Particle-reactive Contaminants Research Articles

Semi-enclosed bays serve as hotspots for black carbon burial: A case study in Jiaozhou Bay, western Yellow Sea

The provenance of black carbon (BC) and its role in affecting contaminant cycling in both the atmosphere and aquatic environments have been extensively studied. However, the fate and cycling dynamics of BC, particularly in marine environments, are poorly understood. Herein, soot BC was determined in the semi-enclosed Jiaozhou Bay to examine the seasonal variability, residence timescale in seawater, and settling flux to sediments, together with particle-reactive 234Th. Soot BC ranged from 0.39 to 4.26 μmol-C L−1. On average, spring produced the highest value of 1.88 ± 0.31 μmol-C L−1, followed by winter (1.59 ± 0.18 μmol-C L−1), summer (0.94 ± 0.09 μmol-C L−1), and autumn (0.90 ± 0.09 μmol-C L−1). The seasonality of soot BC was similar to the activity concentration of particulate 234Th (i.e., 234ThP). The close relationships between soot BC and 234ThP (p < 0.01) provide the basis for the application of 234Th to trace the fate of soot BC. Based on the 234Th deficit with respect to 238U, the residence times of soot BC were estimated to be 41 ± 6 d and 36 ± 5 d for May–August and August–November, respectively. The shorter residence times of soot BC than that of seawater indicated that soot BC delivered to Jiaozhou Bay settled in the local sediments. Furthermore, soot BC concentrations were higher in the inflow seawater from the Yellow Sea than the outflow water from Jiaozhou Bay, implying a net input of soot BC from the Yellow Sea to Jiaozhou Bay. The soot BC fluxes were 0.266 ± 0.035 mmol-C m−2 d−1 and 0.0472 ± 0.0065 mmol-C m−2 d−1 for May–August and August–November, respectively. From the bay-scale perspective, Jiaozhou Bay had buried 0.101 ± 0.010 Gg of soot BC each year. These results indicate that the semi-enclosed Jiaozhou Bay acts as an effective trap for soot BC and particle-reactive contaminants.

Constraining the origin of recently deposited particles using natural radionuclides 7Be and 234Thex in deltaic sediments

7Be and 234Thex activities were determined in sediment cores off the Rhône River mouth (Gulf of Lions), in order to trace the initial transport and deposition of riverine suspended particulate matter (SPM) and evaluate the impact of flood events through 7 cruises carried out between 2007 and 2008. Consistently high 7Be and 234Thex inventories of 2000–3000 mBq cm−2 and 3000–5000 mBq cm−2, respectively, were observed within a ~5 km radius off the Rhône River mouth. Their spatial distributions showed a gradual decrease with increasing distance from the Rhône River mouth, and the decrease in 7Be was more pronounced than that of 234Thex, indicating that recent riverine SPM is rapidly deposited in the area located near the river mouth. This area is also characterized by high accumulation rates determined using 137Cs or 210Pbex. Both 7Be and 234Thex inventories increased in 2008 compared to 2007, and are correlated to the cumulated SPM flux for normal and flood discharge. Moreover, the 7Be/234Thex inventory ratio appears to be a potential tracer to identify the dominant influence of recently deposited particles between terrestrial and marine waters. This ratio provides an effective tool to assess river and marine influence: Zone I at a distance inferior to 3.0 km, with 7Be/234Thex inventory ratio over 0.50 (surface area near river mouth ~ 7 km2) is dominated by riverine influence; in contrast, Zone III at a distance superior to 8.5 km, with 7Be/234Thex inventory ratio less than 0.10 (surface area off river mouth beyond 150 km2) is predominantly under a marine influence. In between, an intermediate area (Zone II at a distance between 3.0 and 8.5 km, with 7Be/234Thex inventory ratios between 0.10 and 0.50) displays a mixed influence. This zoning could help in further understanding the spreading of particle-reactive contaminants and its initial sedimentary deposition in the Gulf of Lions.

Particle-Dissolved Phase Partition of Polychlorinated Biphenyls in High Altitude Alpine Lakes.

We investigated whether polychlorinated biphenyls (PCBs) partitioning between the dissolved and particulate phases in two high altitude alpine lakes was determined by the quantity, size structure, or composition of suspended particles. Within- and between-lakes differences in water-particulate phase partition coefficient (Kp) were not related to total suspended matter, phytoplankton biomass, or taxonomic composition. Yet, a seasonal relationship between Kp and Kow was detected for both lakes, revealing equilibrium of PCBs partition when lakes were ice covered. On the contrary, PCBs partitioning between particles and water appeared kinetically limited during the open water season. Partition is therefore mainly governed by thermodynamic laws during the ice-covered period, while none of the tested physical or biological parameters seemed to explain the distribution of these particle-reactive contaminants in the open water period. PCBs were always mainly associated with particulate matter, but partitioning within different particulate size-fractions varied between seasons and between years during open water periods. When ice cover is absent, PCBs were mainly adsorbed on microplankton, the largest phytoplanktonic size fraction, which is the least likely to get grazed by pelagic microconsumers.

Sources of land-derived runoff to a coral reef-fringed embayment identified using geochemical tracers in nearshore sediment traps

Geochemical tracers, including Ba, Co, Th, 7Be, 137Cs and 210Pb, and magnetic properties were used to characterize terrestrial runoff collected in nearshore time-series sediment traps in Hanalei Bay, Kauai, during flood and dry conditions in summer 2006, and to fingerprint possible runoff sources in the lower watershed. In combination, the tracers indicate that runoff during a flood in August could have come from cultivated taro fields bordering the lower reach of the river. Land-based runoff associated with summer floods may have a greater impact on coral reef communities in Hanalei Bay than in winter because sediment persists for several months. During dry periods, sediment carried by the Hanalei River appears to have been mobilized primarily by undercutting of low 7Be, low 137Cs riverbanks composed of soil weathered from tholeiitic basalt with low Ba and Co concentrations. Following a moderate rainfall event in September, high 7Be sediment carried by the Hanalei River was probably mobilized by overland flow in the upper watershed. Ba-desorption in low-salinity coastal water limited its use to a qualitative runoff tracer in nearshore sediment. 210Pb had limited usefulness as a terrestrial tracer in the nearshore due to a large dissolved oceanic source and scavenging onto resuspended bottom sediment. 210Pb-scavenging does, however, illustrate the role resuspension could play in the accumulation of particle-reactive contaminants in nearshore sediment. Co and 137Cs were not affected by desorption or geochemical scavenging and showed the greatest potential as quantitative sediment provenance indicators in material collected in nearshore sediment traps.

The EXTREME project consequences of paroxystic meteo climatic events on the translocation of contaminants within the geosphere

The EXTREME project was launched by the IRSN in 2005 to study the consequences of extreme meteo climatic events on reuptake of stocks and associated fluxes within the various compartments of the geosphere. Large masses of matter transferred during such events are liable to be displaced between locations, leading to higher pollution levels than those arising from average transfer processes, and producing pollutant fluxes that can be equivalent to the fluxes accumulated over several months or even years. This particularly concerns particle-reactive contaminants such as trace metals and long lived artificial radionuclides. The final aim of the project is to estimate the vulnerability of a coastal system (the Gulf of Lions, north western Mediterranean sea) to global change over the next 30 years. Indeed several programs dedicated to climate change predict a potential increase in the frequency of extreme events such as floods, floodings, saharian dust episodes, forest fire events and storms, particularly within the studied area.

Food acquisition responses of the suspension-feeding bivalve Placopecten magellanicus to the flocculation and settlement of a phytoplankton bloom

In situ technologies were employed to monitor suspended particle flocculation and floc settlement and utilization by a cohort of sea scallops ( Placopecten magellanicus) during the 2000 spring phytoplankton bloom in Bedford Basin, Nova Scotia, Canada. The objectives were to determine the effect of bloom flocculation and settling on food acquisition and utilization by scallops, and to assess the potential role of flocculation in enhancing the bioavailability of trophic resources and particle-reactive contaminants to bivalve filter feeders. The development and flocculation of the phytoplankton bloom were monitored within the surface layer (10 m depth) by in vivo chlorophyll fluorescence and silhouette camera observations. Sedimentation rate, seston abundance and composition, and sea scallop functional responses were monitored at 20 m depth (below the bloom) to provide insight into the potential forcing of feeding and digestion processes by changes in the abundance, composition and properties of the ambient food supply. The bloom began in mid-March and median floc diameter at 10 m depth increased rapidly from 200 μm to greater than 400 μm between 21 and 28 March. Flocs were observed to be abundant in the surface layer up to 4 April. Daily vertical particle flux was high during the last week of March and declined to near zero by 1 April. Clearance rates of scallops held at 20 m depth were relatively high (average ± S.D.; 11.7 ± 4.0 L h − 1 ) during the period of bloom settlement and declined rapidly to low levels (0.4 ± 0.9 L h − 1 ) after 31 March. Average absorption efficiency also declined (0.88 ± 0.01 to 0.78 ± 0.05) after bloom settlement. Daily biodeposition rates by scallops were poorly correlated with temporal variations in the quantity (total particulate matter and chlorophyll a concentration) or quality (organic content) of seston available to the scallops, but were significantly correlated with sedimentation rate. Comparison of disaggregated inorganic particle size distributions for suspended particulate matter, settled particles, and scallop feces indicated that fine-grained particles (1 to 4 μm) were effectively ingested by sea scallops—an indication of whole floc ingestion. The settlement of flocs produced during the spring bloom appears to be important in regulating this species physiological energetics and for enhancing the bioavailablility of fine particles (including picoplankton) and particle-reactive contaminants.

Relative importance of macrofaunal burrows for the microbial mineralization of pyrene in marine sediments: impact of macrofaunal species and organic matter quality

The significance of macrofaunal burrows for microbial organic matter mineralization is well recognized. However, despite the importance of marine sediments as main sinks for organic particle-reactive contaminants such as polyaromatic hydrocarbons (PAHs), the significance of biogenic structures for microbial pollutant mineralization is largely unknown. We measured microbial mineralization of the PAH pyrene in different sediment compartments (surface, burrow and reduced bulk sediments) as a function of contamination history (uncontaminated and pyrene-exposed), macrofaunal species (Amphiura filiformis and Nereis diversicolor) and sediment organic matter quality (labile Tetraselmis sp. and refractory lignin). Sediments were exposed to combinations of the 3 factors for 43 d, after which sediment samples from the 3 compartments were incubated for radio-respirometric measurements in 1 4 C-pyrene-coated flasks to monitor 1 4 CO 2 production (i.e. pyrene mineralization) for 128 d. Pyrene exposure enhanced microbial pyrene mineralization (MPM) rates by an order of magnitude in all compartments, signifying MPM as inducible. MPM rates increased successively from reduced bulk to burrow and surface sediments in uncontaminated treatments, while MPM rates were highest in burrows when exposed to pyrene. This emphasizes the oxygen dependence of MPM and pinpoints burrows as MPM hot spots. Enrichment with labile organic matter doubled MPM rates in pyrene-exposed surface sediment, likely fertilizing MPM where oxygen is readily available. Burrow sediment MPM rates were doubled with A. filiformis, suggesting species-specific stimulation of the microbial community within the burrows. In conclusion, burrow sediment appears to be at least as important as surface sediment for microbial PAH degradation in marine sediments. Furthermore, macrofaunal biodiversity, sedimentation events and the trophic state of the system should be taken into account when the fate and effects of organic contaminants are assessed in marine systems.

Clay mineralogy and multi-element chemistry of surface sediments on the Siberian-Arctic shelf: implications for sediment provenance and grain size sorting

Clay mineral and bulk chemical (Si, Al, K, Mg, Sr, La, Ce, Nd) analyses of terrigenous surface sediments on the Siberian-Arctic shelf indicate that there are five regions with distinct, or endmember, sedimentary compositions. The formation of these geochemical endmembers is controlled by sediment provenance and grain size sorting. (1) The shale endmember (Al, K and REE rich sediment) is eroded from fine-grained marine sedimentary rocks of the Verkhoyansk Mountains and Kolyma-Omolon superterrain, and discharged to the shelf by the Lena, Yana, Indigirka and Kolyma Rivers. (2) The basalt endmember (Mg rich) originates from NE Siberia's Okhotsk-Chukotsk volcanic belt and Bering Strait inflow, and is prevalent in Chukchi Sea Sediments. Concentrations of the volcanically derived clay mineral smectite are elevated in Chukchi fine-fraction sediments, corroborating the conclusion that Chukchi sediments are volcanic in origin. (3) The mature sandstone endmember (Si rich) is found proximal to Wrangel Island and sections of the Chukchi Sea's Siberian coast and is derived from the sedimentary Chukotka terrain that comprises these landmasses. (4) The immature sandstone endmember (Sr rich) is abundant in the New Siberian Island region and reflects inputs from sedimentary rocks that comprise the islands. (5) The immature sandstone endmember is also prevalent in the western Laptev Sea, where it is eroded from sedimentary deposits blanketing the Siberian platform that are compositionally similar to those on the New Siberian Islands. Western Laptev can be distinguished from New Siberian Island region sediments by their comparatively elevated smectite concentrations and the presence of the basalt endmember, which indicate Siberian platform flood basalts are also a source of western Laptev sediments. In certain locations grain size sorting noticeably affects shelf sediment chemistry. (1) Erosion of fines by currents and sediment ice rafting contributes to the formation of the coarse-grained sandstone endmembers. (2) Bathymetrically controlled grain size sorting, in which fines preferentially accumulate offshore in deeper, less energetic water, helps distribute the fine-grained shale and basalt endmembers. An important implication of these results is that the observed sedimentary geochemical endmembers provide new markers of sediment provenance, which can be used to track sediment transport, ice-rafted debris dispersal or the movement of particle-reactive contaminants.

Incorporating soil structure and root distribution into plant uptake models for radionuclides: toward a more physically based transfer model

Most biosphere and contamination assessment models are based on uniform soil conditions, since single coefficients are used to describe the transfer of contaminants to the plant. Indeed, physical and chemical characteristics and root distribution are highly variable in the soil profile. These parameters have to be considered in the formulation of a more realistic soil–plant transfer model for naturally structured soils. The impact of monolith soil structure (repacked and structured) on Zn and Mn uptake by wheat was studied in a controlled tracer application (dye and radioactive) experiment. We used Brilliant Blue and Sulforhodamine B to dye flow lines and 65Zn and 54Mn to trace soil distribution and plant uptake of surface-applied particle-reactive contaminants. Spatial variation of the soil water content during irrigation and plant growth informs indirectly about tracer and root location in the soil profile. In the structured monolith, a till pan at a depth of 30 cm limited vertical water flow and root penetration into deeper soil layers and restricted tracers to the upper third of the monolith. In the repacked monolith, roots were observed at all depths and fingering flow allowed for the fast appearance of all tracers in the outflow. These differences between the two monoliths are reflected by significantly higher 54Mn and 65Zn uptake in wheat grown on the structured monolith. The higher uptake of Mn can be modelled on the basis of radionuclide and root distribution as a function of depth and using a combination of preferential flow and rooting. The considerably higher uptake of Zn requires transfer factors which account for variable biochemical uptake as a function of location.

Scavenging of Thorium Isotopes in the Arctic Regions: Implications for the Fate of Particle-reactive Pollutants

The sources of inorganic pollutants to the Arctic areas are reviewed using previously published results. The removal of particle-reactive pollutants is discussed using thorium scavenging as an analog. The scavenging of 234Th from the upper water column (∼ 100 m ) and sediment inventory of 230Th from the deep Arctic waters is compared to different ocean basins in the subarctic areas. Such a comparison shows that 234Th is in equilibrium with its parent, 238U, in certain regions of the Canada Basin of the Arctic Ocean, while it is deficient in other regions of the arctic as well as in sub-polar ocean basins. This implies that the particle-reactive pollutants in the deep Arctic of the Canada Basin are less likely to be removed from the deep waters and will eventually be transported out of this area. We have utilized the 230Th inventory in sediments from the Arctic area to determine the removal rates of particle-reactive nuclides. The 230Th inventory in the deep Arctic Ocean of the Canada Basin is much lower than the Norwegian Sea and the Fram Strait of the Arctic as well as all other sub-polar world oceans. These observations suggest that any pollutants into the deep Arctic areas of the Canada Basin are less likely to be removed locally and may be transported out of this area. In those areas, the colloidal material could potentially play a major role in the removal of particle-reactive contaminants.

Similar Rates of Decrease of Persistent, Hydrophobic and Particle-Reactive Contaminants in Riverine Systems

Although it is well-known that concentrations of anthropogenic radionuclides and organochlorine compounds in aquatic systems have decreased since their widespread release has stopped in the United States, the magnitude and variability of rates of decrease are not well-known. Paleolimnological studies of reservoirs provide a tool for evaluating these long-term trends in riverine systems. Rates of decrease from the 1960s to the 1990s of {sup 137}Cs, PCBs, and total DDT in dated sediment cores from 11 reservoirs in the eastern and central United States were modeled using first-order rate models. Mean half-times of 10.0 ({+-}2.5), 9.5 ({+-}2.2), and 13 ({+-}5.8) yr for decay-corrected {sup 137}Cs, PCBs, and total DDT, respectively, are surprisingly similar. Similar rates of decrease in a few reservoirs are also demonstrated for chlordane and lead. Conceptual and simple mathematical models relating two soil distributions of {sup 137}Cs to trends in the cores provide insight into differences in trends between watersheds with different land uses and suggest that trends are controlled by erosion, transport, mixing, and deposition of sediments. These results, supported by similar trends reported for other settings and environmental media, could provide an estimate of the decadal response time of riverine systems to changes in the regulationmore » of other persistent hydrophobic or particle-reactive contaminants.« less

Transport of a non-volatile contaminant in unsaturated porous media in the presence of colloids

Stable colloidal particles can travel long distances in subsurface environments and carry particle-reactive contaminants with them to locations further than predicted by the conventional advective-dispersive transport equation. When such carriers exist in a saturated porous medium, the system can be idealized as consisting of three phases: an aqueous phase, a carrier phase, and a stationary solid matrix phase. However, when colloids are present in an unsaturated porous medium, the system representation should include one more phase, i.e. the air phase. In the work reported, a mathematical model was developed to describe the transport and fate of the colloidal particles and a non-volatile contaminant in unsaturated porous media. The model is based on mass balance equations in a four-phase porous medium. Colloid mass transfer mechanisms among aqueous, solid matrix, and air phases, and contaminant mass transfer between aqueous and colloid phases are represented by kinetic expressions. Governing equations are non-dimensionalized and solved to investigate colloid and contaminant transport in an unsaturated porous medium. A sensitivity analysis of the transport model was utilized to assess the effects of several parameters on model behavior. The colloid transport model matches successfully with experimental data of Wan and Wilson. The presence of air-water interface retards the colloid transport significantly counterbalancing the facilitating effect of colloids. However, the retardation of contaminant transport by colloids is highly dependent on the properties of the contaminant and the colloidal surface.

Contaminant dispersal on the Palos Verdes continental margin: III. Processes controlling transport, accumulation and re-emergence of DDT-contaminated sediment particles

A large mass of DDT-contaminated sediment lies buried beneath a thin cover on the Palos Verdes shelf and slope off Los Angeles, California. Analyses, including several types of numerical simulation, have been applied to an extensive data set to evaluate the biological and physical processes controlling the fate of the strongly particle-reactive pollutants. Sequential measurements of the p,p′-DDE (an isomer of DDT) content in cores from monitoring locations indicate that contaminated sediment particles are being re-introduced into the marine environment from the buried historic deposits at a significant rate. There is considerable scatter in the data but the trends for ongoing release over the 8 years between 1983 and 1991 are statistically significant at the 90% level. A comprehensive mathematical model of shelf sediment dynamics (Resuspension Model) has been used to explore sediment erosion and deposition during major storms of the early 1980s and of 1988. This modeling shows that storms alone cannot explain the observed losses of contaminated sediment particles from the historical deposits of the Palos Verdes shelf. On the other hand, it also demonstrates that both severe and common storm events do re-entrain some of the bottom sediment at all water depths across the Palos Verdes shelf. A numerical model (Contaminant Release Model), which couples upward biodiffusion of DDT with storm removal, satisfactorily explains the observed losses. The infaunal activity that creates biodiffusion has been explored in two separate ways. In calibrating the Contaminant Release Model, the depth-dependent biodiffusion coefficient profile is estimated by comparing the predicted and measured depth concentration distributions. A separate analysis has been conducted using the measured vertical distribution of infaunal species (Stull et al. 1995; Swift et al., 1995). The agreement between these two methods is good. Both show that bioturbation extends to the level of the high contamination. Bioturbation is now playing a significant role in redistributing the buried historic contaminants. The Contaminant Release Model, in combination with evaluations of the total sedimentation rate and the natural background sedimentation rate, clearly shows that the flux of solids from the outfall enhances the rate of accumulation of natural sediment on the Palos Verdes shelf. A sharp reduction of the flux of solids, such as would accompany conversion from partial to full secondary treatment, will result in considerably prolonging the high rates with which DDT and other particle-reactive contaminants are re-entering the marine environment.

Contaminant dispersal on the Palos Verdes continental margin: III. Processes controlling transport, accumulation and re-emergence of DDT-contaminated sediment particles

A large mass of DDT-contaminated sediment lies buried beneath a thin cover on the Palos Verdes shelf and slope off Los Angeles, California. Analyses, including several types of numerical simulation, have been applied to an extensive data set to evaluate the biological and physical processes controlling the fate of the strongly particle-reactive pollutants. Sequential measurements of the p,p′-DDE (an isomer of DDT) content in cores from monitoring locations indicate that contaminated sediment particles are being re-introduced into the marine environment from the buried historic deposits at a significant rate. There is considerable scatter in the data but the trends for ongoing release over the 8 years between 1983 and 1991 are statistically significant at the 90% level. A comprehensive mathematical model of shelf sediment dynamics (Resuspension Model) has been used to explore sediment erosion and deposition during major storms of the early 1980s and of 1988. This modeling shows that storms alone cannot explain the observed losses of contaminated sediment particles from the historical deposits of the Palos Verdes shelf. On the other hand, it also demonstrates that both severe and common storm events do re-entrain some of the bottom sediment at all water depths across the Palos Verdes shelf. A numerical model (Contaminant Release Model), which couples upward biodiffusion of DDT with storm removal, satisfactorily explains the observed losses. The infaunal activity that creates biodiffusion has been explored in two separate ways. In calibrating the Contaminant Release Model, the depth-dependent biodiffusion coefficient profile is estimated by comparing the predicted and measured depth concentration distributions. A separate analysis has been conducted using the measured vertical distribution of infaunal species (Stull et al. 1995; Swift et al., 1995). The agreement between these two methods is good. Both show that bioturbation extends to the level of the high contamination. Bioturbation is now playing a significant role in redistributing the buried historic contaminants. The Contaminant Release Model, in combination with evaluations of the total sedimentation rate and the natural background sedimentation rate, clearly shows that the flux of solids from the outfall enhances the rate of accumulation of natural sediment on the Palos Verdes shelf. A sharp reduction of the flux of solids, such as would accompany conversion from partial to full secondary treatment, will result in considerably prolonging the high rates with which DDT and other particle-reactive contaminants are re-entering the marine environment.

Lead isotopic determination of historical sources of lead to Lake Erie, North America

Measurements of lead concentrations and stable lead isotopic compositions ( 204Pb, 206Pb, 207Pb, 208Pb) in sediment cores from Lake Erie document both temporal and spatial variations in lead sources to the lake. These analyses track the history of lead contamination in the lake, as well as the transport of particulate matter which governs the redistribution of particle-reactive contaminants within the lake. The isotopic compositions of the sediments reveal two sources of natural lead (fluvial and shoreline bluff erosion) and three primary sources of anthropogenic lead (coal combustion, gasoline additives, and municipal waste water discharges) to the lake. Lead concentrations and isotopic compositions of 210Pb-dated sediment cores record historical variations in the inputs from these sources. The heterogeneous isotopic composition of the three basins of Lake Erie indicates that lead from municipal effluent is most prominent in the urbanized western region of the lake and that atmospheric deposition is most prominent in the more rural eastern areas. Calculations based on a 207Pb 206Pb vs. 208Pb 206Pb linear mixing model show that as much as 70% of sediment in the Central Basin and 25% in the East Basin originates from the West Basin of Lake Erie. These calculations attest to the interbasinal redistribution of particle-reactive contaminants within the lake.

Transport of the environmental radionuclides in an alpine watershed

The radionuclides 137Cs, 210Pb and 7Be have been examined in the alpine Rhoˆne watershed (Switzerland) during a period of two years in order to evaluate their usefulness as tracers of the removal and transport rate of top-soil particles and particle-reactive contaminants of atmospheric origin. The specific activities of the radionuclides in fluvial suspension show a distinct seasonal pattern which depends on the hydrologic regime of the stream and the sources of the suspended matter. Input-output budgets based on the atmospheric deposition and fluvial removal of three radionuclides in the alpine Rhoˆne watershed are used to estimate their erosional residence times. The simplest one box model yields mean residence times of about 800 and 1400 years for 137Cs and 210Pb, respectively. The removal rate of short-lived 7Be suggests that a part of the watershed (0.6–2.3% of the total surface) is exposed to a rapid erosion, in which the mean residence time of the radionuclides is in the range of 1–220 days. This has little influence on the calculated residence time of 137Cs but increases the estimated residence time of 210Pb in soil to over 1800 years. The use of 210Pb- 7Be pair in fluvial output may be very helpful in the assessment of the impact of atmospheric pollutants on the water quality in rivers and lakes.