Identification of Uranyl Minerals Using Oxygen K‐Edge X‐Ray Absorption Spectroscopy          下载免费PDF全文

Jesse D. Ward  Mark Bowden  C. Tom Resch  Steven Smith  Bruce K. McNamara  Edgar C. Buck  Gregory C. Eiden  Andrew M. Duffin 《Geostandards and Geoanalytical Research》2016,40(1):135-148

Although most of the world's uranium exists as pitchblende or uraninite, this mineral can be weathered to a great variety of secondary uranium minerals, most containing the uranyl cation. Anthropogenic uranium compounds can also react in the environment, leading to spatial–chemical alterations that could be useful for nuclear forensics analyses. Soft X‐ray absorption spectroscopy (XAS) has the advantages of being non‐destructive, element‐specific and sensitive to electronic and physical structure. The soft X‐ray probe can also be focused to a spot size on the order of tens of nanometres, providing chemical information with high spatial resolution. However, before XAS can be applied at high spatial resolution, it is necessary to find spectroscopic signatures for a variety of uranium compounds in the soft X‐ray spectral region. To that end, we collected the near edge X‐ray absorption fine structure (NEXAFS) spectra of a variety of common uranyl‐bearing minerals, including uranyl carbonates, oxyhydroxides, phosphates and silicates. We find that uranyl compounds can be distinguished by class (carbonate, oxyhydroxide, phosphate or silicate) based on their oxygen K‐edge absorption spectra. This work establishes a database of reference spectra for future spatially resolved analyses. We proceed to show scanning X‐ray transmission microscopy (STXM) data from a schoepite particle in the presence of an unknown contaminant.  相似文献   

High Precision Sr‐Nd‐Hf‐Pb Isotopic Compositions of USGS Reference Material BCR‐2          下载免费PDF全文

Jason Jweda  Louise Bolge  Cornelia Class  Steven L. Goldstein 《Geostandards and Geoanalytical Research》2016,40(1):101-115

The Lamont‐Doherty Earth Observatory radiogenic isotope group has been systematically measuring Sr‐Nd‐Pb‐Hf isotopes of USGS reference material BCR‐2 (Columbia River Basalt 2), as a chemical processing and instrumental quality control monitor for isotopic measurements. BCR‐2 is now a widely used geochemical inter‐laboratory reference material (RM), with its predecessor BCR‐1 no longer available. Recognising that precise and accurate data on RMs is important for ensuring analytical quality and for comparing data between different laboratories, we present a compilation of multiple digestions and analyses made on BCR‐2 during the first author's dissertation research. The best estimates of Sr, Nd and Hf isotope ratios and measurement reproducibilities, after filtering at the 2s level for outliers, were ⁸⁷Sr/⁸⁶Sr = 0.705000 ± 11 (2s, 16 ppm, n = 21, sixteen digestions, one outlier), ¹⁴³Nd/¹⁴⁴Nd = 0.512637 ± 13 (2s, 25 ppm, n = 27, thirteen digestions, one outlier) and ¹⁷⁶Hf/¹⁷⁷Hf = 0.282866 ± 11 (2s, 39 ppm, n = 25, thirteen digestions, no outliers). Mean Nd and Hf values were within error of those reported by Weis et al. (2006, 2007) in their studies of RMs; mean Sr values were just outside the 2s uncertainty range of both laboratories. Moreover, a survey of published Sr‐Nd‐Hf data shows that our results fall within the range of reported values, but with a smaller variability. Our Pb isotope results on acid leached BCR‐2 aliquots (n = 26, twelve digestions, two outliers) were ²⁰⁶Pb/²⁰⁴Pb = 18.8029 ± 10 (2s, 55 ppm), ²⁰⁷Pb/²⁰⁴Pb = 15.6239 ± 8 (2s, 52 ppm), ²⁰⁸Pb/²⁰⁴Pb = 38.8287 ± 25 (2s, 63 ppm). We confirm that unleached BCR‐2 powder is contaminated with Pb, and that sufficient leaching prior to digestion is required to achieve accurate values for the uncontaminated Pb isotopic compositions.  相似文献   

Adjoint analysis of Buckley-Leverett and two-phase flow equations     

Savithru Jayasinghe  David L. Darmofal  Marshall C. Galbraith  Nicholas K. Burgess  Steven R. Allmaras 《Computational Geosciences》2018,22(2):527-542

This paper analyzes the adjoint equations and boundary conditions for porous media flow models, specifically the Buckley-Leverett equation, and the compressible two-phase flow equations in mass conservation form. An adjoint analysis of a general scalar hyperbolic conservation law whose primal solutions include a shock jump is initially presented, and the results are later specialized to the Buckley-Leverett equation. The non-convexity of the Buckley-Leverett flux function results in adjoint characteristics that are parallel to the shock front upstream of the shock and emerge from the shock front downstream of the shock. Thus, in contrast to the behavior of Burgers’ equation where the adjoint is continuous at a shock, the Buckley-Leverett adjoint, in general, contains a discontinuous jump across the shock. Discrete adjoint solutions from space-time discontinuous Galerkin finite element approximations of the Buckley-Leverett equation are shown to be consistent with the derived closed-form analytical solutions. Furthermore, a general result relating the adjoint equations for different (though equivalent) primal equations is used to relate the two-phase flow adjoints to the Buckley-Leverett adjoint. Adjoint solutions from space-time discontinuous Galerkin finite element approximations of the two-phase flow equations are observed to obey this relationship.  相似文献   

Upstream—Downstream Shifts in Peak Recruitment of the Native Olympia Oyster in San Francisco Bay During Wet and Dry Years     

Andrew L. Chang  Lindsay J. Sullivan  Steven G. Morgan  Matthew C. Ferner 《Estuaries and Coasts》2018,41(1):65-78

Understanding the conditions that drive variation in recruitment of key estuarine species can be important for effective conservation and management of their populations. The Olympia oyster (Ostrea lurida) is native to the Pacific coast of North America and has been a target of conservation efforts, though relatively little information on larval recruitment exists across much of its range. This study examined the recruitment of Olympia oysters at biweekly to monthly intervals at four sites in northern San Francisco Bay from 2010 to 2015 (except 2013). Mean monthly temperatures warmed at all sites during the study, while winter (January–April) mean monthly salinity decreased significantly during a wet year (2011), but otherwise remained high as a result of a drought. A recurring peak in oyster recruitment was identified in mid-estuary, in conditions corresponding to a salinity range of 25–30 and >16 °C at the time of settlement (April–November). Higher average salinities and temperatures were positively correlated with greater peak recruitment. Interannual variation in the timing of favorable conditions for recruitment at each site appears to explain geographic and temporal variation in recruitment onset. Higher winter/spring salinities and warmer temperatures at the time of recruitment corresponded with earlier recruitment onset within individual sites. Across all sites, higher winter/spring salinities were also correlated with earlier onset and earlier peak recruitment. Lower winter salinities during 2011 also resulted in a downstream shift in the location of peak recruitment.  相似文献   

Defining the Potential of Nanoscale Re‐Os Isotope Systematics Using Atom Probe Microscopy          下载免费PDF全文

Luke Daly  Phil A. Bland  Svetlana Tessalina  David W. Saxey  Steven M. Reddy  Denis Fougerouse  William D.A. Rickard  Lucy V. Forman  Alexandre La Fontaine  Julie M. Cairney  Simon P. Ringer  Bruce F. Schaefer  Daniel Schwander 《Geostandards and Geoanalytical Research》2018,42(3):279-299

Atom probe microscopy (APM) is a relatively new in situ tool for measuring isotope fractions from nanoscale volumes (< 0.01 μm³). We calculate the theoretical detectable difference of an isotope ratio measurement result from APM using counting statistics of a hypothetical data set to be ± 4δ or 0.4% (2s). However, challenges associated with APM measurements (e.g., peak ranging, hydride formation and isobaric interferences), result in larger uncertainties if not properly accounted for. We evaluate these factors for Re‐Os isotope ratio measurements by comparing APM and negative thermal ionisation mass spectrometry (N‐TIMS) measurement results of pure Os, pure Re, and two synthetic Re‐Os‐bearing alloys from Schwander et al. (2015, Meteoritics and Planetary Science, 50, 893) [the original metal alloy (HSE) and alloys produced by heating HSE within silicate liquid (SYN)]. From this, we propose a current best practice for APM Re‐Os isotope ratio measurements. Using this refined approach, mean APM and N‐TIMS ¹⁸⁷Os/¹⁸⁹Os measurement results agree within 0.05% and 2s (pure Os), 0.6–2% and 2s (SYN) and 5–10% (HSE). The good agreement of N‐TIMS and APM ¹⁸⁷Os/¹⁸⁹Os measurements confirms that APM can extract robust isotope ratios. Therefore, this approach permits nanoscale isotope measurements of Os‐bearing alloys using the Re‐Os geochronometer that could not be measured by conventional measurement principles.  相似文献   

Pattern,style and timing of British–Irish Ice Sheet advance and retreat over the last 45 000 years: evidence from NW Scotland and the adjacent continental shelf     

Tom Bradwell  Derek Fabel  Chris D. Clark  Richard C. Chiverrell  David Small  Rachel K. Smedley  Margot H. Saher  Steven G. Moreton  Dayton Dove  S. Louise Callard  Geoff A. T. Duller  Alicia Medialdea  Mark D. Bateman  Matthew J. Burke  Neil McDonald  Sean Gilgannon  Sally Morgan  David H. Roberts  Colm ó Cofaigh 《第四纪科学杂志》2021,36(5):871-933

Predicting the future response of ice sheets to climate warming and rising global sea level is important but difficult. This is especially so when fast-flowing glaciers or ice streams, buffered by ice shelves, are grounded on beds below sea level. What happens when these ice shelves are removed? And how do the ice stream and the surrounding ice sheet respond to the abruptly altered boundary conditions? To address these questions and others we present new geological, geomorphological, geophysical and geochronological data from the ice-stream-dominated NW sector of the last British–Irish Ice Sheet (BIIS). The study area covers around 45 000 km² of NW Scotland and the surrounding continental shelf. Alongside seabed geomorphological mapping and Quaternary sediment analysis, we use a suite of over 100 new absolute ages (including cosmogenic-nuclide exposure ages, optically stimulated luminescence ages and radiocarbon dates) collected from onshore and offshore, to build a sector-wide ice-sheet reconstruction combining all available evidence with Bayesian chronosequence modelling. Using this information we present a detailed assessment of ice-sheet advance/retreat history, and the glaciological connections between different areas of the NW BIIS sector, at different times during the last glacial cycle. The results show a highly dynamic, partly marine, partly terrestrial, ice-sheet sector undergoing large size variations in response to sub-millennial-scale climatic (Dansgaard–Oeschger) cycles over the last 45 000 years. Superimposed on these trends we identify internally driven instabilities, operating at higher frequency, conditioned by local topographic factors, tidewater dynamics and glaciological feedbacks during deglaciation. Specifically, our new evidence indicates extensive marine-terminating ice-sheet glaciation of the NW BIIS sector during Greenland Stadials 12 to 9 – prior to the main ‘Late Weichselian’ ice-sheet glaciation. After a period of restricted glaciation, in Greenland Interstadials 8 to 6, we find good evidence for rapid renewed ice-sheet build-up in NW Scotland, with the Minch ice-stream terminus reaching the continental shelf edge in Greenland Stadial 5, perhaps only briefly. Deglaciation of the NW sector took place in numerous stages. Several grounding-zone wedges and moraines on the mid- and inner continental shelf attest to significant stabilizations of the ice-sheet grounding line, or ice margin, during overall retreat in Greenland Stadials 3 and 2, and to the development of ice shelves. NW Lewis was the first substantial present-day land area to deglaciate, in the first half of Greenland Stadial 3 at a time of globally reduced sea-level c. 26 kabp , followed by Cape Wrath at c. 24 kabp. The topographic confinement of the Minch straits probably promoted ice-shelf development in early Greenland Stadial 2, providing the ice stream with additional support and buffering it somewhat from external drivers. However, c. 20–19 kabp , as the grounding-line migrated into shoreward deepening water, coinciding with a marked change in marine geology and bed strength, the ice stream became unstable. We find that, once underway, grounding-line retreat proceeded in an uninterrupted fashion with the rapid loss of fronting ice shelves – first in the west, then the east troughs – before eventual glacier stabilization at fjord mouths in NW Scotland by ~17 kabp. Around the same time, ~19–17 kabp , ice-sheet lobes readvanced into the East Minch – possibly a glaciological response to the marine-instability-triggered loss of adjacent ice stream (and/or ice shelf) support in the Minch trough. An independent ice cap on Lewis also experienced margin oscillations during mid-Greenland Stadial 2, with an ice-accumulation centre in West Lewis existing into the latter part of Heinrich Stadial 1. Final ice-sheet deglaciation of NW mainland Scotland was punctuated by at least one other coherent readvance at c. 15.5 kabp , before significant ice-mass losses thereafter. At the glacial termination, c. 14.5 kabp , glaciers fed outwash sediment to now-abandoned coastal deltas in NW mainland Scotland around the time of global Meltwater Pulse 1A. Overall, this work on the BIIS NW sector reconstructs a highly dynamic ice-sheet oscillating in extent and volume for much of the last 45 000 years. Periods of expansive ice-sheet glaciation dominated by ice-streaming were interspersed with periods of much more restricted ice-cap or tidewater/fjordic glaciation. Finally, this work indicates that the role of ice streams in ice-sheet evolution is complex but mechanistically important throughout the lifetime of an ice sheet – with ice streams contributing to the regulation of ice-sheet health but also to the acceleration of ice-sheet demise via marine ice-sheet instabilities.  相似文献   

Correction: Hydraulic tomography analysis of municipal-well operation data with geology-based groundwater models     

Tong  Xin  Illman  Walter A.  Berg  Steven J.  Luo  Ning 《Hydrogeology Journal》2021,29(5):1999-2000

Hydrogeology Journal - A Correction to this paper has been published: https://doi.org/10.1007/s10040-021-02351-x  相似文献   

Holocene and Eemian climatic optima in the Korean Peninsula based on textural and carbon isotopic records from the stalagmite of the Daeya Cave,South Korea     

Kyoung-nam Jo  Kyung Sik Woo  Hyoun Soo Lim  Hai Cheng  R. Lawrence Edwards  Yongjin Wang  Xiuyang Jiang  Ryeon Kim  Jae Il Lee  Ho Il Yoon  Kyu-Cheul Yoo 《Quaternary Science Reviews》2011,30(9-10):1218-1231

Textural and stable isotopic records from the absolute-dated stalagmite of the Daeya Cave (DY-1) provide new insights into the climatic evolution of the Korean Peninsula during the Holocene and Eemian climatic optima. The stalagmite yielded ages of 8572 ± 227 to 5907 ± 158 and 1,23,456 ± 535 to 1,19,837 ± 1089 years, which coincide with the Holocene and Eemian climatic optima, respectively. The stalagmite’s δ¹³C record closely resembles previously reported Chinese speleothem δ¹⁸O data. Thus it can be suggested that textural and geochemical results of the DY-1 reflect East Asian monsoon intensity, which is forced by summer insolation patterns in the northern hemisphere. Lighter carbon isotopic compositions, well-developed fibrous calcite crystals, and their relatively faster growth rate in the stalagmite sample are interpreted to reflect the warmest and wettest climate conditions of the Holocene and Eemian interglacials. Both climatic optima took place when insolation was decreasing from its maximum level, temperature in Greenland was highest, and sea level approached its maximum level. These climatic optima also coincide with decreasing Antarctic temperatures. Compared the DY-1 data to other proxies, it is suggested that the Holocene and Eemian climatic optima developed through a balance among boreal insolation, monsoon intensity, and sea level (also continental ice volume), which are the main climatic forcing factors in the northern hemisphere. These trends also follow the bi-polar seesaw mechanism as previously described.  相似文献   

Climate justice and global cities: Mapping the emerging discourses     

Harriet Bulkeley  JoAnn Carmin  Vanesa Castán Broto  Gareth A.S. Edwards  Sara Fuller 《Global Environmental Change》2013,23(5):914-925

Ever since climate change came to be a matter of political concern, questions of justice have been at the forefront of academic and policy debates in the international arena. Curiously, as attention has shifted to other sites and scales of climate change politics matters of justice have tended to be neglected. In this paper, we examine how discourses of justice are emerging within urban responses to climate change. Drawing on a database of initiatives taking place in 100 global cities and qualitative case-study research in Philadelphia, Quito and Toronto, we examine how notions of distributive and procedural justice are articulated in climate change projects and plans in relation to both adaptation and mitigation. We find that there is limited explicit concern with justice at the urban level. However, where discourses of justice are evident there are important differences emerging between urban responses to adaptation and mitigation, and between those in the north and in the south. Adaptation responses tend to stress the distribution of ‘rights’ to protection, although those in the South also stress the importance of procedural justice. Mitigation responses also stress ‘rights’ to the benefits of responding to climate change, with limited concern for ‘responsibilities’ or for procedural justice. Intriguingly, while adaptation responses tend to stress the rights of individuals, we also find discourses of collective rights emerging in relation to mitigation.  相似文献   

Sensitivity of ADOM dry deposition velocities to input parameters: A comparison with measurements for SO2 and NO2 over three land use types     

J. Padro  G.C. Edwards 《大气与海洋》2013,51(4):667-685

Abstract

Dry deposition velocity measurements of SO₂ and NO₂ over a deciduous forest, a carrot field and a snow surface are compared with estimates obtained from the dry deposition module in the regional Eulerian Acid Deposition and Oxidant Model (ADOM). The comparison with measurements taken in the fall and winter shows large model overestimates, sometimes as large as a factor of 5. The NO₂ estimates are particularly poor and support existing evidence that models that employ the constant flux assumption for NO₂ are inadequate. The canopy and the snow surface resistances are the largest contributors to the total resistances for SO₂ and NO₂, except for situations in which some of the snow turns into liquid water, when the aerodynamic resistance becomes important.

Increasing the magnitudes, taken from measurements, of the ADOM original values for the stomatal, cuticle, ground and snow resistances and decreasing the NO₂ mesophyll resistance and the Leaf Area Index (LAI) yield improved model results, particularly for SO₂, reducing the error by almost a factor of 5 at times. The new estimates compare favourably with those from a model that includes Wesely's canopy resistance parametrization. Over snow the NO₂ estimates are improved by as much as a factor of 6. Observed deposition velocities for SO₂ vary from 0 to 0.65 cm s^?2 over a deciduous forest, 0 to 0.60 cm s^?2 over a carrot field and are generally less than 0.05 cm s^?2 over snow.  相似文献