Spatial and temporal changes of TBT pollution along the Portuguese coast: inefficacy of the EEC directive 89/677

Nucella lapillus imposex (superimposition of male characters onto prosobranch females) and organotin body burden were surveyed in the Portuguese coast in 1997 and 2000. Time comparisons of the available data on Nucella lapillus imposex in the Portuguese coast indicate a global increase of TBT pollution in recent years, revealing the inefficacy of the 1993 legislation that bans the use of TBT paints on small boats (<25 m). The absence or scarcity of the species inside harbours, which are the most polluted sites in Portugal, is probably a consequence of extinction due to female sterilisation by TBT.     

Organotin compounds in seawater and Mytilus galloprovincialis mussels along the Croatian Adriatic Coast

In this work, data on the level of organotin compounds (OTCs) in seawater and mussels collected along the entire Croatian Adriatic Coast are presented. The samples were collected in 2009 and 2010 at 48 locations representing different levels of maritime activities, including marinas, ports and reference sites. Butyltins (BuTs) were found in all analyzed samples, representing >97% of OTCs, and ranged from 0.46 to 27.98 ng Sn L(-1) in seawater and from <6 to 1675 ng Sn g(-1) in mussels. The results indicate a recent input of TBT, with the highest concentrations of BuTs found in the marinas. It appears that the Adriatic coast is still polluted with TBT despite the fact that TBT-containing antifouling paints have been banned in Croatia since 2008. It is questionable how much TBT pollution decreased since 2005, when a high incidence of imposex was established in the same area.     

Inshore/offshore gradients of imposex and organotin contamination in Nassarius reticulatus (L.) along the Portuguese coast

Imposex and organotin (OT) tissue contamination of the netted whelk Nassarius reticulatus (L.) were assessed in the continental shelves around the main estuaries of the central coast of Portugal (Lisbon: Tagus estuary; Setúbal: Sado estuary) and the main coastal lagoon in the Southern of Portugal (Faro: Ria Formosa). Pollution levels were higher in areas of more intense boat traffic and shipyard activities and imposex showed a clear decreasing gradient from the estuaries to the offshore, in relation to a similar gradient of tissue contamination by tributyltin. Remarkably, imposex was extensively spread over the adjacent continental shelves of Tagus and Sado estuaries. The current work shows that TBT pollution is undoubtedly a matter of concern not only for the above estuaries where harbours are implanted but also for the adjacent continental shelves, regardless the massive dilution of contaminants that may occur in these deeper areas.     

Imposex in the indigenous Nassarius kraussianus (Mollusca: Neogastropoda) from South African harbours

Nassarius kraussianus populations in the Durban and Richards Bay harbours (along the eastern seaboard of southern Africa) and in the Knysna lagoon (southern Cape coast) showed imposex development, confirming bioavailability of tributyltin (TBT) in these waterways. Incidence of imposex (which ranged from 29% to 100%) and relative penis length of females (RPL; which ranged from 1.3% to 55.2%) were markedly variable among populations from different sites in each waterway, indicative of localised effects of TBT contamination. Shell length of the snails was apparently not correlated with contamination level, as assessed from imposex measurements. While population imposex features are easy to determine and often provide a sensitive biomarker of TBT exposure, the discussion outlines reservations when extrapolating these to general ecological situations. Additionally, this study represents the first published report on the topic for sub-Saharan, African harbours, some of which seem remarkably less affected than suggested for other world regions.     

Imposex levels in the dogwhelk Nucella lapillus (L.)--continuing improvement at high latitudes

In 1990, restrictions on the use of tributyltin (TBT)-based antifouling paints were implemented in Iceland. A previous study showed that the level of imposex in the dogwhelk, Nucella lapillus, in Icelandic waters had decreased significantly between 1992 and 1998. In this study, we repeated the survey on imposex in N. lapillus at 33 locations from the Icelandic coast in 2003. The results indicated that both Vas Deferens Sequence Index (VDSI) and Relative Penis Size Index (RPSI) had further declined in 13 locations since 1998. Among these 13 sites, RPSI was reduced to zero in five cases. While improvements from 1992/1993 to 1998 were seen in reduced levels of imposex near both large and small harbours, the pattern from 1998 to 2003 was somewhat different, with improvement mainly observed near smaller harbours. No significant changes in imposex levels near larger harbours occurred over this period. Although the imposex levels still remain high near the large harbour complexes in Reykjavík and Hafnarfjörður, it is evident that regulations, including the use of less toxic antifouling paints and community action, have lead to substantial improvements in the marine environment of Iceland. International Maritime Organisation’s ban on the application of TBT after 2003 is apparently necessary to allow further improvements in larger harbours. The environmental effects of new antifoulants replacing TBT need to be further evaluated.     

A survey of imposex in muricids from 1996 to 2000 and identification of optimal indicators of tributyltin contamination along the east coast of Phuket Island,Thailand

The present investigation is the most extensive survey of imposex in gastropods from the west coast of Thailand. Imposex in Thais distinguenda increased significantly (p < 0.001; Chi Square test for trend) from 1996 to 2000 at 21 stations in Phangna Bay, Thailand. Females with imposex increased, extending from 3.5 km in 1996 to 10 km from the harbour areas in 1999 and 2000. Increasing intensity of imposex was also observed for Thais bitubercularis from 1996 to 2000. The less sensitive species: Morula musiva, Morula granulata, Morula margariticola and Thais rufotincta only developed imposex at the three main areas of intense shipping activities. T. bitubercularis and T. distinguenda are recommended as indicators of tributyltin (TBT) in Southeast Asia because of their sensitivity and wide distribution in the region. The results suggest that TBT contamination is worsening, against global trends, because regulations prohibiting the use of TBT-based paints, do not exist in Thailand.     

Incidence of imposex in thais orbita from Port Phillip Bay (Victoria, Australia), following 10 years of regulation on use of TBT.

Imposex, the phenomenon in which induced male sex characteristics are superimposed on normal females, still occurs widely in the gastropod Thais orbita from Port Philip Bay, and its incidence is greatest in areas that have high boating and shipping activities. Compared to 1992, both the extent and severity of imposex has reduced. By inference, this means that pollution by tributyltin (TBT) in Port Phillip Bay has decreased and that the bans limiting its use to vessels greater than 25 m in length, in place since 1989, have been effective. However, TBT pollution is still an issue at locations that are adjacent to major ports, such as the Port of Melbourne, where TBT from large ships and ship maintenance activities continues to pollute fish habitats. It is anticipated that the incidence of imposex, and therefore TBT pollution, will continue to decrease in Port Phillip Bay as long as the bans currently in place continue to be observed. If the trends observed in the present study continue, then it is unlikely, with the notable exception of commercial ports, that TBT will pose a threat to the health of fish habitats in Port Phillip Bay.     

TBT-pollution in the Gulf of Thailand: A re-inspection of imposex incidence after 10 years

Imposex in neogastropods was used to determine the relative TBT distribution in the Gulf of Thailand in 2006. To identify the imposex prevalence, 8757 specimens, belonging to 22 species from five families of neogastropods, were collected at 56 sites in 13 sample areas. These areas were located between the Bight of Bangkok in the north and the Malaysian border in the south. A contamination model was developed to compensate for differences in TBT sensitivity among species and to make comparisons among areas. At every area imposex was found in neogastropods. The highest incidence was in the east side of the Bight of Bangkok off Si Racha and Pattaya and in the southern part around Pattani. The same areas showed the highest frequency of imposex in 1996. While the frequency of imposex appeared to have slightly decreased in these areas, increases were found elsewhere. In Pattani Province this could be related to dumping of highly polluted harbour sediments in the shallow coastal area. The overall frequency of imposex in the Gulf of Thailand significantly increased from 1996 to 2006.     

Imposex levels in the dogwhelk Nucella lapillus (L.)—continuing improvement at high latitudes

In 1990, restrictions on the use of tributyltin (TBT)-based antifouling paints were implemented in Iceland. A previous study showed that the level of imposex in the dogwhelk, Nucella lapillus, in Icelandic waters had decreased significantly between 1992 and 1998. In this study, we repeated the survey on imposex in N. lapillus at 33 locations from the Icelandic coast in 2003. The results indicated that both Vas Deferens Sequence Index (VDSI) and Relative Penis Size Index (RPSI) had further declined in 13 locations since 1998. Among these 13 sites, RPSI was reduced to zero in five cases. While improvements from 1992/1993 to 1998 were seen in reduced levels of imposex near both large and small harbours, the pattern from 1998 to 2003 was somewhat different, with improvement mainly observed near smaller harbours. No significant changes in imposex levels near larger harbours occurred over this period. Although the imposex levels still remain high near the large harbour complexes in Reykjavík and Hafnarfjörður, it is evident that regulations, including the use of less toxic antifouling paints and community action, have lead to substantial improvements in the marine environment of Iceland. International Maritime Organisation’s ban on the application of TBT after 2003 is apparently necessary to allow further improvements in larger harbours. The environmental effects of new antifoulants replacing TBT need to be further evaluated.     

Imposex in Three Marine Gastropod Species in Chile and Potential Impact on Muriciculture

A survey of imposex was conducted between the Bay of San Vicente, Concepción, Chile (36° 50′) and the Bay of Renocavi, Puerto Montt, Chile (41° 35′), to determine if imposex is occurring in an area of collection and cultivation of the gastropod, Chorus giganteus. Imposex was recorded in three chilean muricids C. giganteus, Xanthochorus cassidiformis and Nucella crassilabrum complex. Percentage of imposex in females sampled ranged from 0% to 100%. The degree of expression of imposex was not so severe as to elicit sterility in the individuals surveyed. Incidence of imposex was as high as 47% in areas of harvest of C. giganteus for reproductive and cultivation studies for commercial production of this species. A six percent incidence of imposex was observed in Nucella proximal to the facility for cultivation of C. giganteus. Gastropods of the genus Nucella are used in other countries to monitor incidence of imposex and have demonstrated sensitivity toward tributyltin (TBT), the associated causal agent. Since sex of individuals in muriciculture is determined by the presence or absence of a penis, imposex may lead to erroneous classification of males and females. The incidence and severity of imposex in C. giganteus and related species may have a negative impact on sustainable cultivation and harvest of gastropods in Chile.     

Recovery from imposex by a population of the dogwhelk, Nucella lapillus (Gastropoda: Caenogastropoda), on the southeastern coast of England since May 2004: A 52-month study

Over a 52-month period beginning in May 2004 and concluding in August 2008, and coinciding with the period over which TBT was banned as a ship anti-foulant globally, a population of the dogwhelk, Nucella lapillus, was studied for changes in population size and structure, and reproduction. During the study period, the size of the population of N. lapillus on the Mewsbrook Groyne at Littlehampton on the southeastern coast of England grew from ∼25 individuals to >500, i.e., a 20-fold increase. Similarly, population structure normalised to reveal a maximum age of up to ∼3 years. The numbers of egg capsules produced by the N. lapillus population also grew over the study, again by a factor of 20, and the length of the breeding season increased from 7 months in 2004-2005 and 2005-2006 to 11 months in 2006-2007 and 2007-2008. Such changes were reflected in the incidence of imposex from Vas Deferens Index Stages 3 and 4 in 2003 to zero commencing in 2008 and continuing into 2009.Due to a lack of confirmatory chemical data, the changes in population size, structure and reproduction herein reported upon for N. lapillus cannot be correlated positively with changes in ambient TBT levels, but they can and are correlated with freedom from imposex. This is the first time such a dramatic recovery from imposex, following the banning of TBT, has been documented.     

Assessing the spatial variability,level and source of organic chemical contaminants in bivalve fishing grounds on the Galician coast (NW Spain)

Polychlorinated biphenyls, organochlorine pesticides, organotin compounds and triazines were quantified in sediments and bivalves collected in four areas on the Galician coast. One or several species were analysed at each site depending on their availability, including mussels (Mytilus galloprovincialis), cockles (Cerastoderma edule), clams (Venerupis pullastra and Ruditapes decussatus) and razor shells (Ensis siliqua). The general spatial distribution of contaminants was consistent in spite of the different sources of contamination. High inter-species variability was also observed. M. galloprovincialis and V. pullastra showed the highest levels of contaminants and intra-spatial variability, which highlights them as suitable species to be used as sentinel organisms. The area of O Burgo showed some worrisome results: PCB sediment concentrations were within the range that could cause biological effects. Also the level of heptachlor observed in V. pullastra was above limits accepted on edible seafood. Finally TBT concentration in mussels correlated with concentrations causing imposex in snails.     

Integrative assessment of organotin contamination in a southern European estuarine system (Ria de Aveiro, NW Portugal): tracking temporal trends in order to evaluate the effectiveness of the EU ban

Organotin (OT) compounds have been used as biocide agents in antifouling paints since the mid 1960s and are now ubiquitous in the marine environment. Due to their high toxicity to non-target species they were banned from antifouling paints in the European Union in 2003 (2002/62/EC directive). The aim of the present work is to assess any obvious decline of the OT environmental levels at Ria de Aveiro (NW Portugal) after the ban. The organotins - monobutyltin (MBT), dibutyltin (DBT), tributyltin (TBT), monophenyltin (MPT), diphenyltin (DPT), triphenyltin (TPT), monoctyltin (MOT), dioctyltin (DOT) and trioctyltin (TOT) - were quantified in the gastropod Nassarius reticulatus, in the mussel Mytilus galloprovincialis and in sediments. Imposex (imposition of male characters on females of gonochorist gastropods) in N. reticulatus was additionally used as a biomarker of TBT pollution. Time comparisons show a slight decrease of imposex between 2003 and 2005 probably as a consequence of the EU ban, though in some cases this trend seems to have started earlier since 2000. The fraction of TBT relatively to its metabolites has been decreasing over the last years but still remains high suggesting that there are still recent inputs of this compound into the study area.     

Imposex in Japanese gastropods (neogastropoda and mesogastropoda): Effects of tributyltin and triphenyltin from antifouling paints

In Japan, marine pollution by organotin compounds is serious and imposex is known to occur in marine gastropods. However, a detailed survey on imposex had not previously been conducted. The first country-wide survey and laboratory experiments on imposex in Japanese gastropods has now been carried out, and the results are reported herein.     

Tributyltin along the coasts of Corsica (Western Mediterranean): a persistent problem.

Despite optimistic forecasts by various scientists after regulatory measures were taken in the 1980s, coastal tributyltin (TBT) contamination is still a major problem. The present study concerning Corsica (Western Mediterranean) shows that contamination is not limited to harbour areas, but extends along the coast, involving protected nature reserves. The concentrations measured in harbours, which can reach 200 ng TBT l(-1), tend to incriminate both pleasure craft and ferries providing regular service between the island and the continent. Contamination as high as 7 ng TBT l(-1) has been measured in waters of the Scandola nature reserve, which is quite excessive given the no effect concentrations (NOEC) for marine fauna are around 1-2 ng TBT l(-1). The inadequacy of current regulations and their application are a major factor in this situation.     

The significance of imposex levels and TBT contamination in the red whelk, Neptunea antiqua (L.) from the offshore Irish Sea

The extent to which open seas and oceanic waters have been contaminated by TBT is unclear since most sampling programmes have concentrated on inshore areas, particularly near harbours. Accordingly, the red whelk, Neptunea antiqua L. (Mollusca: Prosobranchia), a sublittoral and dioecious prosobranch species, was selected to investigate the potential effects of TBT-induced imposex in the central western Irish Sea. The presence of imposex was noted in > 90% of all female whelks that were examined on a monthly basis over a 12-month period. However, the proliferation of the vas deferens was not considered severe enough to affect the reproductive capabilities of the population. Low concentrations of butyltins were detected in the soft tissues of all whelks examined, ranging from 0.009 to 0.112 microg g(-1) Sn dry wt There was no significant correlation between the documented imposex stages and total butyltin contamination, indicating that the species is not a reliable bioindicator species of the effects of this contaminant.     

Occurrence and effects of organotins on adult common whelk (Buccinum undatum) (Mollusca, Gastropoda) in harbours and in a simulated dredging situation.

Transplanted common whelk (Buccinum undatum) (Mollusca, Gastropoda) accumulated fairly high levels of organotins (tributyltin (TBT) and triphenyltin (TPT)) during exposure in three harbours with different TBT contamination. This did not though lead to an increase in imposex frequency in the adult females studied. Simulating harbour dredging in an experiment using suspended sediment from one of the harbours only resulted in a low concentration of TBT in the tissues of the common whelk and subsequently no changes in the occurrence and degree of imposex. The common whelk seemed to receive the main part of TBT from the water column and the limited bioaccumulation in the experiment indicates that desorption of TBT from the suspended sediment was slow. After TBT has been totally banned, dredging of contaminated sediments will cause increased exposure of the biota to TBT. Due to slow desorption the increase may however, be slight and temporary to pelagic and epibenthic species unless the settled particles are resuspended.     

Re-colonisation and recovery of populations of dogwhelks Nucella lapillus (L.) on shores formerly subject to severe TBT contamination

Dogwhelks Nucella lapillus became locally extinct on some shores adjacent to areas of high shipping/boating activity during the period of high tributyltin (TBT) contamination in the 1980s and early 1990s. However, the species has now re-colonised sites at which extinction occurred on the Isle of Cumbrae, the northeast coast of England, the Shetland Isles and southwest England. There have also been substantial declines in the severity of imposex on adjacent shores where the species has persisted during this period. Re-colonisation and recovery can be attributed to two measures: regulations prohibiting the use of TBT-based paints on vessels < 25 m in length and the development of slow-releasing, self-polishing copolymer paints. Nevertheless, the International Maritime Organisation has now imposed a total ban on the use of TBT-based paints as antifoulants. This is almost certain to result in the use of paints containing alternative biocides and there is widespread concern that there is relatively little information on which to assess their likely environmental impacts. They could cause substantial environmental damage.     

Distribution of Sargassum muticum on the North West coast of Spain: Relationships with urbanization and community diversity

Invasions are common in coastal marine environments where proximity to urban areas should influence the number of non-native organisms due to the likelihood of unintentional introductions from urban centers. Invasive species are widely recognised as important agents of global change, and can colonize new habitats and even cause local extinction of native species. This study was focused on the invasive marine macroalga Sargassum muticum, a problematic invasive species on the West coast of America and in European waters. An intensive survey was carried out along the Galician coast (North West of Spain) from March to August 2008 to determine the current distribution of this species, and its relationship with level of urbanization and native macroalgal diversity. We sampled the presence of S. muticum and native macroalgae in the mid and low intertidal zones of twenty rocky shores distributed along ten rias. Rias were grouped into high and scarcely urbanized based on their population density. Results indicated that S. muticum was present in nine out of the ten rias, confirming its presence in most of the intertidal rocky shores of Galicia twenty years after it was first observed. The presence of S. muticum was not related to the degree of urbanization of the rias, and its distribution and abundance did not seem to be influenced by diversity or functional groups of native algae. In addition, there was a great variability in the percentage cover, number and length of individuals amongst localities and rias suggesting that both large-scale and local processes may play a role in the distribution of this species. This study highlights the importance of future research into the distribution and impact of introduced algae and proves the urgent need for monitoring programmes and increasing efforts to prevent and control new introductions.     

Temporal and spatial distribution of floating objects in coastal waters of central–southern Chile and Patagonian fjords

Floating objects are suggested to be the principal vector for the transport and dispersal of marine invertebrates with direct development as well as catalysts for carbon and nutrient recycling in accumulation areas. The first step in identifying the ecological relevance of floating objects in a specific area is to identify their spatio-temporal distribution. We evaluated the composition, abundance, distribution, and temporal variability of floating objects along the continental coast of central–southern Chile (33–42°S) and the Patagonian fjords (42–50°S) using ship surveys conducted in austral winter (July/August) and spring (November) of the years 2002–2005 and 2008. Potential sources of floating items were identified with the aid of publicly available databases and scientific reports. We found three main types of floating objects, namely floating marine debris (mainly plastic objects and Styrofoam), wood (trunks and branches), and floating kelps (Macrocystis pyrifera and Durvillaea antarctica). Floating marine debris were abundant along most of the examined transects, with markedly lower abundances toward the southern fjord areas. Floating marine debris abundances generally corresponded to the distribution of human activities, and were highest in the Interior Sea of Chiloé, where aquaculture activities are intense. Floating wood appeared sporadically in the study area, often close to the main rivers. In accordance with seasonal river run-off, wood was more abundant along the continental coast in winter (rainy season) and in the Patagonian fjords during the spring surveys (snow melt). Densities of the two floating kelp species were similar along the continental coast, without a clear seasonal pattern. M. pyrifera densities increased towards the south, peaking in the Patagonian fjords, where it was dominant over D. antarctica. Densities of M. pyrifera in the Patagonian fjords were highest in spring. Correlation analyses between the abundances of floating objects and the distance to the nearest sources were generally non-significant, suggesting that post-supply processes affect the distribution of the floating objects in the study region. The identification of several major retention zones supports this idea. Accumulation areas of floating objects appear to be more common in the fjord zones. In general, the results underscore the abundance of floating objects throughout the study region and the fact that floating marine debris sources are mostly local, whereas floating algae may be dispersed over greater distances. Future studies should focus on the ecological role of floating objects in biota dispersal and nutrient cycling.