Anthropogenic activities including metal contamination create well-known problems in coastal mangrove ecosystems but understanding and linking specific pollution sources to distinct trophic levels within these environments is challenging. This study evaluated anthropogenic impacts on two contrasting mangrove food webs, by using stable isotopes (δC, δN, Sr/Sr, Pb/Pb and Pb/Pb) measured in sediments, mangrove trees (Rhizophora mangle, Laguncularia racemosa, Avicennia schaueriana), plankton, shrimps (Macrobranchium sp.), crabs (Aratus sp.), oysters (Crassostrea rhizophorae) and fish (Centropomus parallelus) from both areas. Strontium and Pb isotopes were also analysed in water and atmospheric particulate matter (PM). δN indicated that crab, shrimp and oyster are at intermediate levels within the local food web and fish, in this case C. parallelus, was confirmed at the highest trophic level. δN also indicates different anthropogenic pressures between both estuaries; Vitória Bay, close to intensive human activities, showed higher δN across the food web, apparently influenced by sewage. The ratioSr/Sr showed the primary influence of marine water throughout the entire food web. Pb isotope ratios suggest that PM is primarily influenced by metallurgical activities, with some secondary influence on mangrove plants and crabs sampled in the area adjacent to the smelting works. To our knowledge, this is the first demonstration of the effect of anthropogenic pollution (probable sewage pollution) on the isotopic fingerprint of estuarine-mangrove systems located close to a city compared to less impacted estuarine mangroves. The influence of industrial metallurgical activity detected using Pb isotopic analysis of PM and mangrove plants close to such an impacted area is also notable and illustrates the value of isotopic analysis in tracing the impact and species affected by atmospheric pollution.
We present an advanced method to produce accurate and reproducible U and Th isotope data for carbonate geochronology using very small sample sizes. We analysed speleothem, marine calcite and coral samples by MC-ICP-MS and compared the data and its precision to U and Th data obtained by TIMS using the same samples. MC-ICP-MS needs between 0.05 and 0.34 ng of Th compared with 0.3-1.4 ng Th for TIMS analyses to obtain comparable precision. No separation of Th and U is necessary because of U and Th recoveries of circa 100% and 75-100%, respectively. Th and U analyses are carried out for a range from masses 228 to 238 in two separate runs, with mass 230 Th on the Daly detector for measuring Th isotope ratios and 234 U on the Daly detector for measuring U isotope ratios. Silicate rock standard ''Table Mountain Latite'' (TML) 235 U/ 238 U ratios are used to correct for instrumental mass bias. For calibrating the gain of the Daly and Faraday detectors (Daly-Faraday gain), a 1 ppt Aldrich U solution spiked with 233 U-236 U double spike is measured with mass 235 U in the Daly detector. We demonstrate the accuracy and precision of our analytical data obtained for standard solution UCSC-Th-A, the TML and eleven spiked TML samples over the past 10 months. Literature data obtained by both TIMS and MC-ICP-MS lie well within the error of our UCSC-Th-A 230 Th/ 232 Th value of 0.000 005 85 ¡ 5 (2 sd, n ~29). Our ( 234 U/ 238 U) and ( 230 Th/ 238 U) activity ratios for the TML compare well with results of other MC-ICP-MS studies. Our external precision of 230 Th/ 232 Th and 234 U/ 238 U ratios for the unspiked TML is slightly worse than other MC-ICP-MS studies, but reflects either significantly smaller sample sizes or much shorter time for measurement.
In many forest ecosystems, plant-available pools of Mg, Ca, and K are assumed to be stored in the soil as exchangeable cations adsorbed on the cation exchange complex (exchangeable pools). However, between soil minerals and exchangeable cations exists a gradient of Mg, Ca, and K storage forms that have not been fully characterized and may play an important role in plant nutrition and biogeochemical cycles. We hypothesize that sources of Mg, Ca, and K in the soil other than the conventionally measured exchangeable pools are plant-available on very short time scales (<1 day). In the present study, we developed and applied an isotopic dilution technique using the stable isotopes 26Mg, 44Ca, and 41K to trace and quantify the pools of Mg, Ca, and K (isotopically exchangeable pools) in the soil of a hardwood forest that contribute directly to equilibrium processes between the soil water and the soil. We characterize the equilibrium between the soil and soil solution using both a batch approach and a flow-through approach in order (i) to develop and determine the best routine method to measure the isotopically exchangeable pools and (ii) to further the characterization of the forms of storage of Mg, Ca, and K in the isotopically exchangeable pools. We first show that the flow-through reactor approach (equilibrium in unsaturated soil columns) is the most adequate to measure the isotopically exchangeable pools with the fewest equilibrium disturbances. We then show that isotopically exchangeable pools of Mg, Ca, and K are greater than traditionally measured exchangeable pools. The isotopically exchangeable pools of Mg, Ca, and K are mainly composed of traditionally measured exchangeable pools (88.8–98.5% for Mg, 74.7–97.7% for Ca, and 68.7–77.1% for K) but are also composed of pools extracted with the Tamm reagent (oxalic acid, pH 3) and nitric acid (1 mol·L–1): 1.5–11.2% for Mg, 2.3–25.3% for Ca, and 22.9–31.3% for K. Storage forms of Mg, Ca, and K in the isotopically exchangeable pool could include chelation with soil organic matter, retention on soil aluminum and iron oxides and hydroxides through phosphate and/or organic acid bridges and site-specific adsorption. The isotopic dilution method is a relevant tool to quantify the plant-available pools of Mg, Ca, and K on short time scales (source and sink pools) and is a very promising approach to characterize and quantify the processes responsible for the depletion and/or replenishment of these pools over longer time scales.
Abstract. The study of geological archives of dust is of great relevance as they are directly linked to past atmospheric circulation and bear the potential to reconstruct dust provenance and flux relative to climate changes. Among the dust sinks, loess–palaeosol sequences (LPSs) represent the only continental and non-aquatic archives that are predominantly built up by dust deposits close to source areas, providing detailed information on Quaternary climatic and terrestrial environmental changes. Upper Pleistocene LPSs of western central Europe have been investigated in great detail showing their linkage to millennial-scale northern hemispheric climate oscillations, but comprehensive data on dust composition and potential source–sink relationships as well as inferred past atmospheric circulation patterns for this region are still fragmentary. Here, we present an integrative approach that systematically combines sedimentological, rock magnetic, and bulk geochemical data, as well as information on Sr and Nd isotope composition, enabling a synthetic interpretation of LPS formation. We focus on the Schwalbenberg RP1 profile in the Middle Rhine Valley in Germany and integrate our data into a robust age model that has recently been established based on high-resolution radiocarbon dating of earthworm calcite granules. We show that Schwalbenberg RP1 is subdivided into a lower section corresponding to late oxygen isotope stage 3 (OIS; ∼ 40–30 ka) and an upper section dating into the Last Glacial Maximum (LGM; ∼ 24–22 ka), separated by a major stratigraphic unconformity. Sedimentological proxies of wind dynamics (U ratio) and pedogenesis (finest clay) of the lower section attest to comparable and largely synchronous patterns of northern hemispheric climatic changes supporting the overall synchronicity of climatic changes in and around the North Atlantic region. The anisotropy of magnetic susceptibility (AMS) reveals a clear correlation between finer grain size and increasing AMS foliation within interstadials, possibly owing to continuous accumulation of dust during pedogenic phases. Such a clear negative correlation has so far not been described for any LPS on stadial–interstadial scales. Distinct shifts in several proxy data supported by changes in isotope composition (87Sr/86Sr and εNd) within the lower section are interpreted as changes in provenance and decreasing weathering simultaneously with an overall cooling and aridification towards the end of OIS 3 (after ∼ 35 ka) and enhanced wind activity with significant input of coarse-grained material recycled from local sources related to increased landscape instability (after ∼ 31.5 ka). We find that environmental conditions within the upper section, most likely dominated by local to regional environmental signals, significantly differ from those in the lower section. In addition, AMS-based reconstructions of near-surface wind trends may indicate the influence of north-easterly winds beside the overall dominance of westerlies. The integrative approach contributes to a more comprehensive understanding of LPS formation including changes in dust composition and associated circulation patterns during Quaternary climate changes.
<p>Loess-Palaeosol-Sequences (LPS) are the most widespread aeolian sedimentary deposits providing climatic- and environmental records across continents. As dust sinks, they may archive information on dust source dynamics, if targeted source signals survived processes operating during production, transport, and syn- and post-depositional alteration of particles and sediments. Yet, our knowledge about such dynamics through palaeoenvironmental changes during the Upper Pleistocene remains vague. This limits our understanding of thresholds that may have (de-) activated dust sources causing major environmental changes in prevalent areas. We thus combine results of isotope- (<sup>87/86</sup>Sr, <sup>143/144</sup>Nd) and major element (Si/Al) provenance proxies that react differently to pre-, syn- and post depositional alteration processes, with granulometry (U-ratio) and the anisotropy of magnetic susceptibility (AMS). Granulometry is recognised as an indicator for wind strengths and the primary magnetic fabric of loess deposits has been successfully used to reconstruct surface near wind directions. We apply our approach on the RP1 profile of the Schwalbenberg LPS that covers the late OIS 3 and the OIS 2 in centennial-scale resolution. The site is embedded in the Middle Rhine Valley (Germany) dividing the Rhenish Massif in its western and eastern part. Consequently, the Schwalbenberg seems appropriate to trace provenance shifts as it is linked to a distal dust source via the Rhine and as it is surrounded by potential local dust sources of the Rhenish Massif. Our results indicate shifts in source areas NNE-SSW off the site, contemporary with increasing frost dynamics and aridification. Both factors seem to enhance dust inputs from the Rhine system up to a threshold where the Rhenish Massif gets activated as a dominant source. Geochemical fingerprinting and AMS at the Schwalbenberg RP1 LPS reveal insights into dust source dynamics that allow for estimating their emission potential during Upper Pleistocene palaeoenvironmental changes. &#160;</p>
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