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101.
102.
Several different inventories of global and regional anthropogenic and biomass burning emissions are assessed for the 1980?C2010 period. The species considered in this study are carbon monoxide, nitrogen oxides, sulfur dioxide and black carbon. The inventories considered include the ACCMIP historical emissions developed in support of the simulations for the IPCC AR5 assessment. Emissions for 2005 and 2010 from the Representative Concentration Pathways (RCPs) are also included. Large discrepancies between the global and regional emissions are identified, which shows that there is still no consensus on the best estimates for surface emissions of atmospheric compounds. At the global scale, anthropogenic emissions of CO, NOx and SO2 show the best agreement for most years, although agreement does not necessarily mean that uncertainty is low. The agreement is low for BC emissions, particularly in the period prior to 2000. The best consensus is for NOx emissions for all periods and all regions, except for China, where emissions in 1980 and 1990 need to be better defined. Emissions of CO need better quantification in the USA and India for all periods; in Central Europe, the evolution of emissions during the past two decades needs to be better determined. The agreement between the different SO2 emissions datasets is rather good for the USA, but better quantification is needed elsewhere, particularly for Central Europe, India and China. The comparisons performed in this study show that the use of RCP8.5 for the extension of the ACCMIP inventory beyond 2000 is reasonable, until more global or regional estimates become available. Concerning biomass burning emissions, most inventories agree within 50?C80%, depending on the year and season. The large differences between biomass burning inventories are due to differences in the estimates of burned areas from the different available products, as well as in the amount of biomass burned.  相似文献   
103.
Aliphatic (AHs) and polycyclic aromatic hydrocarbons (PAHs) were analyzed in dissolved and particulate material from surface microlayer (SML) and subsurface water (SSW) sampled at nearshore observation stations, sewage effluents and harbour sites from Marseilles coastal area (Northwestern Mediterranean) in 2009 and 2010. Dissolved and particulate AH concentrations ranged 0.05–0.41 and 0.04–4.3 μg l−1 in the SSW, peaking up to 38 and 1366 μg l−1 in the SML, respectively. Dissolved and particulate PAHs ranged 1.9–98 and 1.9–21 ng l−1 in the SSW, amounting up 217 and 1597 ng l−1 in the SML, respectively. In harbours, hydrocarbons were concentrated in the SML, with enrichment factors reaching 1138 for particulate AHs. Besides episodic dominance of biogenic and pyrogenic inputs, a moderate anthropisation from petrogenic sources dominated suggesting the impact of shipping traffic and surface runoffs on this urbanised area. Rainfalls increased hydrocarbon concentrations by a factor 1.9–11.5 in the dissolved phase.  相似文献   
104.
Hourly resolved cave air PCO2 and cave drip water hydrochemical data illustrate that calcite deposition on stalagmites can be modulated by prior calcite precipitation (PCP) on extremely short timescales. A very clear second-order covariation between cave air PCO2 and drip water Ca2+ concentrations during the winter months demonstrates the effects of degassing-induced PCP on drip water chemistry. Estimating the strength of the cave air PCO2 control on PCP is possible because the PCP signal is so clear; at our drip site a one ppm shift in Ca2+ concentrations requires a PCO2 shift of between 333 and 667 ppm. This value will undoubtedly vary from site to site, depending on drip water flow rate, residence time, drip water-cave air PCO2 differential, and availability of low PCO2 void spaces in the vadose zone above the cave. High-resolution cave environmental measurements were used to model calcite deposition on one stalagmite in Crag Cave, SW Ireland, and modelled growth over the study period (222 μm over 171 days) is extremely similar to the amount of actual calcite growth (240 μm) over the same time interval, strongly suggesting that equations used to estimate stalagmite growth rates are valid. Although cave air PCO2 appears to control drip water hydrochemistry in the winter, drip water dilution caused by rain events may have played a larger role during the summer, as evidenced by a series of sudden drops in Ca2+ concentrations (dilution) followed by much more gradual increases in drip water Ca2+ concentrations (slow addition of diffuse water). This research demonstrates that PCP on stalactites, cave ceilings, and void spaces within the karst above the cave partially controls drip water chemistry, and that thorough characterisation of this process at individual caves is necessary to most accurately interpret climate records from those sites.  相似文献   
105.
Brines in Cambrian sandstones and Ordovician dolostones of the St-Lawrence Lowlands at Bécancour, Québec, Canada were sampled for analysis of all stable noble gases in order to trace their origin and migration path, in addition to quantifying their residence time. Major ion chemistry indicates that the brines are of Na-Ca-Cl type, possibly derived from halite dissolution. 87Sr/86Sr ratios and Ca excess indicate prolonged interactions with silicate rocks of the Proterozoic Grenville basement or the Cambrian Potsdam sandstone. The brines constrain a 2-3% contribution of mantle 3He and large amounts of nucleogenic 21Ne and 38Ar and radiogenic 4He and 40Ar. 4He/40Ar and 21Ne/40Ar ratios, corrected for mass fractionation during incomplete brine degassing, are identical to their production ratios in rocks. The source of salinity (halite dissolution), plus the occurrence of large amounts of 40Ar in brines constrain the residence time of Bécancour brines as being older than the Cretaceous. Evaporites in the St-Lawrence Lowlands likely existed only during Devonian-Silurian time. Brines might result from infiltration of Devonian water leaching halite, penetrating into or below the deeper Cambrian-Ordovician aquifers. During the Devonian, the basin reached temperatures higher than 250 °C, allowing for thermal maturation of local gas-prone source rocks (Utica shales) and possibly facilitating the release of radiogenic 40Ar into the brines. The last thermal event that could have facilitated the liberation of 40Ar into fluids and contributed to mantle 3He is the Cretaceous Monteregian Hills magmatic episode. For residence times younger than the Cretaceous, it is difficult to find an appropriate source of salinity and of nucleogenic/radiogenic gases to the Bécancour brines.  相似文献   
106.
Matrix-diffusion parameters deduced from an infiltration tracer test at Idaho National Laboratory (INL), USA, are combined with other site information in an analysis involving two dimensionless lumped parameters to assess the effects of matrix diffusion on contaminant transport at the INL over longer distance and time scales than were evaluated in the test. Matrix diffusion was interrogated in the test by comparing, in three different observation wells, the breakthrough curves of two simultaneously injected nonsorbing solutes that have different diffusion coefficients. The matrix-diffusion parameters deduced from the different breakthrough curves were in good agreement, suggesting that the parameters may be broadly applicable at the INL. With this in mind, the uncertainties in the individual parameters that make up the two lumped parameters were estimated, and the resulting ranges of parameter values were used to assess matrix diffusion over larger scales. Assessments of the effects of flow transients, spatial heterogeneity in transport parameters, and sorption on solute transport in the shallow subsurface flow system were also conducted. The methods presented here should be generally applicable to other settings for making bounding assessments of the effects of matrix diffusion while honoring the information obtained from tracer tests and other supporting data.  相似文献   
107.
Identifying and mapping olivine on asteroid 4 Vesta are important components to understanding differentiation on that body, which is one of the objectives of the Dawn mission. Harzburgitic diogenites are the main olivine‐bearing lithology in the howardite‐eucrite‐diogenite (HED) meteorites, a group of samples thought to originate from Vesta. Here, we examine all the Antarctic harzburgites and estimate that, on scales resolvable by Dawn, olivine abundances in putative harzburgite exposures on the surface of Vesta are likely at best in the 10–30% range, but probably lower due to impact mixing. We examine the visible/near‐infrared spectra of two harzburgitic diogenites representative of the 10–30% olivine range and demonstrate that they are spectrally indistinguishable from orthopyroxenitic diogenites, the dominant diogenitic lithology in the HED group. This suggests that the visible/near‐infrared spectrometer onboard Dawn (VIR) will be unable to resolve harzburgites from orthopyroxenites on the surface of Vesta, which may explain the current lack of identification of harzburgitic diogenite on Vesta.  相似文献   
108.
This paper investigates the stable isotopic composition from late Pleistocene–Holocene (~ 13 to ~ 10.5 cal ka BP) shells of the land snail Helix figulina, from Franchthi Cave (Greece). It explores the palaeoclimatic and palaeoenvironmental implications of the isotope palaeoecology of archaeological shells at the time of human occupation of the cave. Modern shells from around the cave were also analysed and their isotopic signatures compared with those of the archaeological shells. The carbon isotope composition of modern shells depicts the consumption of C3 vegetation. Shell oxygen isotopic values are consistent with other Mediterranean snail shells from coastal areas. Combining empirical linear regression and an evaporative model, the δ18Os suggest that modern snails in the study area are active during periods of higher relative humidity and lower rainfall δ18O, probably at night. Late glacial and early Holocene δ18Os show lower values compared to modern ones. Early Holocene δ18Os values likely track enhanced moisture and isotopic changes in the precipitation source. By contrast, lower late glacial δ18O could reflect lower temperatures and δ18Op, compared to the present day. Shell carbon isotope values indicate the presence of C3 vegetation as main source of carbon to late glacial and early Holocene snails.  相似文献   
109.
The natural river water certified reference material SLRS‐5 (NRC‐CNRC) was routinely analysed in this study for major and trace elements by ten French laboratories. Most of the measurements were made using ICP‐MS. Because no certified values are assigned by NRC‐CNRC for silicon and 35 trace element concentrations (rare earth elements, Ag, B, Bi, Cs, Ga, Ge, Li, Nb, P, Rb, Rh, Re, S, Sc, Sn, Th, Ti, Tl, W, Y and Zr), or for isotopic ratios, we provide a compilation of the concentrations and related uncertainties obtained by the participating laboratories. Strontium isotopic ratios are also given.  相似文献   
110.
Investigation of chlorins in the oxic surface sediment of a small eutrophic alpine lake (Motte lake) revealed the presence of a new series of steryl chlorin esters containing the pheophorbide a nucleus, together with their pyropheophorbide a steryl ester counterparts previously observed in the anoxic surface sediment of the same lake. Identification of the pheophorbide a steryl esters was based on comparison of spectroscopic, chromatographic and mass spectrometric characteristics of the compounds with those of a synthetic standard and of pyropheophorbide a steryl esters. Combined liquid chromatography-mass spectrometry analysis confirmed the absence of pheophorbide a steryl esters in the anoxic sediment but allowed their detection in traces in the water column, indicating that pheophorbide a steryl esters are, like their pyropheophorbide a analogs, formed in the water column. The distribution of sterols released by hydrolysis of the pheophorbide a steryl esters shows close similarities to that of the free sterols in the water column and of the sterols of the pyropheophorbide a steryl esters. It appears that, like their pyropheophorbide a counterparts, pheophorbide a steryl esters incorporate mainly sterols of phytoplanktonic origin. Their formation probably involves the same mechanism as for pyropheophorbide a steryl ester formation, i.e. metabolism by zooplankton grazing on phytoplankton. The presence of pheophorbide a steryl esters in the oxic sediment and their absence from the anoxic sediment is probably due to a lower stability of compounds containing a carbomethoxy substituent in the anoxic environment.  相似文献   
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