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1.
Existing methods for black carbon (BC) quantification measure different parts of the BC continuum, which complicates the calculation of a global BC budget. Benzenepolycarboxylic acids (BPCA) are used as molecular markers to quantify and characterize BC in soils and sediments using gas chromatography for BPCA separation (GC-BPCA). Recently, this method was refined for BC analysis in seawater using high performance liquid chromatography (LC-BPCA), which omits the cleaning steps and derivatization necessary in GC analysis. As yet it is not clear whether the two analytical methods yield similar results. Here we apply both methods to a suite of laboratory produced charcoals derived from wood and grass. We found systematically lower total BPCA-C contents and larger analytical variability for all tested charcoals when using GC-BPCA compared to LC-BPCA, the latter giving 1.5 ± 0.3 times higher yields for the charcoal samples formed at 275-700 °C. At lower and higher pyrolysis temperatures the differences between the two analytical methods were larger. The main reason for the differences between the two methods is the loss of BPCA during sample preparation for GC analysis. We propose a correction factor of 1.5 to account for at least part of these losses. No qualitative biases, i.e. towards more or less functionalized BPCAs, were observed between the two methods. The relative contribution of mellitic acid C to total BPCA-C, a measure for the degree of condensation of BC, was the same in the two analytical techniques. Qualitative differences between wood and grass charcoals as detected by both methods were small.  相似文献   
2.
The interaction of Cs(I), Eu(III), Th(IV) and U(VI) with montmorillonite colloids was investigated in natural Grimsel Test Site groundwater over a 3 years period. The asymmetric flow field-flow fractionation combined with various detectors was applied to study size variations of colloids and to monitor colloid association of trace metals. The colloids suspended directly in the low ionic strength (I), slightly alkaline granitic groundwater (I = 10−3 mol/L, pH 9.6) showed a gradual agglomeration with a size distribution shift from initially 10-200 nm to 50-400 nm within over 3 years. The Ca2+ concentration of 2.1 × 10−4 mol/L in the ground water is believed to be responsible for the slow agglomeration due to Ca2+ ion exchange against Li+ and Na+ at the permanently charged basal clay planes. Furthermore, the Ca2+ concentration lies close to the critical coagulation concentration (CCC) of 10−3 mol L−1 for clay colloids. Slow destabilization may delimit clay colloid migration in this specific groundwater over long time scales. Eu(III) and Th(IV) are found predominantly bound to clay colloids, while U(VI) prevails as the UO2(OH)3 complex and Cs(I) remains mainly as aquo ion under our experimental conditions. Speciation calculations qualitatively represent the experimental data. A focus was set on the reversibility of metal ion-colloid binding. Addition of humic acid as a competing ligand induces rapid metal ion dissociation from clay colloids in the case of Eu(III) even after previous aging for about 3 years. Interestingly only partial dissociation occurs in the case of Th(IV). Experiments and calculations prove that the humate complexes dominate the speciation of all metal ions under given conditions. The partial irreversibility of clay bound Th(IV) is presently not understood but might play an important role for the colloid-mediated transport of polyvalent actinides over wide distances in natural groundwater.  相似文献   
3.
Groundwater storage, drainage, and interbasin water exchange are common hydrological processes but often difficult to quantify due to a lack of local observations. We present a study of three volcanic mountainous watersheds located in south‐central Chile (~36.9 ° S) in the Chillán volcanic complex (Chillán, Renegado, and Diguillín river basins). These are neighboring basins that are similar with respect to the metrics normally available for characterization everywhere (e.g., precipitation, temperature, and land cover). In a hydrological sense, similar (proportional) behavior would be expected if these catchments would be characterized with this general information. However, these watersheds show dissimilar behavior when analyzed in detail. The surface water balance does not fit for any of these watersheds individually; however, the water balance of the whole system can be explained by likely interbasin water exchanges. The Renegado river basin has an average annual runoff per unit of area on the order of 60–65% less than those of the Diguillín and Chillán rivers, which is contradictory to the hydrological similarity among the basins. To understand the main processes that control streamflow generation, two analyses were performed: (a) basin metrics (land cover, geologic, topographic, and climatological maps) and hydro‐meteorological data analyses and (b) a water balance model approach. The analyses contribute to a plausible explanation for the hydrogeological processes in the system. The soils, topography, and geology of the Chillán–Renegado–Diguillín system favor the infiltration and groundwater movements from the Renegado river basin, mainly to the neighboring Diguillín basin. The interbasin water exchanges affect hydrological similarity and explain the differences observed in the hydrological processes of these three apparently similar volcanic basins. The results highlight the complexity of hydrological processes in volcanic mountainous systems and suggest that a simple watershed classification approach based on widely available data is insufficient. Simple local analyses such as specific flow analysis with a review of the geology and morphology can contribute to a better understanding of the hydrology of volcanic mountainous areas.  相似文献   
4.
Blueschist facies rocks in the Yuli Belt of Taiwan's Central Range record ongoing subduction of the Eurasian plate. We present a prograde Lu–Hf garnet–whole‐rock age of 5.1 ± 1.7 Ma from a retrogressed blueschist in the Yuli Belt. This age is considerably younger than the previously assumed age of 14–8 Ma for high‐pressure metamorphism in the Yuli Belt and represents the youngest Lu–Hf garnet age ever recorded for blueschist facies metamorphism. The age sheds new light on the palaeogeographic origin and exhumation scenario of the Yuli Belt. We propose that the Yuli Belt originated from the ocean–continent boundary of the Chinese passive margin. It was subducted eastward during collision with the Luzon island arc and rapidly exhumed when the forearc lithosphere was removed from above the continental slab by discrete subduction (extraction). This process reduces the pressure above the continental slab and may prompt the ascent of subducted crust into the opening gap. Thus, it can control the exhumation of high‐pressure rocks.  相似文献   
5.
Dissolved organic matter (DOM) was investigated along a gradient across the Subtropical Convergence (STC) off the South Island, New Zealand. Ultrahigh resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS), excitation emission matrix fluorescence (EEM) spectroscopy, and molecular lignin analysis techniques were used to study this DOM. The analysis revealed a group of compounds found only in the coastal DOM samples, which were also characterized by an elevated terrestrial DOM fluorescence pattern and elevated lignin content if compared to the offshore samples. This group exhibited a high degree of carbon unsaturation, as evident from high double bond equivalence minus oxygen values (DBE-O > 9) and maximum fluorescence intensity. Sulfur-containing molecular formulae for summer DOM samples were much more abundant across the entire transect of the STC compared to winter and exhibited distinctly different hydrogen:carbon and oxygen:carbon elemental ratios, suggesting a possible correlation between biological activity and sulfur compounds. The molecular formulae common to all STC samples were compared with those calculated for DOM extracted from freshwater collected from a stream discharging into Doubtful Sound (West Coast, New Zealand). ESI-FT-ICR-MS measurements undertaken in negative electrospray ionization (ESI?) mode indicated that 30% of the molecular formulae were present in both types of DOM, while in positive ESI mode (ESI+) over 90% of the formulae were present in all samples. Hence, a significant portion of the molecular formulae assigned to the solid-phase extractable DOM pool (SPE-DOM) appear to be identical in oceanic and freshwater samples.  相似文献   
6.
Potential pathways in the subsurface may allow upwardly migrating gaseous CO2 from deep geological storage formations to be released into near surface aquifers. Consequently, the availability of adequate methods for monitoring potential CO2 releases in both deep geological formations and the shallow subsurface is a prerequisite for the deployment of Carbon Capture and Storage technology. Geoelectrical surveys are carried out for monitoring a small-scale and temporally limited CO2 injection experiment in a pristine shallow aquifer system. Additionally, the feasibility of multiphase modeling was tested in order to describe both complex non-linear multiphase flow processes and the electrical behavior of partially saturated heterogeneous porous media. The suitability of geoelectrical methods for monitoring injected CO2 and geochemically altered groundwater was proven. At the test site, geoelectrical measurements reveal significant variations in electrical conductivity in the order of 15?C30?%. However, site-specific conditions (e.g., geological settings, groundwater composition) significantly influence variations in subsurface electrical conductivity and consequently, the feasibility of geoelectrical monitoring. The monitoring results provided initial information concerning gaseous CO2 migration and accumulation processes. Geoelectrical monitoring, in combination with multiphase modeling, was identified as a useful tool for understanding gas phase migration and mass transfer processes that occur due to CO2 intrusions in shallow aquifer systems.  相似文献   
7.
The precise estimation of precipitation quantities in tropical mountain regions is in great demand by ecological and hydrological studies, due to the heterogeneity of the rainfall distribution and the lack of meteorological station data. This study uses radar images and ground station data to provide the required high-resolution precipitation maps. Also wind data are taken into account, due to its influence on the precipitation formation and to demonstrate the relation between synoptic wind, topography and the precipitation distribution inside small mountain valleys. The study analyses the rainfall distribution and amounts of 4 days inside the San Francisco Valley, a small catchment in the tropical Andes of southern Ecuador, representing different seasons and the typical atmospheric flows, which are correlated to the annual precipitation map. The results show that the rainfall distribution and amounts are generally defined by the wind direction and velocity, besides the topographic location in relation to the main barriers and pathways. The dominant wind direction causes a division of the catchment in a wetter eastern and a dryer western part. Moreover, the annual seasons are reversed; the main rainy season for the eastern part occurs between June and August, while the western part reaches the precipitation maximum between January and March. This may have influence on the species composition at the different slopes and the annual hydrological cycle inside the catchment.  相似文献   
8.
ABSTRACT Palaeoceanographic reconstructions from the North Atlantic indicate massive ice breakouts from East Greenland near the onset of cold Dansgaard–Oeschger (D–O) stadials. In contrast to these coolings in the North Atlantic area, a new sea-surface temperature record reveals concomitant warm spells in the northern North Pacific. A sensitivity experiment with an atmospheric general circulation model is used to test the potential impact of sea-surface warmings by 3.5 °C in the North Pacific, on top of otherwise cold stadial climate conditions, on the precipitation regime over the Northern Hemisphere ice sheets. The model predicts a maximum response over East Greenland and the Greenland Sea, where a 40% increase in net annual snow accumulation occurs. This remote effect of North Pacific warm spells on the East Greenland snow-accumulation rate may play an important role in generating D–O cycles by rebuilding the ice lost during ice breakouts. In addition, the increased precipitation over the Greenland Sea may help to sustain the D–O stadial climate state.  相似文献   
9.
The crystallographic structures of the synthetic cheralite, CaTh(PO4)2, and its homolog CaNp(PO4)2 have been investigated by X-ray diffraction at room temperature. Rietveld analyses showed that both compounds crystallize in the monoclinic system and are isostructural to monazite LnPO4 (Ln = La to Gd). The space group is P21/n (I.T. = 14) with Z = 2. The refined lattice parameters of CaTh(PO4)2 are a = 6.7085(8) Å, b = 6.9160(6) Å, c = 6.4152(6) Å, and β = 103.71(1)° with best fit parameters R wp = 4.87%, R p = 3.69% and R B = 3.99%. For CaNp(PO4)2, we obtained a = 6.6509(5) Å, b = 6.8390(3) Å, c = 6.3537(8) Å, and β = 104.12(6)° and R wp = 6.74%, R p = 5.23%, and R B = 6.05%. The results indicate significant distortions of bond length and angles of the PO4 tetrahedra in CaTh(PO4)2 and to a lesser extent in CaNp(PO4)2. The structural distortions were confirmed by Raman spectroscopy of CaTh(PO4)2. A comparison with the isostructural compounds LnPO4 (Ln = Ce and Sm) confirmed that the substitution of the large rare earth trivalent cations with Ca2+ and Th4+ introduces a distortion of the PO4 tetrahedra.  相似文献   
10.
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