Uranyl adsorption onto montmorillonite: Evaluation of binding sites and carbonate complexation   总被引：2，自引：0，他引：2  

Jeffrey G. Catalano  Gordon E. Brown Jr. 《Geochimica et cosmochimica acta》2005,69(12):2995-3005

The fate and transport of uranium in contaminated soils and sediments may be affected by adsorption onto the surface of minerals such as montmorillonite. Extended X-ray absorption fine structure (EXAFS) spectroscopy has been used to investigate the adsorption of uranyl (UO₂²⁺) onto Wyoming montmorillonite. At low pH (∼4) and low ionic strength (10⁻³ M), uranyl has an EXAFS spectrum indistinguishable from the aqueous uranyl cation, indicating binding via cation exchange. At near-neutral pH (∼7) and high ionic strength (1 M), the equatorial oxygen shell of uranyl is split, indicating inner-sphere binding to edge sites. Linear-combination fitting of the spectra of samples reacted under conditions where both types of binding are possible reveals that cation exchange at low ionic strengths on SWy-2 may be more important than predicted by past surface complexation models of U(VI) adsorption on related montmorillonites. Analysis of the binding site on the edges of montmorillonite suggests that U(VI) sorbs preferentially to [Fe(O,OH)₆] octahedral sites over [Al(O,OH)₆] sites. When bound to edge sites, U(VI) occurs as uranyl-carbonato ternary surface complexes in systems equilibrated with atmospheric CO₂. Polymeric surface complexes were not observed under any of the conditions studied. Current surface complexation models of uranyl sorption on clay minerals may need to be reevaluated to account for the possible increased importance of cation exchange reactions at low ionic strengths, the presence of reactive octahedral iron surface sites, and the formation of uranyl-carbonato ternary surface complexes. Considering the adsorption mechanisms observed in this study, future studies of U(VI) transport in the environment should consider how uranium retardation will be affected by changes in key solution parameters, such as pH, ionic strength, exchangeable cation composition, and the presence or absence of CO₂.  相似文献   

Fluid generation and evolution during exhumation of deeply subducted UHP continental crust: Petrogenesis of composite granite–quartz veins in the Sulu belt,China          下载免费PDF全文

S.‐J. Wang  L. Wang  M. Brown  P. M. Piccoli  T. E. Johnson  P. Feng  H. Deng  K. Kitajima  Y. Huang 《Journal of Metamorphic Geology》2017,35(6):601-629

Composite granite–quartz veins occur in retrogressed ultrahigh pressure (UHP) eclogite enclosed in gneiss at General's Hill in the central Sulu belt, eastern China. The granite in the veins has a high‐pressure (HP) mineral assemblage of dominantly quartz+phengite+allanite/epidote+garnet that yields pressures of 2.5–2.1 GPa (Si‐in‐phengite barometry) and temperatures of 850–780°C (Ti‐in‐zircon thermometry) at 2.5 GPa (~20°C lower at 2.1 GPa). Zircon overgrowths on inherited cores and new grains of zircon from both components of the composite veins crystallized at c. 221 Ma. This age overlaps the timing of HP retrograde recrystallization dated at 225–215 Ma from multiple localities in the Sulu belt, consistent with the HP conditions retrieved from the granite. The ε_Hf(t) values of new zircon from both components of the composite veins and the Sr–Nd isotope compositions of the granite consistently lie between values for gneiss and eclogite, whereas δ¹⁸O values of new zircon are similar in the veins and the crustal rocks. These data are consistent with zircon growth from a blended fluid generated internally within the gneiss and the eclogite, without any ingress of fluid from an external source. However, at the peak metamorphic pressure, which could have reached 7 GPa, the rocks were likely fluid absent. During initial exhumation under UHP conditions, exsolution of H₂O from nominally anhydrous minerals generated a grain boundary supercritical fluid in both gneiss and eclogite. As exhumation progressed, the volume of fluid increased allowing it to migrate by diffusing porous flow from grain boundaries into channels and drain from the dominant gneiss through the subordinate eclogite. This produced a blended fluid intermediate in its isotope composition between the two end‐members, as recorded by the composite veins. During exhumation from UHP (coesite) eclogite to HP (quartz) eclogite facies conditions, the supercritical fluid evolved by dissolution of the silicate mineral matrix, becoming increasingly solute‐rich, more ‘granitic’ and more viscous until it became trapped. As crystallization began by diffusive loss of H₂O to the host eclogite concomitant with ongoing exhumation of the crust, the trapped supercritical fluid intersected the solvus for the granite–H₂O system, allowing phase separation and formation of the composite granite–quartz veins. Subsequently, during the transition from HP eclogite to amphibolite facies conditions, minor phengite breakdown melting is recorded in both the granite and the gneiss by K‐feldspar+plagioclase+biotite aggregates located around phengite and by K‐feldspar veinlets along grain boundaries. Phase equilibria modelling of the granite indicates that this late‐stage melting records P–T conditions towards the end of the exhumation, with the subsolidus assemblage yielding 0.7–1.1 GPa at <670°C. Thus, the composite granite–quartz veins represent a rare example of a natural system recording how the fluid phase evolved during exhumation of continental crust. The successive availability of different fluid phases attending retrograde metamorphism from UHP eclogite to amphibolite facies conditions will affect the transport of trace elements through the continental crust and the role of these fluids as metasomatic agents interacting with the mantle wedge in the subduction channel.  相似文献   

Metrics to assess how longitudinal channel network connectivity and in‐stream Atlantic salmon habitats are impacted by hydropower regulation          下载免费PDF全文

Willem B. Buddendorf  Iain A. Malcolm  Josie Geris  Mark E. Wilkinson  Chris Soulsby 《水文研究》2017,31(12):2132-2142

Habitat fragmentation in channel networks and riverine ecosystems is increasing globally due to the construction of barriers and river regulation. The resulting divergence from the natural state poses a threat to ecosystem integrity. Consequently, a trade‐off is required between the conservation of biodiversity in channel networks and socio‐economic factors including power generation, potable water supplies, fisheries, and tourism. Many of Scotland's rivers are regulated for hydropower generation but also support populations of Atlantic salmon (Salmo salar L.) that have high economic and conservation value. This paper investigates the use of connectivity metrics and weightings to assess the impact of river barriers (impoundments) associated with hydropower regulation on natural longitudinal channel connectivity for Atlantic salmon. We applied 2 different weighting approaches in the connectivity models that accounted for spatial variability in habitat quality for spawning and fry production and contrasted these models with a more traditional approach using wetted area. Assessments of habitat loss using the habitat quality weighted models contrasted with those using the less biologically relevant wetted area. This highlights the importance of including relevant ecological and hydrogeomorphic information in assessing regulation impacts on natural channel connectivity. Specifically, we highlight scenarios where losing a smaller area of productive habitat can have a larger impact on Atlantic salmon than losing a greater area of less suitable habitat. It is recommended that future channel connectivity assessments should attempt to include biologically relevant weightings, rather than relying on simpler metrics like wetted area which can produce misleading assessments of barrier impacts.  相似文献   

Appreciation     

Iain Suthers 《Deep Sea Research Part II: Topical Studies in Oceanography》2011,58(5):537

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A critical evaluation of multi‐proxy dendroclimatology in northern Finland     

Danny McCarroll  Mervi Tuovinen  Rochelle Campbell  Mary Gagen  Håkan Grudd  Risto Jalkanen  Neil J. Loader  Iain Robertson 《第四纪科学杂志》2011,26(1):7-14

Twentieth‐century summer (July–August) temperatures in northern Finland are reconstructed using ring widths, maximum density and stable carbon isotope ratios (δ¹³C) of Scots pine tree rings, and using combinations of these proxies. Verification is based on the coefficient of determination (r²), reduction of error (RE) and coefficient of efficiency (CE) statistics. Of the individual proxies, δ¹³C performs best, followed by maximum density. Combining δ¹³C and maximum density strengthens the climate signal but adding ring widths leads to little improvement. Blue intensity, an inexpensive alternative to X‐ray densitometry, is shown to perform similarly. Multi‐proxy reconstruction of summer temperatures from a single site produces strong correlations with gridded climate data over most of northern Fennoscandia. Since relatively few trees are required (<15) the approach could be applied to long sub‐fossil chronologies where replication may be episodically low. Copyright © 2010 John Wiley & Sons, Ltd.  相似文献   

Estimation of flood damage functions for river basin planning: a case study in Bangladesh     

Y. C. Ethan Yang  Patrick A. Ray  Casey M. Brown  Abedalrazq F. Khalil  Winston H. Yu 《Natural Hazards》2015,75(3):2773-2791

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Water source dynamics of high Arctic river basins          下载免费PDF全文

Phillip J. Blaen  David M. Hannah  Lee E. Brown  Alexander M. Milner 《水文研究》2014,28(10):3521-3538

Arctic river basins are amongst the most vulnerable to climate change. However, there is currently limited knowledge of the hydrological processes that govern flow dynamics in Arctic river basins. We address this research gap using natural hydrochemical and isotopic tracers to identify water sources that contributed to runoff in river basins spanning a gradient of glacierization (0–61%) in Svalbard during summer 2010 and 2011. Spatially distinct hydrological processes operating over diurnal, weekly and seasonal timescales were characterized by river hydrochemistry and isotopic composition. Two conceptual water sources (‘meltwater’ and ‘groundwater’) were identified and used as a basis for end‐member mixing analyses to assess seasonal and year‐to‐year variability in water source dynamics. In glacier‐fed rivers, meltwater dominated flows at all sites (typically >80%) with the highest contributions observed at the beginning of each study period in early July when snow cover was most extensive. Rivers in non‐glacierized basins were sourced initially from snowmelt but became increasingly dependent on groundwater inputs (up to 100% of total flow volume) by late summer. These hydrological changes were attributed to the depletion of snowpacks and enhanced soil water storage capacity as the active layer expanded throughout each melt season. These findings provide insight into the processes that underpin water source dynamics in Arctic river systems and potential future changes in Arctic hydrology that might be expected under a changing climate. Copyright © 2013 John Wiley & Sons, Ltd.  相似文献   

Reply to Comment on “Post‐impact event bed (tsunamite) at the Cretaceous–Palaeogene boundary deposited on a distal carbonate platform interior”          下载免费PDF全文

Tvrtko Korbar  Iain McDonald  Vlasta Premec Fućek  Ladislav Fuček  Hrvoje Posilović 《地学学报》2017,29(5):332-334

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Modelling the influences of climate change-associated sea-level rise and socioeconomic development on future storm surge mortality     

Simon J. Lloyd  R. Sari Kovats  Zaid Chalabi  Sally Brown  Robert J. Nicholls 《Climatic change》2016,134(3):441-455

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Drivers of ecosystem and climate change in tropical West Africa over the past ∼540 000 years          下载免费PDF全文

Charlotte S. Miller  Angela L. Coe  Iain Gilmour 《第四纪科学杂志》2016,31(7):671-677

A paucity of empirical non‐marine data means that uncertainty surrounds the impact of climate change on terrestrial ecosystems in tropical regions beyond the last glacial period. The sedimentary fill of the Bosumtwi impact crater (Ghana) provides the longest continuous Quaternary terrestrial archive of environmental change in West Africa, spanning the last ～1.08 million years. Here we explore the drivers of change in ecosystem and climate in tropical West Africa for the past ～540 000 years using pollen analysis and the nitrogen isotope composition of bulk organic matter preserved in sediments from Lake Bosumtwi. Variations in grass pollen abundance (0?99%) indicate transitions between grassland and forest. Coeval variations in the nitrogen isotopic composition of organic matter indicate that intervals of grassland expansion coincided with minimum lake levels and low regional moisture availability. The observed changes responded to orbitally paced global climate variations on both glacial–interglacial and shorter timescales. Importantly, the magnitude of ecosystem change revealed by our data exceeds that previously determined from marine records, demonstrating for the first time the high sensitivity of tropical lowland ecosystems to Quaternary climate change.

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