Assessment of alternative adsorption models and global sensitivity analysis to characterize hexavalent chromium loss from soil to surface runoff          下载免费PDF全文

Chuan‐An Xia  Juxiu Tong  Bill X. Hu  Xiujie Wu  Alberto Guadagnini 《水文研究》2018,32(20):3140-3157

We investigate our ability to assess transfer of hexavalent chromium, Cr(VI), from the soil to surface runoff by considering the effect of coupling diverse adsorption models with a two‐layer solute transfer model. Our analyses are grounded on a set of two experiments associated with soils characterized by diverse particle size distributions. Our study is motivated by the observation that Cr(VI) is receiving much attention for the assessment of environmental risks due to its high solubility, mobility, and toxicological significance. Adsorption of Cr(VI) is considered to be at equilibrium in the mixing layer under our experimental conditions. Four adsorption models, that is, the Langmuir, Freundlich, Temkin, and linear models, constitute our set of alternative (competing) mathematical formulations. Experimental results reveal that the soil samples characterized by the finest grain sizes are associated with the highest release of Cr(VI) to runoff. We compare the relative abilities of the four models to interpret experimental results through maximum likelihood model calibration and four model identification criteria (i.e., the Akaike information criteria [AIC and AIC_C] and the Bayesian and Kashyap information criteria). Our study results enable us to rank the tested models on the basis of a set of posterior weights assigned to each of them. A classical variance‐based global sensitivity analysis is then performed to assess the relative importance of the uncertain parameters associated with each of the models considered, within subregions of the parameter space. In this context, the modelling strategy resulting from coupling the Langmuir isotherm with a two‐layer solute transfer model is then evaluated as the most skilful for the overall interpretation of both sets of experiments. Our results document that (a) the depth of the mixing layer is the most influential factor for all models tested, with the exception of the Freundlich isotherm, and (b) the total sensitivity of the adsorption parameters varies in time, with a trend to increase as time progresses for all of the models. These results suggest that adsorption has a significant effect on the uncertainty associated with the release of Cr(VI) from the soil to the surface runoff component.  相似文献   

Luminescence dating of sand–loess sequences and response of Mu Us and Otindag sand fields (north China) to climatic changes     

Yali Zhou  Huayu Lu  Jiafu Zhang  Joseph A. Mason  Liping Zhou 《第四纪科学杂志》2009,24(4):336-344

The sand–loess transition zone in north China is sensitive to climate change, and is an ideal place to investigate past environmental changes. However, past climate change at millennial–centennial timescales in this region has not been well reconstructed because of limited numerical dating. Alternations of sandy loam soils with aeolian sand layers in the Mu Us and Otindag sand fields, which lie along the sand–loess transition zone, indicate multiple intervals of dune activity and stability. This change is probably a response to variations of the East Asian monsoon climate during the late Quaternary. The single aliquot regeneration (SAR) optically stimulated luminescence (OSL) dating protocol, which has been successfully applied to aeolian deposits worldwide, is applied to these two sand fields in this study. The OSL ages provide reliable constraints for reconstruction of past climate changes at suborbital timescale. Sections in both sand fields contain aeolian sand beds recording millennial‐scale episodes of dry climate and widespread dune activation, including episodes at about the same time as Heinrich Event 5 and the Younger Dryas in the North Atlantic region. These results demonstrate the potential of aeolian sediments in semi‐arid north China to record millennial‐scale climatic events, and also suggest that dry–wet climate variation at the desert margin in China may be linked to climatic change elsewhere in the Northern Hemisphere, through atmospheric circulation. This article was published online on 27 November 2008. An error was subsequently identified. This notice is included in the online and print versions to indicate that both have been corrected (16 December 2008). Copyright © 2008 John Wiley & Sons, Ltd.  相似文献   

Papers to Appear in Forthcoming Issues     

《Applied Geochemistry》2006,21(1):I

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Decoupling of stalagmite-derived Asian summer monsoon records from North Atlantic temperature change during marine oxygen isotope stage 5d   总被引：2，自引：0，他引：2  

Houyun Zhou  Jianxin Zhao  Chuan-Chou Shen  Yuexing Feng  Huazheng Guan  Chen-Feng You 《Quaternary Research》2008,70(2):315-321

The Asian monsoon is an important component of the global climate system. Seasonal variations in wind, rainfall, and temperature associated with the Asian monsoon systems affect a vast expanse of tropical and subtropical Asia. Speleothem-derived summer monsoon variation in East Asia was previously found to be closely associated with millennial-scale change in temperature in the North Atlantic region between 75 and 10 ka. New evidence recovered from East Asia, however, suggests that the teleconnection between summer monsoon in East Asia and temperature change in the North Atlantic region may have significantly reduced during 120 to ~ 110 ka, a period directly after the full last interglaciation and corresponding roughly to marine oxygen isotope stage 5d. This reduction may be due to the low ice volume in the North Hemisphere at that time, which makes the millennial-scale change in temperature in the North Atlantic region less effective in influencing the Asian summer monsoon. This is important for investigating the mechanisms controlling the Asian summer monsoon and the paleoclimatic teleconnection between East Asia and the North Atlantic region, and for predicting monsoon-associated precipitation in East Asia under a global-warming trend.  相似文献   

Dehydration and melting during continental collision: Constraints from element and isotope geochemistry of low-T/UHP granitic gneiss in the Dabie orogen     

Qiong-Xia Xia  Yong-Fei Zheng  Li-Gang Zhou 《Chemical Geology》2008,247(1-2):36-65

A combined study of petrography, whole-rock major and trace elements as well as Rb?Sr and Sm?Nd isotopes, and mineral oxygen isotopes was carried out for two groups of low-T/UHP granitic gneiss in the Dabie orogen. The results demonstrate that metamorphic dehydration and partial melting occurred during exhumation of deeply subducted continent. Zircon δ¹⁸O values of ? 2.8 to + 4.7‰ for the gneiss are all lower than normal mantle values of 5.3 ± 0.3‰, consistent with ¹⁸O depletion of protolith due to high-T meteoric-hydrothermal alteration at mid-Neoproterozoic. Most samples have extremely low ⁸⁷Sr/⁸⁶Sr ratios at t₁ = 780 Ma, but very high ⁸⁷Sr/⁸⁶Sr ratios at t₂ = 230 Ma. This suggests intensive fluid disturbance due to the hydrothermal alteration of protoliths during Neoproterozoic magma emplacement and the metamorphic dehydration during Triassic continental collision. Rb–Sr isotopes, Th/Ta vs. La/Ta and Th/Hf vs. La/Nb relationships suggest that Group I gneiss experienced lower degrees of hydrothermal alteration, but higher degrees of dehydration, than Group II gneiss. The two groups of gneiss have similar patterns of REE and trace element partition. Group I gneiss displays good correlations between Nb and LREEs but no correlations between Nb and LILEs (Rb, Ba, Pb, Th and U), indicating differential mobilities of LILEs during the dehydration. Thus the correlation between Nb and LREEs is inherited from protolith rather than caused by metamorphic modification. Relative to Group I gneiss, Group II gneiss has stronger negative Eu anomaly, lower contents of Sr and Ba but higher contents of Rb, Th and U. In particular, Nb correlates with LILEs (e.g., Rb, Sr, Ba, Th and U), but not with LREEs (La and Ce). This may indicate decoupling between the dehydration and LILEs transport during continental collision. Furthermore, dehydration melting may have occurred due to breakdown of muscovite during “hot” exhumation. Group II gneiss has extremely low contents of FeO + MgO + TiO₂ (1.04 to 2.08 wt.%), high SiO₂ contents of 75.33 to 78.23 wt%, and high total alkali (Na₂O + K₂O) contents (7.52 to 8.92 wt.%), comparable with compositions predicted from partial melting of felsic rocks by experimental studies. Almost no UHP metamorphic minerals survived; felsic veins of fine-grain minerals occurs locally between coarse-grain minerals, resulting in a kind of metatexite migmatites due to dehydration melting without considerable escape of felsic melts from the host gneiss. In contrast, Group I gneiss only shows metamorphic dehydration. Therefore, the two groups of gneiss show contrasting behaviors of fluid–rock interaction during the continental collision.  相似文献   

Water release patterns of heated speleothem calcite and hydrogen isotope composition of fluid inclusions     

Sophie Verheyden  Dominique Genty  Olivier Cattani  Martin R. van Breukelen 《Chemical Geology》2008,247(1-2):266-281

Speleothem fluid inclusions are a potential paleo-precipitation proxy to reconstruct past rainwater isotopic composition (δ¹⁸O, δD). To get a better insight in the extraction of inclusion water from heated speleothem calcite, we monitored the water released from crushed and uncrushed speleothem calcite, heated to 900 °C at a rate of 300 °C/h, with a quadrupole mass spectrometer. Crushed calcite released water in three not well individualised peaks between 25 and 360 °C, 360 and 650 °C and between 650 and 800 °C while uncrushed calcite released water in two distinct temperature intervals: between 25 and 550 °C and between 550 and 900 °C.Water from two speleothems from the Han-sur-Lesse cave was recovered using three different techniques: i) the crushing and heating to 360 °C technique, ii) the decrepitation by heating to 550 °C and iii) the decomposition by heating to 900 °C technique. Measurements of the δD of water recovered by the decomposition of Han-sur-Lesse calcite heated to 900 °C did not show a 20 to 30‰ offset as found by previous authors. However a difference of 7‰ was observed between water released before and after decomposition of the calcite. Water recovery from the Han-sur-Lesse samples suggests that a simple heating technique (up to 550 °C) without crushing could both (a) recover water with δD representative of that of the drip water and (b) double the water yield as compared to the crushing and heating method.Our study warns for possible contamination of the recovered inclusion water with hydration water of lime, responsible for the recovery of water with very negative δD values.  相似文献   

Complex replacement patterns in garnets from Bergen Arcs eclogites: A combined EBSD and analytical TEM study     

Kilian Pollok  Geoffrey E. Lloyd  Hkon Austrheim  Andrew Putnis 《Chemie der Erde / Geochemistry》2008,68(2):177-191

Eclogite-facies rocks within the Bergen Arcs, western Norway, have formed from granulites along shear zones and fluid pathways. Garnets that were inherited from granulite facies protoliths show different types of replacement patterns due to an incomplete eclogitisation process including concentric rim zoning, zoning along vein fillings and inclusion trails, and zoning bands without inclusions. The interfacial part between the granulitic core and the eclogitic rim of garnet as well as the microstructure of other relevant minerals (omphacite, plagioclase) has been analysed using analytical transmission electron microscopy (ATEM). In garnet, the interface is characterised by gradual changes in composition from X_alm=0.31, X_pyr=0.50 to X_alm=0.54, and X_pyr=0.25 within ≈20 μm and exhibits no distinct change in microstructure. Granulitic plagioclase shows exsolution lamellae of the Bøggild intergrowth. In omphacite, anti-phase domains (APDs) which potentially record the temperature of cation ordering after mineral growth have been observed and their size suggest eclogitisation at 600–700 °C. The electron backscatter diffraction (EBSD) analysis revealed that the lattice orientation of the granulitic feldspar is basically unrelated to tectonic axes whereas newly formed eclogitic minerals omphacite and kyanite show a crystallographic relation to the foliation. In garnet, no change in the basic crystallographic orientation between the eclogitic and granulitic garnet composition was confirmed. However, misorientation analysis suggests a cellular microstructure not more than 1° misorientation in the core of the garnets, which is missing in the eclogitic rim indicating textural equilibration of the latter. The heterogeneous replacement patterns are characteristic for dissolution and re-precipitation reactions in an open system limited to fluid availability. The appearance of the compositional profile in garnet is interpreted as a diffusional re-equilibration step after the time-limited, fluid-mediated eclogitisation event that apparently obscured the initially sharp interface within the further retrograde metamorphic history.  相似文献   

Proterozoic (pre-Ediacaran) glaciation and the high obliquity,low-latitude ice,strong seasonality (HOLIST) hypothesis: Principles and tests     

《Earth》2008,88(3-4):61-93

Sedimentological observations and palaeomagnetic data for Cryogenian glacial deposits present the climatic paradox of grounded glaciers and in situ cold climate near sea-level, glaciomarine deposition, and accompanying large (up to 40 °C) seasonal changes of temperature, all in low to near-equatorial (< 10°) palaeolatitudes (equated with geographic latitudes). Neither the “snowball Earth” nor the “slushball Earth” hypothesis can account for such strong seasonality near the palaeoequator, which together with findings from sedimentology, chemostratigraphy, biogeochemistry, micropalaeontology, geochronology and climate modelling argue against those scenarios. An alternative explanation of glaciation and strong seasonality in low palaeolatitudes is offered by a high (> 54°) obliquity of the ecliptic, which would render the equator cooler than the poles, on average, and amplify global seasonality. A high obliquity per se would not have been a primary trigger for glaciation, but would have strongly influenced the latitudinal distribution of glaciers. The principle of low-latitude glaciation on a terrestrial planet with high obliquity is validated by theoretical studies and observations of Mars. A high obliquity for the early Earth is a likely outcome of a single giant impact at 4.5 Ga, the widely favoured mechanism for lunar origin. This implies that a high obliquity could have prevailed during most of the Precambrian, controlling the low palaeolatitude of glaciations in the early and late Palaeoproterozoic and Cryogenian. It is postulated that the obliquity changed to < 54° between the termination of the last Cryogenian low-palaeolatitude glaciation at ≤ 635 Ma and the initiation of Late Ordovician–Early Silurian circum-polar glaciation at 445 Ma.The High Obliquity, Low-latitude Ice, STrong seasonality (HOLIST) hypothesis for pre-Ediacaran glaciation emerges favourably from numerous glacial and non-glacial tests. The hypothesis is in accord with such established or implied features of Cryogenian glaciogenic successions as extensive and long-lived open seas, an active hydrological cycle, aridity and palaeowesterly (reversed zonal) winds in low palaeolatitudes, and the apparent diachronism or non-correlation of some low-palaeolatitude glaciations. A pre-Ediacaran high obliquity also offers a viable solution of the faint young Sun paradox of a warm Archaean Earth. Furthermore, reduction of obliquity during the Ediacaran–early Palaeozoic would have yielded a more habitable globe with much reduced seasonal stresses and may have been an important factor influencing the unique evolutionary events of the Ediacaran and Cambrian. The palaeolatitudinal distribution of evaporites cannot discriminate unambiguously between high- and low-obliquity states for the pre-Ediacaran Earth. Intervals of true polar wander such as postulated by others for the Ediacaran and Early Cambrian imply major mass-redistributions within the Earth at those times, which may provide a potential mechanism for reducing the obliquity during the Ediacaran–early Palaeozoic.  相似文献   

A strong temperature effect on U/Ca in planktonic foraminiferal carbonates     

Jimin Yu  Henry Elderfield  Linda Booth 《Geochimica et cosmochimica acta》2008,72(20):4988-5000

Three planktonic foraminiferal species Globigerina bulloides, Neogloboquadrina pachyderma (d), and Globorotalia inflata collected from core-tops spanning 35° to 65°N in the North Atlantic were used for U/Ca and Mg/Ca and foraminiferal shell weight analyses. Except for U/Ca in G. bulloides calcified under warm conditions (>∼13 °C), U/Ca ratios in all three studied species increase with decreasing latitude and show strong positive correlations with Mg/Ca ratios. A dissolution effect on planktonic U/Ca is suggested by decreased shell weight and U/Ca and Mg/Ca ratios for shells from very deep water depth (>4.4 km) along the latitudinal transect. G. bulloides from down core samples in the North Atlantic show low U/Ca ratios during the last glacial and high ratios during the Holocene, similar to the Mg/Ca evolution trend. In general, our data indicate that the U incorporation into planktonic foraminiferal carbonates is strongly influenced by calcification temperature, although U/Ca in G. bulloides may be affected by seawater carbonate ion concentration under warm conditions and/or other factors.  相似文献   

Radon transfer from groundwater used in showers to indoor air     

David S. Vinson  Ted R. Campbell  Avner Vengosh 《Applied Geochemistry》2008

Estimation of Rn transfer from water to indoor air based on multi-day measurements may underestimate alpha exposure that occurs at short time scales in confined spaces, such as from showering, in houses with high Rn activities in the water supply. In order to examine one such incremental increase in exposure, variations in Rn in water and indoor air in 18 houses with private wells in western North Carolina (USA) were investigated. Radon in well water ranged from 158 to 811 Bq L⁻¹ (median 239 Bq L⁻¹). After 20-min showers in bathrooms with closed doors, peak Rn in air increases (above background) ranged from 71 to 4420 Bq m⁻³ (median 1170 Bq m⁻³). Calculated transfer coefficients at the scale of a 40-min closed bathroom (20-min shower plus 20 min post-shower) are described by a lognormal distribution whose geometric mean exceeds the widely-used ∼10⁻⁴ whole-house transfer coefficient by about one order of magnitude. As short-lived decay products grow from shower-derived Rn, short-term alpha energy exposure occurs in bathrooms in addition to the exposure caused by Rn mixed throughout the volume of the house. Due to the increasing ratio of Rn decay products to Rn, alpha energy exposure is greatest several minutes after the shower is turned off. For a 7.2-min shower with 10 min of additional exposure before opening the door, a geometric mean 5.6% increase in exposure over the ∼10⁻⁴ whole-house transfer coefficient derived from longer measurement periods was estimated. In addition to Rn activity in water, short-term shower exposure to Rn progeny depends on exposure time, ventilation, attachment and deposition, among other variable factors that characterize individual houses and residents.  相似文献