Shellfish and residual chemical contaminants: hazards, monitoring, and health risk assessment along French coasts.

In this review, we address the identification of residual chemical hazards in shellfish collected from the marine environment or in marketed shellfish. Data, assembled on the concentration of contaminants detected, were compared with the appropriate regulatory and food safety standards. Moreover, data on human exposure and body burden levels were evaluated in the context of potential health risks.Shellfish farming is a common industry along European coasts. The primary types of shellfish consumed in France are oysters, mussels, king scallops, winkles,whelks, cockles, clams, and other scallops. Shellfish filter large volumes of water to extract their food and are excellent bioaccumulators. Metals and other pollutants that exist in the marine environment partition into particular organs, according to their individual chemical characteristics. In shellfish, accumulation often occurs in the digestive gland, which plays a role in assimilation, excretion, and detoxification of contaminants. The concentrations of chemical contaminants in bivalve mollusks are known to fluctuate with the seasons.European regulations limit the amount and type of contaminants that can appear in foodstuffs. Current European standards regulate the levels of micro-biological agents, phycotoxins, and some chemical contaminants in food. Since 2006, these regulations have been compiled into the "Hygiene Package." Bivalve mollusks must comply with maximum levels of certain contaminants as follows:lead (1.5 mg kg-1), cadmium (1 mg kg-1), mercury (0.5 mg kg-1), dioxins (4 pg g-1 and dioxins + DL-PCBs 8 pg g-1), and benzo[a]pyrene (10 µp.g kg-1).In this review, we identify the levels of major contaminants that exist in shellfish(collected from the marine environment and/or in marketed shellfish). The follow-ing contaminants are among those that are profiled: Cd, Pb, Hg, As, Ni, Cr, V,Mn, Cu, Zn, Co, Se, Mg, Mo, radionuclides, benzo[a]pyrene, PCBs, dioxins and furans, PAHs, TBT, HCB, dieldrin, DDT, lindane, triazines, PBDE, and chlorinated paraffins.In France, the results of contaminant monitoring have indicated that Cd, but not lead (< 0.26 mg kg-1) or mercury (< 0.003 mg kg-1), has had some non-compliances. Detections for PCBs and dioxins in shellfish were far below the regulatory thresholds in oysters (< 0.6 pg g-l), mussels (< 0.6 pg g-1), and king scallops (< 0.4 pg g-1). The benzo[a]pyrene concentration in marketed mussels and farmed shellfish does not exceed the regulatory threshold. Some monitoring data are available on shellfish flesh contamination for unregulated organic contaminants.Of about 100 existing organo stannic compounds, residues of the mono-, di-, and tributyltin (MBT, DBT, and TBT) and mono-, di-, and triphenyltin (MPT, DPT,and TPT) compounds are the most frequently detected in fishery products. Octyltins are not found in fishery products. Some bivalve mollusks show arsenic levels up to 15.8 mg kg-1. It seems that the levels of arsenic in the environment derive less from bioaccumulation, than from whether the arsenic is in an organic or an inorganic form. In regard to the other metals, levels of zinc and magnesium are higher in oysters than in mussels.To protect shellfish from chemical contamination, programs have been established to monitor water masses along coastal areas. The French monitoring network(ROCCH) focuses on environmental matrices that accumulate contaminants. These include both biota and sediment. Example contaminants were studied in a French coastal lagoon (Arcachon Bay) and in an estuary (Bay of Seine), and these were used to illustrate the usefulness of the monitoring programs. Twenty-one pesticidal and biocidal active substances were detected in the waters of Arcachon Bay during the summers from 1999 to 2003, at concentrations ranging from a few nanograms per liter to several hundred nanograms per liter. Most of the detected substances were herbicides, including some that are now banned. Organotin compounds have been detected in similarly semi-enclosed waters elsewhere (bays, estuaries, and harbors).However, the mean concentrations of cadmium, mercury, lead, and benzo[a]pyrene,in transplanted mussels, were below the regulatory limits.In 2007, the mean daily consumption of shellfish in the general French population was estimated to be 4.5 g in adults; however, a wide variation occurs by region and season (INCA 2 study). Tabulated as a proportion of the diet, shellfish consumption represents only 0.16% of overall solid food intake. However, the INCA 2 survey was not well suited to estimating shellfish consumption because of the small number of shellfish consumers sampled. In contrast, the mean consumption rate of bivalve mollusks among adult high consumers of fish and seafood products, i.e., adults who eat fish or seafood at least twice a week, was estimated to be 153 g week-1 (8 kg yr-1). The highest mean consumption is for king scallops (39 g week-1), followed by oysters (34 g week-1) and mussels (22 g week-1). Thus, for high seafood consumers, the contribution of shellfish to inorganic contaminant levels is 1-10% TWI or PTWI for Cd, MeHg, and Sn (up to 19% for Sn), and the arsenic body burden is higher for 22% of individuals studied.The human health risks associated with consuming chemical contaminants in shellfish are difficult to assess for several reasons: effects may only surface after long-term exposure (chronic risk), exposures may be discontinuous, and contamination may derive from multiple sources (food, air, occupational exposure, etc.).Therefore, it is not possible to attribute a high body burden specifically to shellfish consumption even if seafood is a major dietary contributor of any contaminant, e.g.,arsenic and mercury.The data assembled in this review provide the arguments for maintaining the chemical contaminant monitoring programs for shellfish. Moreover, the results presented herein suggest that monitoring programs should be extended to other chemicals that are suspected of presenting a risk to consumers, as illustrated by the high concentration reported for arsenic (in urine) of high consumers of seafood products from the CALIPSO study. In addition, the research conducted in shellfish-farming areas of Arcachon Bay highlights the need to monitor TBT and PAH contamination levels to ensure that these chemical pollutants do not migrate from the harbor to oyster farms.Finally, we have concluded that shellfish contamination from seawater offers a rather low risk to the general French population, because shellfish do not constitute a major contributor to dietary exposure of chemical contaminants. Notwithstanding,consumer vigilance is necessary among regular shellfish consumers, and especially for those residing in fishing communities, for pregnant and breast-feeding women,and for very young children.

Seasonal and decadal variations in lead sources to eastern North Atlantic mussels.

The concentration of Pb and its stable isotope composition were measured in 216 composite samples of 50 blue mussels (Mytilus edulis (M. edulis)) collected quarterly between 1985 and 2005 at three sites along the French Atlantic coast, one in the La Fresnaye Bay and the others in the Loire and Seine River estuaries. Depending on the sites and time periods, Pb concentrations were 5-66 times higher than the natural background value for the North Atlantic. Even for the samples with the lowest Pb concentrations, the isotopic signature of Pb is very different than that of the regional natural Pb, suggesting that most of the bioaccumulated Pb is anthropogenic in origin. Stable Pb isotope ratios measured in the mussels differ markedly from that of Pb emitted in Western Europe as a result of leaded gasoline combustion, which was still a dominant source of contaminant Pb to the atmosphere during most of our study period. The isotope composition of Pb in the mussels was instead more typical of that of the Pb released to the environment by wastewater treatment plants, municipal waste incinerators, and industries such as metal refineries and smelters. Continental runoff, rather than atmospheric deposition, is therefore identified as the leading transport pathway of Pb along the French Atlantic coast. From the strong seasonal variations in (206)Pb/(208)Pb ratios in the mussels from the Seine Estuary site we also conclude that the resuspension of contaminated sediments, triggered by high river runoff events, is a chief factor affecting the bioaccumulation of Pb in M. edulis . The value of this organism as a biomonitor of coastal contamination is thus further demonstrated.

Comparison of polycyclic aromatic hydrocarbon levels in mussels and oysters in France and the United States.

This paper compares data of 15 individual polycyclic aromatic hydrocarbon (PAH) concentrations from two monitoring programs: the French Rdseau National d'Observation de la qualité du milieu marin (RNO) and the Mussel Watch project of the U.S. National Status and Trends (NST) program. Polycyclic aromatic hydrocarbon measurements in bivalve (mussels and oysters) are made from samples collected at 265 sites along the U.S. coastline and at 97 sites in the French coastal waters. Individual PAH patterns were found strikingly similar between the two countries with higher concentrations for high-molecular-weight (HMW) PAHs. Principal component analysis results for both RNO and NST show the variability to be dominated by just two components with HMW compounds contributing primarily to the first and low-molecular-weight (LMW) compounds to the second. This could imply a separation of petrogenic and pyrolytic sources with the latter being the more important in both nations accounting for the similarity in results.