Mussel Watch Research Articles

Toxicokinetics and Mussel Watch: Addressing Interspecies Differences for Coastal Cadmium Contamination Assessment.

Bivalves are often employed for biomonitoring contaminants in marine environments; however, in these large-scale programs, unavoidably, using multiple species presents a significant challenge. Interspecies differences in contaminant bioaccumulation can complicate data interpretation, and direct comparisons among species may result in misleading conclusions. Here, we propose a robust framework based on toxicokinetic measurements that accounts for interspecies differences in bioaccumulation. Specifically, via a recently developed double stable isotope tracer technique, we determined the toxicokinetics of cadmium (Cd)─a metal known for its high concentrations in bivalves and significant interspecies bioaccumulation variability─in six widespread bivalve species including mussels (Perna viridis, Mytilus unguiculatus, Mytilus galloprovincialis) and oysters (Magallana gigas, Magallana hongkongensis, Magallana angulata). Results show that oysters generally have higher Cd uptake rate constants (ku: 1.18-3.09 L g-1 d-1) and lower elimination rate constants (ke: 0.008-0.017 d-1) than mussels (ku: 0.21-0.64 L g-1 d-1; ke: 0.018-0.037 d-1). The interspecies differences in tissue Cd concentrations are predominantly due to Cd uptake rather than elimination. Utilizing toxicokinetic parameters to back-calculate Cd concentrations in seawater, we found that the ranking of Cd contamination levels at the six sites markedly differs from those based on tissue Cd concentrations. We propose that this approach will be useful for interpreting data from past and future biomonitoring programs.

An assessment and characterization of pharmaceuticals and personal care products (PPCPs) within the Great Lakes Basin: Mussel Watch Program (2013–2018)

Defining the environmental occurrence and distribution of chemicals of emerging concern (CECs), including pharmaceuticals and personal care products (PPCPs) in coastal aquatic systems, is often difficult and complex. In this study, 70 compounds representing several classes of pharmaceuticals, including antibiotics, anti-inflammatories, insect repellant, antibacterial, antidepressants, chemotherapy drugs, and X-ray contrast media compounds, were found in dreissenid mussel (zebra/quagga; Dreissena spp.) tissue samples. Overall concentration and detection frequencies varied significantly among sampling locations, site land-use categories, and sites sampled proximate and downstream of point source discharge. Verapamil, triclocarban, etoposide, citalopram, diphenhydramine, sertraline, amitriptyline, and DEET (N,N-diethyl-meta-toluamide) comprised the most ubiquitous PPCPs (> 50%) detected in dreissenid mussels. Among those compounds quantified in mussel tissue, sertraline, metformin, methylprednisolone, hydrocortisone, 1,7-dimethylxanthine, theophylline, zidovudine, prednisone, clonidine, 2-hydroxy-ibuprofen, iopamidol, and melphalan were detected at concentrations up to 475 ng/g (wet weight). Antihypertensives, antibiotics, and antidepressants accounted for the majority of the compounds quantified in mussel tissue. The results showed that PPCPs quantified in dreissenid mussels are occurring as complex mixtures, with 4 to 28 compounds detected at one or more sampling locations. The magnitude and composition of PPCPs detected were highest for sites not influenced by either WWTP or CSO discharge (i.e., non-WWTPs), strongly supporting non-point sources as important drivers and pathways for PPCPs detected in this study. As these compounds are detected at inshore and offshore locations, the findings of this study indicate that their persistence and potential risks are largely unknown, thus warranting further assessment and prioritization of these emerging contaminants in the Great Lakes Basin.Graphical

The French Mussel Watch Program reveals the attenuation of coastal lead contamination over four decades

The mid-20th century industrial peak caused severe global lead (Pb) marine contamination. Although Europe initiated Pb emission reduction regulations in the 1980s, the short- and long-term impacts remain unclear. This study investigates the evolution of Pb contamination on the French coast through elemental and isotope analysis in oysters and mussels from the French “Mussel Watch” Program. Observations at 114 monitoring stations over four decades have shown decreasing Pb levels in these bivalve mollusks. In 1988, 95 % exceeded the background reference values; this level had dropped to 39 % by 2021. The Pb isotope ratios in bivalves from eight target sites revealed a reduction in bioaccumulated anthropogenic Pb, albeit without complete elimination. The long residence time of legacy Pb combined with inputs from diffuse urban sources likely explains the persistent presence of anthropogenic Pb on the French coast. This study endorses the importance of continuous biomonitoring to evaluate environmental regulations and policies.

Untargeted Metabolomics Analyses and Contaminant Chemistry of Dreissenid Mussels at the Maumee River Area of Concern in the Great Lakes.

Bivalves serve as an ideal ecological indicator; hence, their use by the NOAA Mussel Watch Program to monitor environmental health. This study aimed to expand the baseline knowledge of using metabolic end points in environmental monitoring by investigating the dreissenid mussel metabolome in the field. Dreissenids were caged at four locations along the Maumee River for 30 days. The mussel metabolome was measured using nuclear magnetic resonance spectroscopy, and mussel tissue chemical contaminants were analyzed using gas or liquid chromatography coupled with mass spectrometry. All Maumee River sites had a distinct mussel metabolome compared to the reference site and revealed changes in the energy metabolism and amino acids. Data also highlighted the importance of considering seasonality or handling effects on the metabolome at the time of sampling. The furthest upstream site presented a specific mussel tissue chemical signature of pesticides (atrazine and metolachlor), while a downstream site, located at Toledo's wastewater treatment plant, was characterized by polycyclic aromatic hydrocarbons and other organic contaminants. Further research into the dreissenid mussel's natural metabolic cycle and metabolic response to specific anthropogenic stressors is necessary before successful implementation of metabolomics in a biomonitoring program.

Vanishing lead in the Loire River estuary: An example of successful environmental regulation

The behavior, and history of lead (Pb) contamination in the ecosystem of the Loire estuary was examined using elemental concentrations and Pb isotope data in water, sediment, bivalves, shrimps, and fish. In the estuary and in the surrounding coastal area, Pb concentrations in water and sediment decreased compared to concentrations determined in the 1980s, with concentrations ranging from 15.8 to 65.7 mg kg−1 in the surface sediment, 0.04–0.26 nM in the water column, and 48.0–77.9 mg kg−1 in suspended particles. Pb biomonitoring using blue mussels collected by the French Mussel Watch Program over the last 40 years showed a concentration decrease from 3.8 to 0.8 mg kg−1. A similar trend is observed in an estuarine sediment core. Changes in accompanying Pb isotope compositions strongly suggest a binary mixing process between Pb derived from terrigenous material and anthropogenic sources. Thus, environmental regulations restricting the release of lead into the environment contribute to a decrease in estuarine levels of this pollutant, which occurs on a decadal time scale.

Employing molecular, chemical and physiological techniques using Crassostrea virginica to assess ecosystem health along coastal South Carolina and North Carolina, United States

Natural and anthropogenic environmental impacts can introduce contaminants into sensitive habitats, threatening ecosystems and human health. Consistent monitoring of coastal areas provides critical environmental assessment data. Sediments and Eastern Oyster (Crassostrea virginica) tissues were collected at fourteen South Carolina (SC) and four North Carolina (NC) sites as part of the National Oceanic and Atmospheric Administration's Mussel Watch environmental monitoring program. Cellular and molecular techniques were employed to measure C. virginica stress response, specifically, Lipid Peroxidation (LPx), Glutathione (GSH), and qPCR techniques. Gene specific primers targeted for detecting oxidative stress and cellular death were developed in C. virginica to gauge response to current environmental conditions using gill and hepatopancreas (HP) tissue. In order to validate gene specific markers as additional assessment tools, a 96 h zinc (Zn) laboratory exposure was performed. Cellular biomarker data revealed tissue specific responses. Hepatopancreas data showed C. virginica exhibited stress through the lipid peroxidation assay amongst sampling sites, however, response was managed through glutathione detoxification. Gill tissue data had significantly lower levels of cellular biomarker response compared to hepatopancreas. Molecular biomarkers targeting these cellular stress pathways through qPCR analysis show upregulation of Metallothionein in hepatopancreas and gill tissue with a concurrent > 2-fold upregulation in the detoxification marker Superoxide Dismutase (SOD) at three NC sites. SC sites displayed higher stress levels through LPx assays and down-regulation in GPx gene activity. Laboratory zinc exposure revealed no significance in cellular biomarker results, however, molecular data showed gills responding to zinc treatment through upregulation of Metallothionein, SOD and Cathepsin L, indicating an acute response in gills. Collectively, chemical, cellular and molecular methods clarify sentinel stress response of biological impacts and aid in evaluating environmental health in coastal ecosystems. This combined methodological approach provides a detailed analysis of environmental conditions and improves land-use management decisions.

The French Mussel Watch: More than two decades of chemical contamination survey in Mediterranean coastal waters

Active biomonitoring of chemical contamination (e.g., Cd, Hg, Pb, DDT, PCB, PAH) in French Mediterranean coastal waters has been performed for more than two decades. This study aimed at presenting the current contamination in 2021 and the temporal evolution of concentrations from 2000. Based on a relative spatial comparison, low concentrations were measured in 2021 at most sites (>83 %). Also, several stations with moderate to high levels were highlighted in the vicinity of major urban industrial centers (e.g., Marseille, Toulon) and near river mouths (e.g., Rhône, Var). Over the last 20 years, no major trend was revealed, mostly, especially for the relative high-level sites. This likely constant contamination over time, plus slight increases of metallic elements at a few sites, still raise questions on the efforts that remain to be made. The decreasing trends of organic compounds, in particular PAH, provide evidence of the efficiency of some management actions.

The Connections between Mussel Watch for Potentially Toxic Metals and Nexus Seafood-Water-Energy

The previous assessment intends to support the inaugural International Mussel Watch program's use of marine mussels as biomonitors of potentially toxic metals in aquacultural areas has been considered of low novelty even though it is a necessary biomonitoring. When it is looked into the connections between Mussel Watch and Nexus seafood-water-energy, the questions can be raised up because there is apparently no such discussion in the literature. Therefore, the objective of this review is to discuss the connections between Mussel Watch for potentially toxic metals and Nexus seafood-water-energy, based on the topic reported in the literature separately. The current short review can act as a springboard for additional insights to offer fresh perspectives and original suggestions on using marine mussels more effectively in biomonitoring investigations in connections to Nexus seafood-water-energy. Nowadays, the biomonitoring by using Mussel Watch has remained effective and sustainable which further highlighted their importance in pollution monitoring. The likelihood of improved and wider-ranging molluscan uses in environmental monitoring in the future is almost inevitable. However, more research is still needed to address the rising demand in line with sustainable, attainable United Nation Sustainable Development Goals (‘‘Responsible consumption and production’’, and ‘Good Health and Well-beings’). This is surely a major player in the Nexus’s seafood in cycle with water and energy that should be addressed in future biomonitoring studies.

Distribution of cadmium and lead levels in the intertidal clam Glauconome virens: A biomonitoring study

The intertidal clam, Glauconome virens, was collected in the northwestern portion of Peninsular Malaysia near Kuala Perlis, Sungai Layar, and Pantai Teluk Air Tawar. This research attempted to determine the cadmium (Cd) and lead (Pb) concentrations in the various G. virens’s organs. The Cd concentrations (mg/kg dry weight) in five distinct soft tissues ranged from 0.90 to 1.89, but the concentrations in shells ranged from 0.95 to 1.25. Pb concentrations (mg/kg dry weight) in the five distinct soft tissues ranged from 27.0 to 44.9, whereas shell concentrations ranged from 74.8 to 75.3. In general, the shell had more Pb than the soft tissue components. Future biomonitoring research on this type of clams should concentrate on certain tissues (such as the remainder, shell, and gill) to identify their potential as biomonitoring organs/materials. This biomonitoring study is of paramount importance to establish the intertidal clams as a good biomonitor under the umbrella of International Mussel Watch. Besides, establishment of such biomonitoring baseline data is important for future references and human health risk assessments.

Mussel watch program for microplastics in the Mediterranean sea: Identification of biomarkers of exposure using Mytilus galloprovincialis

Microplastics (MPs) are ubiquitous pollutants that have also been detected in the aquatic ecosystems at high concentrations. The use of shellfish as bioindicators is widespread for assessing and monitoring the environmental quality in both freshwater and marine environments. On this path, biomarkers represent an effective tool in monitoring programs. This minireview would broaden the existing knowledge on biomarkers of MPs in the Mediterranean mussel Mytilus galloprovincialis. This species was selected as it is widely distributed across the Mediterranean Sea and used as a bioindicator to monitor the presence of MPs in the marine environment. The literature search returned only 11 studies, mainly related to oxidative stress biomarkers. Although certain biomarkers were explored to estimate the effects of MPs on M. galloprovincialis, a battery of standardized and validated biomarkers as well as the inclusion of new ones are needed in future studies to obtain more comparable and robust findings across the Mediterranean Sea.

Mussel watch monitoring program: a practical monitoring tool of potentially toxic metals pollution from 1970 to beyond 2070

Mussel watch monitoring program: a practical monitoring tool of potentially toxic metals pollution from 1970 to beyond 2070

Contaminant concentrations and risks associated with the Pacific oyster in the highly urbanized San Diego Bay

Contaminant concentrations in filter-feeding shellfish may indicate the health of coastal waters and consumption risks. Widespread expansion of the Pacific oyster (Crassostrea gigas) and its popularity as food make it a useful sentinel. We surveyed intertidal Pacific oysters in San Diego Bay, California for contaminants during summer 2018 and winter 2019. We compared contaminants in Pacific oyster to California mussel from California's State Mussel Watch Program (1993–2003) and human consumption thresholds. Contaminants such as neonicotinoid and chlorinated pesticides, selenium, and several metals were higher in Pacific oysters in summer, while PBDEs, benzylbutyl phthalate, and plastics were higher in winter. Contaminant levels were generally lower in Pacific oyster than mussel except for copper and zinc. Bay-wide PCB concentrations in oysters exceeded thresholds but individual samples (locations) also met or surpassed chlordane, PCB and PAH thresholds. Monitoring and risk assessments that consider species' biology, season, location, effects of multiple contaminants, and human consumption patterns will contribute to more effective consumption guidelines.

Characterization of polycyclic aromatic hydrocarbons in the Great Lakes Basin using dreissenid mussels

The National Oceanic and Atmospheric Administration (NOAA), National Centers for Coastal Ocean Science (NCCOS) Mussel Watch Program (MWP), conducts basin-wide monitoring and place-based assessments using dreissenid mussels as bioindicators of chemical contamination in the Laurentian Great Lakes. Polycyclic aromatic hydrocarbons (PAHs) body burden results for the period 2009–2018 were combined into one dataset from multiple MWP studies allowing for a robust characterization of PAH contamination. Patterns in PAH data were identified using descriptive statistics and machine learning techniques. Relationships between total PAH concentration in dreissenid mussel tissue, impervious surface percentages, and PAH relative concentration were identified and used to build a predictive model for the Great Lakes Basin. Significant positive correlation was identified by the Spearman’s rank correlation test between total PAH concentration and percent impervious surface. The findings support the paradigm that PAHs are primarily derived from land-based sources. Offshore and riverine locations had the lowest and highest median total PAH concentrations, respectively. PAH assemblages and ratios indicated that pyrogenic sources were more predominant than petrogenic sources and that PAHs at offshore sites exhibited relatively more weathering compared to inshore sites.

The influence of natural vs anthropogenic factors on trace metal(loid) levels in the Mussel Watch programme: Two decades of monitoring in the Spanish Mediterranean sea

The spatial distribution and temporal trends of trace metals (i.e. Cd, Cu, Hg, Pb and Zn) and a metalloid (i.e. As) along the Spanish Mediterranean coast from 1993 to 2013 are presented with a new estimation of their background levels monitored using wild mussels. Over a 20 years period, yearly mussel monitoring was undertaken with a rigorous field sampling protocol using 3 pooled samples strategy (3 x n = 80, with 8 mussels in the 3.0 to 3.9 size categories at each site), obtained in the pre-spawning period (May–June) to minimize biological factors and seasonal variability, which is a fundamental element of the international programme. Spatial distribution was characterized every 5 years and temporal trends were determined in 11 locations. The main aims of the present long term study are to evaluate the environmental status of different coastal locations regarding trace metal levels and follow the evolution of these levels over time after the implementation of regulatory measures. Regarding spatial distribution, the highest values for Cd, Cu, Hg and Pb were found close to known highly anthopogenic cities or shipyard areas. However, As and Zn did not strictly follow this pattern, showing natural increased concentrations in the Levantine Balearic and Strait of Gibraltar-Alboran Sea demarcations respectively. These distributions are associated with the conjunction of two geological formation inputs (Massif Central in France and Iberian Pyritic Belt in Spain) and the oceanographic conditions in the adjacent coastal area. In the case of temporal trends, metal concentrations decreased significantly over time in most stations, confirming the effectiveness of the regulatory measures and prohibitions established under European legislation. Concentrations of Pb were above the established thresholds for human consumption in only 12–14% of the sampling areas. With the information obtained for this study, we estimate background concentrations and propose new Background Assesment Criteria (BAC) for the Spanish Mediterranean coast as a threshold criterion: 1.62 mg/kg d.w. for Cd, 8.75 mg/kg d.w. for Cu, 0.202 mg/kg d.w. for Hg and 2.83 mg/kg d.w. for Pb.Exceptions should exist for As and Zn, for which there should be different levels in each demarcation, due to the geological, hydrological and oceanographic peculiarities of the Spanish coast. For the Levantine-Balearic demarcation, the proposed background concentrations are 117 mg/kg d.w. for As and 200 mg/kg d.w. for Zn., whereas in the Strait of Gibraltar-Alboran Sea demarcation, they are 27.5 mg/kg d.w. for As, and 471 mg/kg d.w. for Zn. This work demonstrates the vital importance of defining the background levels of metal(loid)s at a regional or subregional level because, for areas not affected by anthropogenic causes which have high values as the result of natural processes, this would avoid the risk of constantly surpassing the levels proposed in directives.

Cadmium bioaccumulation and distribution in the freshwater bivalve Anodonta woodiana exposed to environmentally relevant Cd levels

Anodonta woodiana is a globally distributed freshwater bivalve, which is a unique bioindicator in the “Freshwater Mussel Watch” project. Numerous countries have used A. woodiana for biomonitoring the aqueous cadmium (Cd) contamination. However, the bioaccumulation and distribution characteristics of environmentally relevant Cd concentrations in the bivalve were unknown. In this study, A. woodiana was exposed to aqueous Cd concentrations (1.1, 2.6, and 5.5 μg/L) for 30 days. The concentrations of Cd in the whole soft tissues were linearly and positively correlated with the aqueous Cd concentrations and exposure time (P < 0.05). Analysis of the organic bioaccumulation and distribution showed that Cd concentrations and proportions in the gills and mantle were linearly and positively correlated with aqueous Cd concentrations and with the Cd concentrations in the whole soft tissues (P < 0.05). Analyses of the subcellular fractions showed that Cd concentrations and proportions in the metal-rich granule (MRG) were linearly and positively correlated with aqueous Cd concentrations and with the Cd concentrations in the whole soft tissues (P < 0.05). This suggests that the gills and mantle could be the main target organs for Cd bioaccumulation, and that the MRG could be the major site for Cd bioaccumulation and distribution. These results improve our understanding of the bioaccumulation and distribution mechanisms of Cd in bivalves.

Spatiotemporal change of cesium-137 in the Pacific coast of Tohoku, Japan: The mussel watch approach

We measured radiocesium in mussel tissue collected from the Pacific coast of Tohoku from 2011 to 2015 to investigate the temporal and spatial dynamics of radiocesium in the coastal area. Radioactive 137Cs was detected in all the samples collected in 2011, but it was not found in samples from localities north of Sendai after 2012. In contrast, 137Cs was detected in many sites in the Fukushima area even from 2012 to 2015. The fluctuation of 137Cs concentration in mussel tissue seems to reflect the 137Cs concentration in suspended particles in the seawater, suggesting that there was an influx of soil deposition and resuspension of seabed sediment. These results suggest that the 137Cs concentration in mussel tissue sensitively indicates the 137Cs concentration in the environment, and that the “mussel watch” approach is an effective way to understand the dynamics of radiocesium concentrations in coastal areas.

A Commentary on the Use of Bivalve Mollusks in Monitoring Metal Pollution Levels.

The objective of this commentary is to promote the use of bivalves as biomonitors, which is a part of the continual efforts of the International Mussel Watch. This commentary is an additional discussion on “Bivalve mollusks in metal pollution studies: From bioaccumulation to biomonitoring” by Zuykov et al., published in Chemosphere 93, 201–208. The present discussion can serve as a platform for further insights to provide new thoughts and novel ideas on how to make better use of bivalves in biomonitoring studies. The certainty of better and more extensive applications of mollusks in environmental monitoring in the future is almost confirmed but more studies are urgently needed. With all the reported studies using bivalves as biomonitors of heavy metal pollution, the effectiveness of using Mussel Watch is beyond any reasonable doubts. The challenge is the development of more accurate methodologies for of heavy metal data interpretation, and the precision of the biomonitoring studies using bivalves as biomonitors, whether in coastal or freshwater ecosystems. Lastly, inclusion of human health risk assessment of heavy metals in commercial bivalves would make the research papers of high public interest.

Rare Earth Element in Bivalves' Soft Tissues of French Metropolitan Coasts: Spatial and Temporal Distribution.

Rare earth elements (REE) are becoming an environmental pollutant of emerging concern, linked to their use in various anthropic processes. Because REE bioconcentrate in marine organisms throughout their food webs, a better understanding of biogeochemical processes leading to REE concentrations found in coastal species is necessary. This study was designed to assess REEs concentrations in various common bivalves from the French coastline to identify possible geographic, taxonomic, or temporal variations of concentrations. Based on the French Mussel Watch program, three species of bivalves (oyster Crassostrea gigas and mussels Mytilus edulis and Mytilus galloprovincialis) were collected all along the French metropolitan coast and soft tissues were analyzed forREEconcentrations. Results have shown higher REE concentrations in bivalve soft tissues near estuaries without taxonomic nor national geographic differences. The highest levels have been observed in the Gironde estuary with total REE concentrations (∑REE) in oysters up to 10.94µgg-1 d.w. The REE distribution pattern in both mussel species described a particle-like (inverse V-shape) pattern, whereas C. gigas REE distribution pattern changes from a particle-like to a dissolved-like pattern with a heavy REE (HREE) enrichment. However, no environmental parameter could be linked to these pattern changes. Finally, neither Gd anomalies nor an evolution of REE concentrations over a 30-year period have been detected in bivalves' soft tissues.

Application of Zn Isotope Compositions in Oysters to Monitor and Quantify Anthropogenic Zn Bioaccumulation in Marine Environments over Four Decades: A “Mussel Watch Program” Upgrade

The application of zinc (Zn) isotope compositions in bivalve organisms to quantify anthropogenic Zn bioaccumulation in marine biota is of great interest to environmental marine management programs ...

Mercury in Marine Mussels from the St. Lawrence Estuary and Gulf (Canada): A Mussel Watch Survey Revisited after 40 Years

Various species of marine mussels have been used, in the last 50 years, as sentinel organisms for monitoring metal contamination along marine coasts. There are two main reasons for this: these mollusks concentrate metals in their soft tissue and they are geographically widespread. In practice, trace metal concentrations in mussel soft tissue reveal (after some correction for biotic effects) the contamination level of their surrounding environment. We present the results of a mercury (Hg) survey in Mytilus spp. collected in the summers of 2016, 2018, and 2019 at 51 stations distributed along the coasts of the Estuary and Gulf of St. Lawrence. Mercury concentrations ranged from 0.063 to 0.507 µg g−1 (dry weight, dw), with a grand mean of 0.173 ± 0.076 µg g−1 dw (±1 standard deviation), and a median of 0.156 µg g−1 dw for the 504 individuals analyzed. Mercury contents per individual mussel were significantly (p &lt; 0.01) related to shell length and dry tissue weight, with the smaller individuals having the highest Hg concentrations. To take into account these biotic effects, we normalized Hg concentrations of the mussel soft tissue for constant shell length (L) and soft tissue weight (TW) based on the log-log relationships between Hg content and L or TW. The normalized Hg contents of mussels varied from 10.9 to 66.6 ng per virtual individual of 35 mm length and 0.17 g dry weight. A similar normalization procedure applied to 1977–1979 data, yielded a very similar range: 12 to 64 ng. This observation suggests that the Hg bioavailable to marine mussels in the study area did not change over a span of 40 years. Regional Hg distribution patterns indicate a gradual decrease of Hg content in mussels downstream from freshwater discharges to the St. Lawrence Estuary and the Baie des Chaleurs, suggesting that rivers constitute a significant Hg source in these estuarine systems. Atmospheric Hg deposition and concentration in marine waters of the Atlantic Ocean are known to have decreased in the last decades. However, in coastal environments, the response to these changes does not seem to be rapid, probably because of the long residence time of Hg in soils before being exported to coastal areas.