Environmental records of carbonaceous fly-ash particles from fossil-fuel combustion

Analysis of fly-ash particles in lake sediments has become increasingly important in studies of environmental pollution and lake acidification history. Most fly-ash studies have concerned black spheroidal carbonaceous particles (SCP)(>5 m) produced from oil and coal combustion. This review paper provides a summary of this technique and its application, and focusses on our investigations in Sweden between 1979 and 1993. It consists of five parts: i) preparation and analysis methods, ii) historical trends in atmospheric deposition, iii) geographical surveys of atmospheric deposition, iv) sediment dating, and v) studies of sedimentation processes in lakes. Methods for preparation and analyses of SCP have been developed and applied to investigations using sediment, soil and snow samples. Stratigraphic trends of SCP concentrations in lake-sediment cores reflect the consumption history of fossil fuels. A characteristic temporal SCP pattern, with a marked concentration increase beginning after the 1940's and a peak in the early 1970's, has been recognized in most Swedish lakes and elsewhere in Europe. A survey of SCP concentrations in surface sediments of >100 lakes covering Sweden demonstrated that polluted areas in southern Sweden had >100 times higher SCP concentrations than clean areas in the north. The spatial distribution of SCP over Sweden is similar to the deposition pattern of long-range transported airborne pollutants, such as excess sulphate monitored by network stations. SCP also accumulate in soils, and soil analyses can be used for determining the integrated historical deposition of SCP at the local or regional scale. Finally, SCP have been used for indirect dating of sediment cores and as a marker to assess sediment distribution patterns within lake basins.     

Evidence of magmatic CO2-rich fluids in peraluminous graphite-bearing leucogranites from Deep Freeze Range (northern Victoria Land,Antarctica)

Fine-grained peraluminous synkinematic leuco-monzogranites (SKG), of Cambro-Ordovician age, occur as veins and sills (up to 20–30 m thick) in the Deep Freeze Range, within the medium to high-grade metamorphics of the Wilson Terrane. Secondary fibrolite + graphite intergrowths occur in feldspars and subordinately in quartz. Four main solid and fluid inclusion populations are observed: primary mixed CO₂+H₂O inclusions + Al₂SiO₅ ± brines in garnet (type 1); early CO₂-rich inclusions (± brines) in quartz (type 2); early CO₂+CH₄ (up to 4 mol%)±H₂O inclusions + graphite + fibrolite in quartz (type 3); late CH₄+CO₂+N₂ inclusions and H₂O inclusions in quartz (type 4). Densities of type 1 inclusions are consistent with the crystallization conditions of SKG (750°C and 3 kbar). The other types are post-magmatic: densities of type 2 and 3 inclusions suggest isobaric cooling at high temperature (700–550°C). Type 4 inclusions were trapped below 500°C. The SKG crystallized from a magma that was at some stage vapour-saturated; fluids were CO₂-rich, possibly with immiscible brines. CO₂-rich fluids (±brines) characterize the transition from magmatic to post-magmatic stages; progressive isobaric cooling (T<670°C) led to a continuous decrease off _{O 2} can entering in the graphite stability field; at the same time, the feldspars reacted with CO₂-rich fluids to give secondary fibrolite + graphite. Decrease ofT andf _{O 2} can explain the progressive variation in the fluid composition from CO₂-rich to CH₄ and water dominated in a closed system (in situ evolution). The presence of N₂ the late stages indicates interaction with external metamorphic fluids.Contribution within the network Hydrothermal/metamorphic water-rock interactions in crystalline rocks: a multidisciplinary approach on paleofluid analysis. CEC program: Human Capital and Mobility     

Evidence of recent climatic anomalies at Trieste (Italy)

A recent noticeable climatic anomaly in some meteomarine quantities is analysed based on observations during the period March 1, 1971-February 28, 1993 taken in Trieste (Italy). Marked deviations from the normal values of the coupled quantities atmospheric pressure-solar irradiance and atmospheric pressure-sea level elevation, during the last 22 years, are analysed. The procedures used bring out a clear and persistent configuration of high pressure, high irradiance and low sea level from 1989 on, previously unmatched.     

Regional Seas and Sustainable Development Results of an International Workshop

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Regional Seas and Sustainable Development Results of an International Workshop     

Search for nucleosynthetic and radiogenic tellurium isotope anomalies in carbonaceous chondrites

Tellurium isotope data acquired by multiple-collector inductively coupled plasma-mass spectrometry (MC-ICPMS) are presented for sequential acid leachates of the carbonaceous chondrites Orgueil, Murchison, and Allende. Tellurium isotopes are produced by a broad range of nucleosynthetic pathways and they are therefore of particular interest given the isotopic anomalies previously identified for other elements in these meteorites. In addition, the data provide new constraints on the initial solar system abundance of the r-process nuclide ¹²⁶Sn, which decays to ¹²⁶Te with a half-life of 234,500 years. The ¹²⁶Te/¹²⁸Te ratios of all leachates were found to be identical, within uncertainty, despite variations in ¹²⁴Sn/¹²⁸Te of between about 0.002 and 1.4. The data define a ¹²⁶Sn/¹²⁴Sn ratio of <7.7 × 10⁻⁵ at the time of last isotopic closure, consistent with the value of <18 × 10⁻⁵ previously reported for bulk carbonaceous chondrites. How close this is to the initial ¹²⁶Sn/¹²⁴Sn ratio of the solar system depends on when the investigated samples last experienced redistribution of Sn and Te. No clear evidence is found for nucleosynthetic anomalies in the abundances of p-, s-, and r-process nuclides. The largest effect detected in this study is a small excess of the r-process nuclide ¹³⁰Te in a nitric acid leachate of Murchison. This fraction displays an anomalous ε¹³⁰Te of +3.5 ± 2.5. Although barely resolvable given the analytical uncertainties, this is consistent with the presence of a small excess r-process component or an s-process deficit. The general absence of anomalies contrasts with previous results obtained for K, Cr, Zr, Mo, and Ba isotopes in similar leachates, which display nucleosynthetic anomalies of up to 3.8%. The reason for this discrepancy is unclear but it may reflect volatility and more efficient mixing of Te in the solar nebula.     

Elucidation of different forms of organic carbon in marine sediments from the Atlantic coast of Spain using thermal analysis coupled to isotope ratio and quadrupole mass spectrometry

Analysis of river, estuary and marine sediments from the Atlantic coast of Spain using thermogravimetry–differential scanning calorimetry–quadrupole mass spectrometry–isotope ratio mass spectrometry (TG–DSC–QMS–IRMS) was used to (a) distinguish bulk chemical hosts for C within a sediment and humic acid fraction, (b) track C pools with differing natural C isotope ratios and (c) observe variation with distance from the coast. This is the first application of such a novel method to the characterisation of organic matter from marine sediments and their corresponding humic acid fractions. Using thermal analysis, a labile, a recalcitrant and a refractory carbon pool can be distinguished. Extracted humic fractions are mainly of recalcitrant nature. The proportion of refractory carbon is greatest in marine sediments and humic acid fractions. Quadrupole mass spectrometry confirmed that the greatest proportion of m/z 44 (CO₂) and m/z 18 (H₂O) were detected at temperatures associated with recalcitrant carbon (510–540 °C). Isotope analysis detected progressive enrichment in δ¹³C for the sediment samples with an increase in marine influence. Isotopic heterogeneity in the refractory organic matter in marine sediments could be due to products of anthropogenic origin or natural combustion products. Isotope homogeneity of humic acids confirms the presence of terrigenous C in marine sediments, allowing the terrestrial input to be characterised.     

Multiple magnetization events in the Red River carbonates, Williston Basin, Canada: Evidence for fluid-flow?

Samples collected from the Upper Ordovician Red River carbonates in a well at the centre of the Williston Basin revealed two paleomagnetic components with different inclinations, 60.3 ± 3.9° (k = 70.7, N = 12) and 20.4 ± 3.3° (k = 141.2, N = 8), but similar declination values in individual specimens. Inclination-only analysis indicates two possible scenarios for the age of these two magnetizations: in scenario (a) the timing of magnetization happened sometime between Late Ordovician to Devonian; and in scenario (b) there are two different remagnetizations, one that overlaps Pennsylvanian to Permian time while the other can have either a Late Jurassic or a Tertiary age. Whereas dolomitization and some isotopic data tend to support scenario (a), previous paleomagnetic data from the Williston Basin and from younger units in the same well, the tectonic evolution of the basin, and the hydrocarbon maturation pattern in the Red River carbonates all favour chemical remagnetization(s) driven by orogenic fluids during the Alleghenian and Laramide orogenies.     

The bimodal rift-related Juscelândia volcanosedimentary sequence in central Brazil: Mesoproterozoic extension and Neoproterozoic metamorphism

The Barro Alto Complex and Juscelândia volcanosedimentary sequence are exposed in the central part of the Neoproterozoic Brasília belt of central Brazil. The former is a large (approximately 150 km long), boomerang-shaped, mafic-ultramafic, layered complex formed by two different intrusions metamorphosed under granulite facies. These rocks are tectonically overlain by rocks of the Juscelândia volcanosedimentary sequence, represented mainly by biotite-gneiss and amphibolite, or amphibolite facies metamorphic equivalents of rhyolite and basalt, respectively. New SIMS U–Pb zircon data and Sm–Nd isochron data presented herein help clarify the igneous and metamorphic evolution of the Juscelândia volcanosedimentary sequence, as well as its relationship with the Barro Alto Complex. Zircon grains from two biotite gneisses were analyzed by SIMS (SHRIMP) and indicate Mesoproterozoic dates, approximately 1.28 Ga, interpreted as the time of bimodal volcanism in a tectonic setting transitional between a continental rift and an ocean basin. Metamorphism is constrained by Sm–Nd garnet-whole-rock isochrons for garnet amphibolite and pelitic schists of the Juscelândia sequence, as well as for clinopyroxene-garnet amphibolite and garnet granulite of the Barro Alto Complex, which give ages between 0.74 and 0.76 Ga, in agreement with SIMS dates for metamorphic zircon rims. These new data are significant, because they establish that a single metamorphic event affected both the Barro Alto Complex and the Juscelândia sequence. Based on these new data, we present a modified tectonic model for the Brasília belt.