) and organic carbon normalised partition coefficient ( K oc) are widely used in various biogeochemical models. Such partition coefficients may be calculated from the so-called linear free energy relationships between K p, K oc and more easily measured parameters such as the octanol-water partition coefficient ( K ow). However K p and K oc values measured for real environmental samples of water and particles obtained from seasonal field surveys in the Humber Estuary, UK deviated from such ideals. For example, K P values showed no correlation with the fraction organic carbon content of particles ( f oc) and instead of being constant, K oc, values varied with f oc. Both K p and K oc were 1–3 orders of magnitude higher than those predicted from the simple equilibrium–partitioning model, but were in good agreement with several other recently published field studies. To improve our understanding of PAH partitioning, the soot carbon (SC) content of particulate samples was measured so that the simple partition model can be extended to incorporate SC. The partition coefficients derived from the extended partition model are very close to the field K ps. The results suggest that PAHs associated with particles are in fact present in the form of soot and soot-like particles that are not subject to particle–water equilibrations. In other words, the PAHs on soot-like particles are extremely strongly bound and not influenced by further partitioning between the particles and water. However, there are still limitations with the extended partition model as it failed to simulate the field K oc values. No correlation was found between the partition coefficients and salinity, which again we attribute to the non-equilibrium nature of the PAHs. However both K p and K oc generally decreased with increasing suspended solids concentrations (SSC) in the estuary. Such a relationship is probably due to the mixing of soot-like permanently suspended particles with resuspended estuarine sedimentary particles at the higher SSC values, and to the increased concentrations of dissolved organic carbon (DOC) associated with increase in SSC. However, it has been shown that DOC concentrations are not a suitable tool for correcting the SSC effect. There is therefore an urgent need to harmonise the laboratory and field approaches for K p measurements.
Particle-water interactions are one of the most important mechanisms controlling the distribution and movement of hydrophobic organic chemicals such as polycyclic aromatic hydrocarbons (PAHs) in aquatic environments (e.g. estuaries and oceans). To accurately predict the transport and fates of hydrophobic contaminants in estuarine and coastal marine environments, the partition coefficient (K sub(p)) and organic carbon normalised partition coefficient (K sub(oc)) are widely used in various biogeochemical models. Such partition coefficients may be calculated from the so-called linear free energy relationships between K sub(p), K sub(oc) and more easily measured parameters such as the octanol-water partition coefficient (K sub(ow)). However K sub(p) and K sub(oc) values measured for real environmental samples of water and particles obtained from seasonal field surveys in the Humber Estuary, UK deviated from such ideals. For example, K sub(p) values showed no correlation with the fraction organic carbon content of particles (f sub(oc)) and instead of being constant, K sub(oc), values varied with f sub(oc). Both K sub(p) and K sub(oc) were 1-3 orders of magnitude higher than those predicted from the simple equilibrium-partitioning model, but were in good agreement with several other recently published field studies. To improve our understanding of PAH partitioning, the soot carbon (SC) content of particulate samples was measured so that the simple partition model can be extended to incorporate SC. The partition coefficients derived from the extended partition model are very close to the field K sub(p)s. The results suggest that PAHs associated with particles are in fact present in the form of soot and soot-like particles that are not subject to particle-water equilibrations. In other words, the PAHs on soot-like particles are extremely strongly bound and not influenced by further partitioning between the particles and water. However, there are still limitations with the extended partition model as it failed to simulate the field K sub(oc) values. No correlation was found between the partition coefficients and salinity, which again we attribute to the non-equilibrium nature of the PAHs. However both K sub(p) and K sub(oc) generally decreased with increasing suspended solids concentrations (SSC) in the estuary. Such a relationship is probably due to the mixing of soot-like permanently suspended particles with resuspended estuarine sedimentary particles at the higher SSC values, and to the increased concentrations of dissolved organic carbon (DOC) associated with increase in SSC. However, it has been shown that DOC concentrations are not a suitable tool for correcting the SSC effect. There is therefore an urgent need to harmonise the laboratory and field approaches for K sub(p) measurements.
Author Donkin, P
Fileman, T.W
Evans, S
Readman, J.W
Rowland, S
Mantoura, R.F.C
Zhou, J.L
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Snippet Particle–water interactions are one of the most important mechanisms controlling the distribution and movement of hydrophobic organic chemicals such as...
Particle-water interactions are one of the most important mechanisms controlling the distribution and movement of hydrophobic organic chemicals such as...
Particle-water interactions predicting the transport and fates of hydrophobic contaminants rely on partition coefficient (K p), the organic carbon normalized...
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StartPage 305
SubjectTerms Brackish
British Isles, England, Humber Estuary
Estuaries
fluoranthene
hydrophobic compounds
PAHs
Partition coefficient
pyrene
Soot
Suspended particulate matter
Title The partition of fluoranthene and pyrene between suspended particles and dissolved phase in the Humber Estuary: a study of the controlling factors
URI https://dx.doi.org/10.1016/S0048-9697(99)00404-0
https://www.proquest.com/docview/17479783
https://www.proquest.com/docview/17679290
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