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Occurrence and environmental risk assessment of antifouling paint biocides from leisure boats
Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.ORCID iD: 0000-0002-7526-5295
2019 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The use of biocidal antifouling (AF) paints is the most common way to prevent fouling on leisure boat hulls. The main aim of this thesis was to investigate the pathways through which AF biocides, past and present, may reach the environment through their use on leisure boats and to improve the risk assessment of biocidal AF paints intended for amateur use. The work presented focuses mainly on the Baltic Sea, with emphasis on regulation and risk assessment procedures in Sweden. A new method was developed for the quantification of nowadays banned organotin compounds (OTCs) such as tributyltin (TBT) in paint flakes (paper I). OTCs were detected in hull paint scrapings from three countries around the Baltic Sea. Thus, historic layers of organotin paint on leisure boats may constitute as sources of TBT to the marine environment. Total tin was identified as an indicator for the presence of OTCs on boat hulls, allowing for quicker identification of vessels in need of remediation. Nowadays, most AF paints tend to contain high amounts of copper (Cu) and zinc (Zn). The use of AF paints was shown to cause exceedance of guideline values for these two metals in soil, sediment and water in various investigated marinas (papers II and IV). The pollution of boatyard soil was linked to hull maintenance activities carried out over unprotected ground (paper II). AF paints were also found to impact both the concentration and speciation of dissolved Cu and Zn in two Baltic Sea marinas, with increased concentrations as well as an increased proportion of bioavailable species as a function of an increased number of moored boats (paper IV). A new method utilizing X-Ray Fluorescence (XRF) was used to derive the release rates of Cu and Zn in the field for five commercially available AF paints for amateur use (paper III). Salinity and paint properties were found to be important parameters affecting the release. The in situ release rates were also found to exceed those derived with current standardized release rate methods. Given the high release rates, none of the studied paints should have been approved for the Swedish market. This finding likely explains the exceedance of guideline values for dissolved Cu and Zn in investigated Baltic Sea marinas (paper IV). In conclusion, there is a need for caution when authorizing new biocides as the phasing out of banned substances can be a lengthy process due to their continued presence in historic paint layers. Additionally, paint-specific release rates determined under conditions reflecting the intended use of the product should be used for a more realistic environmental risk assessment of AF paints.

Place, publisher, year, edition, pages
Stockholm: Department of Environmental Science and Analytical Chemistry, Stockholm University , 2019. , p. 49
Keywords [en]
Antifouling paint, XRF, leisure boat, recreational boating, copper, zinc, tributyltin, organotin compounds, risk assessment, biocide, metals, release rate
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
URN: urn:nbn:se:su:diva-167281ISBN: 978-91-7797-655-4 (print)ISBN: 978-91-7797-663-9 (electronic)OAI: oai:DiVA.org:su-167281DiVA, id: diva2:1298662
Public defence
2019-05-24, William-Olssonsalen, Geovetenskapens hus, Svante Arrhenius väg 14, Stockholm, 10:00 (English)
Opponent
Supervisors
Funder
BONUS - Science for a better future of the Baltic Sea regionSwedish Environmental Protection Agency
Note

At the time of the doctoral defense, the following paper was unpublished and had a status as follows: Paper 4: Manuscript.

Available from: 2019-04-29 Created: 2019-03-25 Last updated: 2019-05-23Bibliographically approved
List of papers
1. Total tin and organotin speciation in historic layers of antifouling paint on leisure boat hulls
Open this publication in new window or tab >>Total tin and organotin speciation in historic layers of antifouling paint on leisure boat hulls
2017 (English)In: Environmental Pollution, ISSN 0269-7491, E-ISSN 1873-6424, Vol. 220, p. 1333-1341Article in journal (Refereed) Published
Abstract [en]

Despite their ban on small vessels in 1989 in the EU, organotin compounds (OTCs) are still being released into the environment due to their presence in historic paint layers on leisure boats. 23 paint samples scraped from recreational boats from three countries around the Baltic Sea were analyzed for total tin (Sn) and OTCs. Two antifouling paint products were also subjected to the same analyses. A new method for the detection of Sn in paint flake samples was developed and found to yield more accurate results compared to four different acid digestion methods. A new method was also developed for the extraction of OTCs from ground paint flakes. This endeavor revealed that existing methods for organotin analysis of sediment may not have full recoveries of OTCs if paint flakes are present in the sample. The hull paint samples had Sn concentrations ranging from 25 to 18,000 mg/kg paint and results showed that tributyltin (TBT) was detected in all samples with concentrations as high as 4.7 g (as Sn)/kg paint. TBT was however not always the major OTC. Triphenyltin (TPhT) was abundant in many samples, especially in those originating from Finland. Several other compounds such as monobutyltin (MBT), dibutyltin (DBT), tetrabutyltin (TeBT), monophenyltin (MPhT) and diphenyltin (DPhT) were also detected. These could be the result of degradation occurring on the hull or of impurities in the paint products as they were also identified in the two analyzed paint products. A linear correlation (r(2) = 0.934) was found between the total tin content and the sum of all detected OTCs. The detection of tin can therefore be used to indicate the presence of OTCs on leisure boats. (C) 2016 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license.

Keywords
Organotin compounds, Tributyltin, Triphenyltin, Antifouling paint, Paint particles
National Category
Earth and Related Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-139376 (URN)10.1016/j.envpol.2016.11.001 (DOI)000390732300061 ()27836476 (PubMedID)
Available from: 2017-02-07 Created: 2017-02-06 Last updated: 2019-04-05Bibliographically approved
2. Metal contamination at recreational boatyards linked to the use of antifouling paints-investigation of soil and sediment with a field portable XRF
Open this publication in new window or tab >>Metal contamination at recreational boatyards linked to the use of antifouling paints-investigation of soil and sediment with a field portable XRF
2016 (English)In: Environmental science and pollution research international, ISSN 0944-1344, E-ISSN 1614-7499, Vol. 23, no 10, p. 10146-10157Article in journal (Refereed) Published
Abstract [en]

The application of a field portable X-ray fluorescence spectrometer (FPXRF) to measure Cu, Zn, and Pb in soil and sediments at recreational boatyards by Lake Malaren in Sweden was investigated. Confirmatory chemical analysis on freeze-dried samples shows that, ex situ, the FPXRF produces definitive level data for Cu and Zn and quantitative screening data for Pb, according to USEPA criteria for data quality. Good agreement was also found between the ex situ measurements and the in situ screening. At each of the two studied boatyards, >40 in situ soil measurements were carried out. Statistical differences in soil concentration based on land use were consequently found: the areas used for boat storage and maintenance were significantly higher in Cu and Zn than the areas used for car parking and transportation. The metal pollution in the boat storage areas is therefore shown to be directly linked to hull maintenance activities during which metal-containing antifouling paint particles are shed, end up on the ground, and consequently pollute the soil. In the boat storage areas, the Cu and Zn concentrations often exceeded the national guideline values for soil. In this study, they were also shown to increase with increasing age of the boatyard operation. Pb soil concentrations were only elevated at a few measurement points, reflecting the phasing out of Pb compounds from antifouling products over the past 2 decades. In the surface sediments, concentrations of Cu and Zn were 2-3 times higher compared to deeper levels. No decrease in metal concentration with time was found in the sediments, indicating that boat owners are not complying with the ban of biocide-containing paints in freshwater introduced over 20 years ago.

Keywords
Antifouling paint, Boatyard, Soil, Sediment, XRF, Cu, Zn, Pb
National Category
Earth and Related Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-131544 (URN)10.1007/s11356-016-6241-0 (DOI)000376421400085 ()26873824 (PubMedID)
Available from: 2016-06-30 Created: 2016-06-21 Last updated: 2019-04-05Bibliographically approved
3. In situ release rates of Cu and Zn from commercial antifouling paints at different salinities
Open this publication in new window or tab >>In situ release rates of Cu and Zn from commercial antifouling paints at different salinities
Show others...
2018 (English)In: Marine Pollution Bulletin, ISSN 0025-326X, E-ISSN 1879-3363, Vol. 127, p. 289-296Article in journal (Refereed) Published
Abstract [en]

Antifouling paints are environmentally risk assessed based on their biocidal release rates to the water phase. In situ release rates of copper (Cu) and zinc (Zn) were derived for five commercial paints in two recreational marinas with different salinities (5 and 14 PSU) using an X-Ray Fluorescence spectrometer (XRF). Salinity was found to significantly affect the Cu release, with twice the amount of Cu released at the higher salinity, while its influence on the Zn release was paint-specific. Site-specific release rates for water bodies with salinity gradients, e.g. the Baltic Sea, are therefore necessary for more realistic risk assessments of antifouling paints. Furthermore, the in situ release rates were up to 8 times higher than those generated using standardized laboratory or calculation methods. The environmental risk assessment repeated with the field release rates concludes that it is questionable whether the studied products should be allowed on the Swedish market.

Keywords
Antifouling paint, Copper, Zinc, Environmental risk assessment, XRF
National Category
Earth and Related Environmental Sciences Biological Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-156013 (URN)10.1016/j.marpolbul.2017.12.027 (DOI)000427332900033 ()29475665 (PubMedID)
Available from: 2018-05-08 Created: 2018-05-08 Last updated: 2019-04-05Bibliographically approved
4. Flawed risk assessment of antifouling paints leads to exceedance of guideline values in Baltic Sea marinas
Open this publication in new window or tab >>Flawed risk assessment of antifouling paints leads to exceedance of guideline values in Baltic Sea marinas
(English)Manuscript (preprint) (Other academic)
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-167288 (URN)
Available from: 2019-03-25 Created: 2019-03-25 Last updated: 2019-03-25Bibliographically approved

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