We performed a risk assessment of metal exposure to population subgroups living on, and growing food on, urban sites. We modeled uptake of cadmium, copper, nickel, lead, and zinc for a selection of commonly grown allotment and garden vegetables. Generalized linear cross-validation showed that final predictions of Cd, Cu, Ni, and Zn content of food crops were satisfactory, whereas the Pb uptake models were less robust. We used predicted concentrations of metals in the vegetables to assess the risk of exposure to human populations from homegrown food sources. Risks from other exposure pathways (consumption of commercially produced foodstuffs, dust inhalation, and soil ingestion) were also estimated. These models were applied to a geochemical database of an urban conurbation in the West Midlands, United Kingdom. Risk, defined as a "hazard index," was mapped for three population subgroups: average person, highly exposed person, and the highly exposed infant (assumed to be a 2-year-old child). The results showed that food grown on 92% of the urban area presented minimal risk to the average person subgroup. However, more vulnerable population subgroups (highly exposed person and the highly exposed infant) were subject to hazard index values greater than unity. This study highlights the importance of site-specific risk assessment and the "suitable for use" approach to urban redevelopment.
We characterise the sources, pathways and export fluxes of particulate organic carbon (POC) in a headwater catchment in the Swiss Alps, where suspended sediment has a mean organic carbon concentration of 1.45% ± 0.06 . By chemically fingerprinting this carbon and its potential sources using carbon and nitrogen elemental and isotopic compositions, we show that it derives from binary mixing between bedrock and modern biomass with a soil-like composition. The hillslope and channel are strongly coupled, allowing runoff to deliver recent organic carbon directly to the stream beyond a moderate discharge threshold. At higher flows, more biomass is mobilized and the fraction of modern carbon in the suspended load reaches 0.70, increased from 0.30 during background conditions. Significant amounts of non-fossil organic carbon are thus transferred from the hillslope without the need for extreme events such as landsliding. Precipitation is key: as soon as the rain stops, biomass supply ceases and fossil carbon again dominates. We use rating curves modeled using samples from five storm events integrated over 29-year discharge records to calculate long-term export fluxes of total POC and non-fossil POC from the catchment of 23.3 ± 5.8 and 14.0 ± 4.4 tonnes km -2 yr -1 respectively. These yields are comparable to those from active mountain belts, yet the processes responsible are much more widely applicable.Such settings have the potential to play a significant role in the global drawdown of carbon dioxide via riverine biomass erosion, and their contribution to the global flux of POC to the ocean may be more important than previously thought.
Summary Isotopically exchangeable cadmium and zinc (‘E values’) were measured on soils historically contaminated by sewage sludge and ones on zinc‐rich mine spoil. The E‐value assay involves determining the distribution of an added metal isotope, e.g. 109Cd, between the solid and solution phases of a soil suspension. The E values for both metals were found to be robust to changes in the position of the metal solid⇔solution equilibrium, even though the concentration of dissolved metal varied substantially with electrolyte composition and soil:solution ratio. Concentration of labile metal was also invariant over isotope equilibration times of 2–6 days. The use of a submicron filtration procedure, in addition to centrifuging at 2200 g, proved unnecessary if 0.1 m Ca electrolyte was used to suspend the soils. The proportion of ‘fixed’ metal, in non‐labile forms, apparently increased with increasing pH, although there was considerable variation in both sets of contaminated soil. Zinc and cadmium in the sludged soils were similarly labile. Several possible methods for the measurement of chemically reactive metal were explored for comparison with E values, including single extraction with 1 m CaCl2 and a ‘pool depletion’ (PD) method. The latter involves comparing solid⇔solution metal equilibria in two electrolytes with differing degrees of (solution) complex formation, 0.1 m Ca(NO3)2 and CaCl2. Both the single extraction and the PD method gave good estimates of E value for Cd, although the single extraction was more consistent. Neither technique was a useful substitute for determining labile Zn, because of weak chloro‐complexation of Zn2+. We therefore suggest that 1 m CaCl2 extraction of Cd alone be used as an alternative to E values to avoid the inconvenience of isotopic dilution procedures.
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The two approaches most commonly applied to characterizing the chemical form and 'reactivity' of metals in the soil solid phase are sequential extraction procedures (SEPs) and isotopic dilution (ID). The development and limitations of both approaches are described and their application to contaminated soils discussed. It may be argued that ID offers a better means of discriminating between 'reactive' and 'inert' forms of metal. However, the literature on SEPs is considerably larger, providing greater scope for comparative analysis of new data. Although ID methods are subject to operational constraints, the procedural dependency of SEPs is probably much greater. Thus greater effort has been expended to standardize and verify methodologies for SEPs. However, despite achieving a level of 'political ratification' at the procedural level, the use of SEPs within risk assessments for planning or development purposes is currently almost absent. The future for ID methods in this context may lie in site-specific risk assessments that include improved methods for the prediction of metal solubility and bioavailability.
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