Mobility and Effects in Liner Clay of Fluorobenzene Tracer and Leachate     

E. M. Llgenfritz  Fred A. Blanchard  R. L. Masselink  Bijay K. Panigrahi 《Ground water》1988,26(1):22-30

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Speciation of organic carbon,Cu and Mn in the River Marne (France): the role of colloids     

A. Jaïry  B. Garban  M. Blanchard  A. Chesterikoff 《水文研究》1999,13(2):223-237

The distribution of organic carbon (OC) and of some metals (Cu, Mn) amongst the particulate (>0·2 μm), colloidal (10 kDa–0·2 μm) and the truly dissolved (<10 kDa) fractions of the River Marne was investigated during the phytoplankton spring bloom. A tangential ultrafiltration (UF) device was utilized to separate the colloidal fraction. On average, 22% of the OC, 31% of the Cu and 53% of the Mn, usually assigned to the so‐called dissolved fraction, were found in the colloidal fraction. The colloidal fraction exhibited a behaviour different from that of the particulate and truly dissolved fractions. Autochthonous production led to enrichment in the colloidal and particulate OC pools: up to 47% of the total dissolved OC was in the colloidal fraction. An increase in the colloidal metal fraction, concomitant with a fall in the truly dissolved fraction, coincided with peaks in phytoplankton during the bloom. These phenomena might be related either to an increase in pH associated with photosynthetic activity, resulting in the precipitation of truly dissolved forms into the colloidal fraction, or to scavenging of the truly dissolved metals by the algal species of colloidal size. The interaction between the colloidal and the truly dissolved phases was very important. The partition coefficients of the Cu and Mn between the colloidal and truly dissolved fractions were higher than between the particulate and the truly dissolved fractions. This pattern is consistent with a greater specific surface area of colloids than macroparticles. Consequently, the adsorption and complexation capacities are enhanced in the colloidal fraction of the particulate matter. The extraction of hydrophobic complexes with Cu using C₁₈ Sep‐Pak columns, showed that the Cu occurring in colloidal, total dissolved or truly dissolved forms was significantly complexed by the organic matter. The truly dissolved fraction might be complexed up to 100% during a phytoplankton bloom. Copyright © 1999 John Wiley & Sons, Ltd.  相似文献   

Atmospheric Mercury Concentrations from Several Observatory Sites in the Northern Hemisphere   总被引：4，自引：0，他引：4  

Ki-Hyun?KimEmail author  R.?Ebinghaus  W.?H.?Schroeder  P.?Blanchard  H.?H.?Kock  A.?Steffen  F.?A.?Froude  Min-Young?Kim  Sungmin?Hong  Jae-Hwan?Kim 《Journal of Atmospheric Chemistry》2005,50(1):1-24

In an effort to investigate both large-scale (spatial) and short/long-term (temporal) distribution characteristics of atmospheric mercury, we have combined and analyzed the Hg concentration data sets collected continuously by four different scientific groups for the areas and periods covering (1) America (three sites near the Canadian Great Lakes (CGL): 1997–2000), (2) Asia (Seoul, Korea (SEL): 1997–2002), (3) Arctic (Alert, Canada (ALT): 1995–2001), and (4) Europe (Mace Head, Ireland (MH): 1996–2002). The mean concentrations of Hg data from those widely dispersed monitoring stations were computed to be (1) 1.58 ± 0.23, 1.69 ± 0.32, and 1.93 ± 0.44 (three sites in CGL), (2) 5.06 ± 2.46 ng m^–3 (SEL), (3) 1.55 ± 0.41 (ALT), and (4) 1.76 ± 0.31 (MH). Intersite relationships were investigated among all different stations using the data groups divided into different temporal intervals. The analysis of diurnal variation patterns of Hg indicated differences in regional source/sink characteristics, with increasing amplitudes of variability toward areas under the strong influence of anthropogenic sources. When the analysis was made over different seasons, the patterns contrasted greatly between the Arctic and the other areas. It was found that the relative enhancement of Hg concentrations was dominant during winter/spring in most areas due to direct or indirect influences of anthropogenic emissions. However, the pattern for the Arctic area was distinguished pronouncedly from others with the spring minimum and summer maximum both of which reflect the potent effects of mercury depletion phenomenon (MDP). By contrast, no long-term trend, either being an increase or decrease, was evident from any of the stations during each respective study period. Although our initial attempts to examine the distribution characteristics of Hg analyzed by different scientific groups were successful, we feel that these efforts should be continued further to extend the compatibility of the global database of Hg.  相似文献   

Trophic importance of diatoms in an intertidal Zostera noltii seagrass bed: Evidence from stable isotope and fatty acid analyses     

Benoit Lebreton  Pierre Richard  Robert Galois  Gilles Radenac  Camille Pfléger  Gaël Guillou  Françoise Mornet  Gérard F. Blanchard 《Estuarine, Coastal and Shelf Science》2011

A current predominant paradigm emphasizes the role of epiphytic algae for invertebrates in most seagrass food webs. However, in some intertidal Zostera noltii beds, epiphyte biomass is very low compared to microphytobenthos and seagrass biomasses. We assessed the role of microphytobenthos in a temperate intertidal Z. noltii bed by combining stable isotope and fatty acid (FA) analyses on primary producers, composite sources — suspended particulate organic matter (SPOM) and sediment surface organic matter (SSOM) — and the main macrofaunal consumers. Z. noltii showed high δ¹³C (−9.9‰) and high 18:2(n-6) and 18:3(n-3) contents. Microphytobenthos was slightly more ¹³C-depleted (−15.4‰) and had high levels of diatom markers: 14:0, 16:1(n-7)c, 20:5(n-3). Low mean δ¹³C (−22.0‰) and large amounts of diatom and bacteria (18:1(n-7)c) markers indicated that SPOM was mainly composed of a mixture of fresh and decayed pelagic diatoms. Higher mean δ¹³C (−17.9‰) and high amounts of diatom FAs were found in SSOM, showing that microphytobenthic diatoms dominate. Very low percentages of 18:2(n-6) and 18:3(n-3) in consumers indicated a low contribution of Z. noltii material to their diets. Grazers, deposit and suspension-deposit feeders had δ¹³C close to microphytobenthos and high levels of diatom FAs, confirming that microphytobenthos represented the main part of their diet. Lower δ¹³C and higher amounts of flagellate FAs – 22:6(n-3) and 16:4(n-3) – in suspension feeders indicated that their diet resulted from a mixture of SPOM and microphytobenthos. These results demonstrate that invertebrates do not consume high amounts of seagrass and highlight the main role of benthic diatoms in this intertidal seagrass bed.  相似文献   

The Paris CM chondrite: Secondary minerals and asteroidal processing     

Yves Marrocchi  Matthieu Gounelle  Ingrid Blanchard  Florent Caste  Anton T. Kearsley 《Meteoritics & planetary science》2014,49(7):1232-1249

We report a petrographic and mineralogical survey of Paris, a new CM chondrite considered to be the least‐altered CM identified so far (Hewins et al. 2014 ). Compared to other CMs, Paris exhibits (1) a higher concentration of Fe‐Ni metal beads, with nickel contents in the range 4.1–8.1 wt%; (2) the systematic presence of thin lamellae and tiny blebs of pentlandite in pyrrhotite grains; and (3) ubiquitous tochilinite/cronstedtite associations with higher FeO/SiO₂ and S/SiO₂ ratios. In addition, Paris shows the highest concentration of trapped ³⁶Ar reported so far for a CM chondrite (Hewins et al. 2014 ). In combination with the findings of previous studies, our data confirm the reliability of (1) the alteration sequence based on the chemical composition of tochilinite/cronstedtite associations to quantify the fluid alteration processes and (2) the use of Cr content variability in type II ferroan chondrule olivine as a proxy of thermal metamorphism. In contrast, the scales based on (1) the Fe³⁺ content of serpentine in the matrix to estimate the degree of aqueous alteration and (2) the chemical composition of Fe‐Ni metal beads for quantifying the intensity of the thermal metamorphism are not supported by the characteristics of Paris. It also appears that the amount of trapped ³⁶Ar is a sensitive indicator of the secondary alteration modifications experienced by chondrites, for both aqueous alteration and thermal metamorphism. Considering Paris, our data suggest that this chondrite should be classified as type 2.7 as it suffered limited but significant fluid alteration and only mild thermal metamorphism. These results point out that two separated scales should be used to quantify the degree of the respective role of aqueous alteration and thermal metamorphism in establishing the characteristics of CM chondrites.  相似文献   

Theoretical study of the local charge compensation and spectroscopic properties of B-type carbonate defects in apatite     

Haohao Yi  Etienne Balan  Christel Gervais  Loïc Ségalen  Marc Blanchard  Michele Lazzeri 《Physics and Chemistry of Minerals》2014,41(5):347-359

The structure and spectroscopic properties of selected models of B-type carbonate defects in apatite locally compensated by fluoride or hydroxyl ions are investigated using first-principles quantum mechanical calculations. Theoretical infrared absorption spectra and ¹³C, and ¹⁹F nuclear magnetic resonance chemical shifts are determined. Among the investigated models, only the clumped (CO₃ ^2?, F^?) defect, with the carbonate group close to the sloping face of the tetrahedral site and the F^? ion at the remaining apex, corresponds to previous experimental observations performed on carbonate-fluorapatite samples. Although the substitution of hydroxyl by fluoride ions is commonly observed in minerals, the clumped (CO₃ ^2?, OH^?) defects are unlikely to occur in apatite, considering both their theoretical spectroscopic properties and relative stability. Anionic F^? for OH^? exchange between channel and B sites displays a preference of ~20 kJ/mol for the local charge compensation by fluoride ions at the B-site, pointing to a significantly different behavior of F^? and OH^? ions in the charge compensation mechanism. This difference is ascribed to the poor H-bond acceptor character of available oxygen atoms surrounding the apex of the tetrahedral site. The explicit calculation of the infrared absorption spectra of the defect models is also used to interpret the significant difference observed in the linewidth of the ν₂ and ν₃ CO₃ infrared powder absorption bands of carbonated apatite samples. It is shown that for a concentration of 4.4 wt% of CO₂, long-range electrostatic effects already significantly contribute to the broadening of the ν₃ CO₃ bands in apatite.  相似文献   

Experimental and theoretical study of the vibrational properties of diaspore (α-AlOOH)     

Simon?Delattre  Etienne?BalanEmail author  Michele?Lazzeri  Marc?Blanchard  Maxime?Guillaumet  Olivier?Beyssac  Eiken?Haussühl  Bj?rn?Winkler  Ekhard?K.?H.?Salje  Georges?Calas 《Physics and Chemistry of Minerals》2012,39(2):93-102

Vibrational properties of diaspore, α-AlOOH, have been re-investigated using room-temperature single-crystal Raman spectroscopy and low-temperature powder infrared (IR) transmission spectroscopy. First-principles harmonic calculations based on density functional theory provide a convincing assignment of the major Raman peaks and infrared absorption bands. The large width of the Raman band related to OH stretching modes is ascribed to mode–mode anharmonic coupling due to medium-strength H-bonding. Additional broadening in the powder IR spectrum arises from depolarization effects in powder particles. The temperature dependence of the IR spectrum provides a further insight into the anharmonic properties of diaspore. Based on their frequency and temperature behavior, narrow absorption features at ~2,000 cm⁻¹ and anti-resonance at ~2,966 cm⁻¹ in the IR spectrum are interpreted as overtones of fundamental bending bands.  相似文献   

Analysis of Radionuclide Releases from the Fukushima Dai-ichi Nuclear Power Plant Accident Part II     

Pascal Achim  Marguerite Monfort  Gilbert Le Petit  Philippe Gross  Guilhem Douysset  Thomas Taffary  Xavier Blanchard  Christophe Moulin 《Pure and Applied Geophysics》2014,171(3-5):645-667

The present part of the publication (Part II) deals with long range dispersion of radionuclides emitted into the atmosphere during the Fukushima Dai-ichi accident that occurred after the March 11, 2011 tsunami. The first part (Part I) is dedicated to the accident features relying on radionuclide detections performed by monitoring stations of the Comprehensive Nuclear Test Ban Treaty Organization network. In this study, the emissions of the three fission products Cs-137, I-131 and Xe-133 are investigated. Regarding Xe-133, the total release is estimated to be of the order of 6 × 10¹⁸ Bq emitted during the explosions of units 1, 2 and 3. The total source term estimated gives a fraction of core inventory of about 8 × 10¹⁸ Bq at the time of reactors shutdown. This result suggests that at least 80 % of the core inventory has been released into the atmosphere and indicates a broad meltdown of reactor cores. Total atmospheric releases of Cs-137 and I-131 aerosols are estimated to be 10¹⁶ and 10¹⁷ Bq, respectively. By neglecting gas/particulate conversion phenomena, the total release of I-131 (gas + aerosol) could be estimated to be 4 × 10¹⁷ Bq. Atmospheric transport simulations suggest that the main air emissions have occurred during the events of March 14, 2011 (UTC) and that no major release occurred after March 23. The radioactivity emitted into the atmosphere could represent 10 % of the Chernobyl accident releases for I-131 and Cs-137.  相似文献   

Iron isotope fractionation between pyrite (FeS₂), hematite (Fe₂O₃) and siderite (FeCO₃): A first-principles density functional theory study     

Marc Blanchard  Franck Poitrasson  Michele Lazzeri  Etienne Balan 《Geochimica et cosmochimica acta》2009,73(21):6565-776

In addition to equilibrium isotopic fractionation factors experimentally derived, theoretical predictions are needed for interpreting isotopic compositions measured on natural samples because they allow exploring more easily a broader range of temperature and composition. For iron isotopes, only aqueous species were studied by first-principles methods and the combination of these data with those obtained by different methods for minerals leads to discrepancies between theoretical and experimental isotopic fractionation factors. In this paper, equilibrium iron isotope fractionation factors for the common minerals pyrite, hematite, and siderite were determined as a function of temperature, using first-principles methods based on the density functional theory (DFT). In these minerals belonging to the sulfide, oxide and carbonate class, iron is present under two different oxidation states and is involved in contrasted types of interatomic bonds. Equilibrium fractionation factors calculated between hematite and siderite compare well with the one estimated from experimental data (ln α⁵⁷Fe/⁵⁴Fe = 4.59 ± 0.30‰ and 5.46 ± 0.63‰ at 20 °C for theoretical and experimental data, respectively) while those for Fe(III)_aq-hematite and Fe(II)_aq-siderite are significantly higher that experimental values. This suggests that the absolute values of the reduced partition functions (β-factors) of aqueous species are not accurate enough to be combined with those calculated for minerals. When compared to previous predictions derived from Mössbauer or INRXS data [Polyakov V. B., Clayton R. N., Horita J. and Mineev S. D. (2007) Equilibrium iron isotope fractionation factors of minerals: reevaluation from the data of nuclear inelastic resonant X-ray scattering and Mössbauer spectroscopy. Geochim. Cosmochim. Acta71, 3833-3846], our iron β-factors are in good agreement for siderite and hematite while a discrepancy is observed for pyrite. However, the detailed investigation of the structural, electronic and vibrational properties of pyrite as well as the study of sulfur isotope fractionation between pyrite and two other sulfides (sphalerite and galena) indicate that DFT-derived β-factors of pyrite are as accurate as for hematite and siderite. We thus suggest that experimental vibrational density of states of pyrite should be re-examined.  相似文献   

Early burial mud diapirism and its impact on stratigraphic architecture in the Carboniferous of the Shannon Basin,County Clare,Ireland     

Sbastien Blanchard  Edward J. Matheson  Christopher R. Fielding  James L. Best  Alexander B. Bryk  Kalin J. Howell  Charles C. Monson  Gosia Mahoney  Jeffrey Peakall 《Sedimentology》2019,66(1):329-361

Delta fronts are often characterized by high rates of sediment supply that result in unstable slopes and a wide variety of soft‐sediment deformation, including the formation of overpressured and mobile muds that may flow plastically during early burial, potentially forming mud diapirs. The coastal cliffs of County Clare, western Ireland, expose Pennsylvanian (Namurian) delta‐front deposits of the Shannon Basin at large scale and in three dimensions. These deposits include decametre‐scale, internally chaotic mudstone masses that clearly impact the surrounding sedimentary strata. Evidence indicates that these were true mud (unlithified sediment) diapirs that pierced overlying strata. This study documents a well‐exposed ca 20 m tall mud diapir and its impact on the surrounding mouth‐bar deposits of the Tullig Cyclothem. A synsedimentary fault and associated rollover dome, evident from stratal thicknesses and the dip of the beds, define one edge of the diapir. These features are interpreted as recording the reactive rise of the mud diapir in response to extensional faulting along its margin. Above the diapir, heterolithic sandstones and siltstones contain evidence for the creation of localized accommodation, suggesting synsedimentary filling, tilting and erosion of a shallow sag basin accommodated by the progressive collapse of the diapir. Two other diapirs are investigated using three‐dimensional models built from ‘structure from motion’ drone imagery. Both diapirs are interpreted to have grown predominantly through passive rise (downbuilding). Stratal relationships for all three diapirs indicate that they were uncompacted and fluid‐rich mud beds that became mobilized through soft‐sediment deformation during early burial (i.e. <50 m, likely <10 m depth). Each diapir locally controlled the stratigraphic architecture in the shallow subsurface and potentially influenced local palaeocurrents on the delta. The mud diapirs studied herein are distinct from deeper ‘shale diapirs’ that have been inferred from seismic sections worldwide, now largely disputed.  相似文献