Arsenic redox transformation by humic substances and Fe minerals     

Andreas Kappler  Katja Amstaetter  Thomas Borch  Philip Larese-Casanova  Jie Jiang  Iris Bauer  Andrea Paul 《Applied Geochemistry》2011

The toxicity and mobility of the redox-active metalloid As strongly depends on its oxidation state, with As(III) (arsenite) being more toxic and mobile than As(V) (arsenate). It is, therefore, necessary to know the biogeochemical processes potentially influencing As redox state to understand and predict its environmental behavior. The first part of this presentation will discuss the quantification of As redox changes by pH-neutral mineral suspensions of goethite [α-Fe^IIIOOH] amended with Fe(II) using wet-chemical and synchrotron X-ray absorption (XANES) analysis (Amstaetter et al., 2010). First, it was found that goethite itself did not oxidize As(III). Second, in contrast to thermodynamic predictions, Fe(II)–goethite systems did not reduce As(V). However, surprisingly, rapid oxidation of As(III) to As(V) was observed in Fe(II)–goethite systems. Iron speciation and mineral analysis by Mössbauer spectroscopy showed rapid formation of ⁵⁷Fe–goethite after ⁵⁷Fe(II) addition and the formation of a so far unidentified additional Fe(II) phase. No other Fe(III) phase could be detected by Mössbauer spectroscopy, EXAFS, scanning electron microscopy, X-ray diffraction or high-resolution transmission electron microscopy. This suggests that reactive Fe(III) species form as an intermediate Fe(III) phase upon Fe(II) addition and electron transfer into bulk goethite but before crystallization of the newly formed Fe(III) as goethite.The second part of the presentation will show that semiquinone radicals produced during microbial or chemical reduction of a humic substance model quinone (AQDS, 9,10-anthraquinone-2,6-disulfonic acid) can react with As and change its redox state (Jiang et al., 2009). The results of these experiments showed that these semiquinone radicals are strong oxidants and oxidize arsenite to arsenate, thus decreasing As toxicity and mobility. The oxidation of As(III) depended strongly on pH. More arsenite (up to 67.3%) was oxidized at pH 11 compared to pH 7 (12.6% oxidation) and pH 3 (0.5% oxidation). In addition to As(III) oxidation by semiquinone radicals, hydroquinones that were also produced during quinone reduction, reduced As(V) to As(III) at neutral and acidic pH values (less than 12%) but not at alkaline pH. In an attempt to understand the observed redox reactions between As and reduced/oxidized quinones present in humic substances, the radical content in reduced AQDS solutions was quantified and Eh-pH diagrams were constructed. Both the radical quantification and the Eh-pH diagram allowed explaining the observed redox reactions between the reduced AQDS solutions and the As.In summary these studies indicate that in the simultaneous presence of Fe(III) oxyhydroxides, Fe(II), and humic substances as commonly observed in environments inhabited by Fe-reducing microorganisms, As(III) oxidation can occur. This potentially explains the presence of As(V) in reduced groundwater aquifers.  相似文献   

Is Ocean Acidification an Open-Ocean Syndrome? Understanding Anthropogenic Impacts on Seawater pH   总被引：2，自引：0，他引：2  

Carlos M. Duarte  Iris E. Hendriks  Tommy S. Moore  Ylva S. Olsen  Alexandra Steckbauer  Laura Ramajo  Jacob Carstensen  Julie A. Trotter  Malcolm McCulloch 《Estuaries and Coasts》2013,36(2):221-236

Ocean acidification due to anthropogenic CO₂ emissions is a dominant driver of long-term changes in pH in the open ocean, raising concern for the future of calcifying organisms, many of which are present in coastal habitats. However, changes in pH in coastal ecosystems result from a multitude of drivers, including impacts from watershed processes, nutrient inputs, and changes in ecosystem structure and metabolism. Interaction between ocean acidification due to anthropogenic CO₂ emissions and the dynamic regional to local drivers of coastal ecosystems have resulted in complex regulation of pH in coastal waters. Changes in the watershed can, for example, lead to changes in alkalinity and CO₂ fluxes that, together with metabolic processes and oceanic dynamics, yield high-magnitude decadal changes of up to 0.5 units in coastal pH. Metabolism results in strong diel to seasonal fluctuations in pH, with characteristic ranges of 0.3 pH units, with metabolically intense habitats exceeding this range on a daily basis. The intense variability and multiple, complex controls on pH implies that the concept of ocean acidification due to anthropogenic CO₂ emissions cannot be transposed to coastal ecosystems directly. Furthermore, in coastal ecosystems, the detection of trends towards acidification is not trivial and the attribution of these changes to anthropogenic CO₂ emissions is even more problematic. Coastal ecosystems may show acidification or basification, depending on the balance between the invasion of coastal waters by anthropogenic CO₂, watershed export of alkalinity, organic matter and CO₂, and changes in the balance between primary production, respiration and calcification rates in response to changes in nutrient inputs and losses of ecosystem components. Hence, we contend that ocean acidification from anthropogenic CO₂ is largely an open-ocean syndrome and that a concept of anthropogenic impacts on marine pH, which is applicable across the entire ocean, from coastal to open-ocean environments, provides a superior framework to consider the multiple components of the anthropogenic perturbation of marine pH trajectories. The concept of anthropogenic impacts on seawater pH acknowledges that a regional focus is necessary to predict future trajectories in the pH of coastal waters and points at opportunities to manage these trajectories locally to conserve coastal organisms vulnerable to ocean acidification.  相似文献   

The great sulfur depletion of Earth’s mantle is not a signature of mantle–core equilibration     

Chris?BallhausEmail author  Raúl?O.?C.?Fonseca  Carsten?Münker  Arno?Rohrbach  Thorsten?Nagel  Iris?M.?Speelmanns  Hassan?M.?Helmy  Aurelia?Zirner  Antje?K.?Vogel  Alexander?Heuser 《Contributions to Mineralogy and Petrology》2017,172(8):68

The extreme depletion of the Earth’s mantle in sulfur is commonly seen as a signature of metal segregation from Earth’s mantle to Earth’s core. However, in addition to S, the mantle contains other elements as volatile as S that are hardly depleted relative to the lithophile volatility trend although they are potentially as siderophile as sulfur. We report experiments in metal-sulfide–silicate systems to show that the CI normalized abundances of S, Pb, and Sn in Earth’s mantle cannot be reproduced by element partitioning in Fe ± S–silicate systems, neither at low nor at high pressure. Much of the volatile inventory of the Earth’s mantle must have been added late in the accretion history, when metal melt segregation to the core had become largely inactive. The great depletion in S is attributed to the selective segregation of a late sulfide matte from an oxidized and largely crystalline mantle. Apparently, the volatile abundances of Earth’s mantle are not in redox equilibrium with Earth’s core.  相似文献   

Physical characteristics of Acidic Mining Lake 111     

G?kay?KarakasEmail author  Iris?Brookland  Bertram?Boehrer 《Aquatic Sciences - Research Across Boundaries》2003,65(3):297-307

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Bioassay‐directed fractionation for analyzing estrogens in surface waters of the German Baltic Sea     

Iris‐Constanze Beck  Regina Bruhn  Juergen Gandrass 《洁净——土壤、空气、水》2006,34(6):560-567

A reversed‐phase fractionation method with subsequent biological and chemical analysis has been developed to estimate the contributions of the most potent estrogens to observed estrogenic effect potentials. Surface water samples were taken in the German Baltic Sea (Inner Wismar Bay and Darss Peninsula, sampling campaign July 2003) and were separated into seven individual fractions. Three fractions showed significant estrogenic activities and clear dose‐dependant responses were obtained in the yeast estrogen screen (YES). In the 2nd fractions liquid chromatographic‐electrospray‐tandem mass spectrometric (LC‐ESI‐MS‐MS) analyses showed the presence of bisphenol A (Inner Wismar Bay: 4.8 ng L^–1 and 6 ng L^–1; Darss Peninsula: 0.91 ng L^–1 and 1.7 ng L^–1) and ethinylestradiol (Inner Wismar Bay: 2.0 ng L^–1 and 6.0 ng L^–1; Darss Peninsula: < MDL and 1.7 ng L^–1), whereas estrogenic activities in the YES were only around 10% of the positive control E2. Although not identified prior in the total extract the natural hormones estradiol (Inner Wismar Bay: 0.13 ng L^–1 and 0.19 ng L^–1; Darss Peninsula: 0.12 ng L^–1 and 0.16 ng L^–1) and estriol (Inner Wismar Bay: < MDL and 0.33 ng L^–1; Darss Peninsula: < MDL) could be detected in the 3rd fractions, where high estrogenic potentials could be observed. The 4th fractions showed high responses as well and estrone were herein quantified with concentrations of 0.16 ng L^–1 and 0.18 ng L^–1 (Darss Peninsula) up to 0.37 ng L^–1 (Inner Wismar Bay). Measured and calculated estradiol equivalents for individual fractions correlated very well (R² = 0.78), when disregarding results of the 2nd fraction, where high deviations occurred.  相似文献   

What is the Meaning of ‘Social Mix’? Shifting perspectives in planning and implementing public housing estate redevelopment     

Kathy Arthurson  Iris Levin  Anna Ziersch 《The Australian geographer》2015,46(4):491-505

This paper unravels a variety of perspectives about the concept of social mix, drawing on a case study of the implementation of a redevelopment project in Melbourne. The first part provides a theoretical overview of two internationally predominant academic debates around policy interpretations of this concept, namely social mix as a means for promotion of social inclusion; and as a state-led form of gentrification. These two arguments are usually presented as one, with social inclusion and reductions of concentrations of disadvantage one side of the ‘social mix policy’ coin, and state-led gentrification the other. This paper contributes to the national and international literature on public housing estate regeneration and social mix policies through exploring the question of whether these two ideas about social mix were shared by different stakeholders as the ‘messy’ process of redevelopment unfurled. Interviews were conducted with public tenants, homeowners and homebuyers, private renters and local service providers at the Carlton Housing Estate to explore the diverse perspectives of various stakeholder groups as estate design and implementation shifted. The study identified that as a result of the global financial crisis and the developers exerting pressure on government there was a gradual move away from perceiving social mix as a policy tool for encouraging social inclusion at Carlton, between public housing tenants and private residents, towards a different form of social mix and inclusion. Contrary to intentions, the revised form of social mix at Carlton was perceived as a means to harness market capital and attract higher income residents to the inner city.  相似文献   

Effects of land cover change on streamflow in the interior Columbia River Basin (USA and Canada)     

Bernt Matheussen  Robin L. Kirschbaum  Iris A. Goodman  Greg M. O'Donnell  Dennis P. Lettenmaier 《水文研究》2000,14(5):867-885

An analysis of the hydrological effects of vegetation changes in the Columbia River basin over the last century was performed using two land cover scenarios. The first was a reconstruction of historical land cover vegetation, c. 1900, as estimated by the federal Interior Columbia Basin Ecosystem Management Project (ICBEMP). The second was current land cover as estimated from remote sensing data for 1990. Simulations were performed using the variable infiltration capacity (VIC) hydrological model, applied at one‐quarter degree spatial resolution (approximately 500 km² grid cell area) using hydrometeorological data for a 10 year period starting in 1979, and the 1900 and current vegetation scenarios. The model represents surface hydrological fluxes and state variables, including snow accumulation and ablation, evapotranspiration, soil moisture and runoff production. Simulated daily hydrographs of naturalized streamflow (reservoir effects removed) were aggregated to monthly totals and compared for nine selected sub‐basins. The results show that, hydrologically, the most important vegetation‐related change has been a general tendency towards decreased vegetation maturity in the forested areas of the basin. This general trend represents a balance between the effects of logging and fire suppression. In those areas where forest maturity has been reduced as a result of logging, wintertime maximum snow accumulations, and hence snow available for runoff during the spring melt season, have tended to increase, and evapotranspiration has decreased. The reverse has occurred in areas where fire suppression has tended to increase vegetation maturity, although the logging effect appears to dominate for most of the sub‐basins evaluated. Predicted streamflow changes were largest in the Mica and Corralin sub‐basins in the northern and eastern headwaters region; in the Priest Rapids sub‐basin, which drains the east slopes of the Cascade Mountains; and in the Ice Harbor sub‐basin, which receives flows primarily from the Salmon and Clearwater Rivers of Idaho and western Montana. For these sub‐basins, annual average increases in runoff ranged from 4·2 to 10·7% and decreases in evapotranspiration ranged from 3·1 to 12·1%. In comparison with previous studies of individual, smaller sized watersheds, the modelling approach used in this study provides predictions of hydrological fluxes that are spatially continuous throughout the interior Columbia River basin. It thus provides a broad‐scale framework for assessing the vulnerability of watersheds to altered streamflow regimes attributable to changes in land cover that occur over large geographical areas and long time‐frames. Copyright © 2000 John Wiley & Sons, Ltd.  相似文献   

Stormy geomorphology: an introduction to the Special Issue          下载免费PDF全文

Tom Spencer  Larissa Naylor  Stuart Lane  Stephen Darby  Mark Macklin  Francis Magilligan  Iris Möller 《地球表面变化过程与地形》2017,42(1):238-241

The degree to which the climate change signal can be seen in the increasing frequency and/or magnitude of extreme events forms a key part of the global environmental change agenda. Geomorphology engages with this debate through extending the instrumental record with palaeogeomorphological research; studying resilience and recovery of geomorphic systems under extreme disturbance; documenting the mediation by catchment organisation of transport processes during extreme events; applying new monitoring methods to better understand process‐response systems; and illustrating how process, experimental and modelling insights can be used to define the buffering of geomorphic systems and human assets from the effects of extremes, providing practical outcomes for practitioners. Copyright © 2016 John Wiley & Sons, Ltd.  相似文献   

Identification of extreme storm surges with high-impact potential along the German North Sea coastline     

Anette Ganske  Natacha Fery  Lidia Gaslikova  Iris Grabemann  Ralf Weisse  Birger Tinz 《Ocean Dynamics》2018,68(10):1371-1382

Planning and design of coastal protection rely on information about the probabilities of very severe storm tides and the possible changes that may occur in the course of climate change. So far, this information is mostly provided in the form of high percentiles obtained from frequency distributions or return values. More detailed information and assessments of events that may cause extreme damages or have extreme consequences at the coast are so far still unavailable. We describe and compare two different approaches that may be used to identify highly unlikely but still physically possible and plausible events from model simulations. Firstly, in the case when consistent wind and tide-surge data are available, different metrics such as the height of the storm surge can be derived directly from the simulated water levels. Secondly, in cases where only atmospheric data are available, the so called effective wind may be used. The latter is the projection of the horizontal wind vector on that direction which is most effective in producing surges at the coast. Comparison of events identified by both methods show that they can identify extreme events but that knowledge of the effective wind alone does not provide sufficient information to identify the highest storm surges. Tracks of the low-pressure systems over the North Sea need to be investigated to find those cases, where the duration of the high wind is too short to induce extreme storm tides. On the other hand, factors such as external surges or variability in mean sea level may enhance surge heights and are not accounted for in estimates based on effective winds only. Results from the analysis of an extended data set suggest that unprecedented storm surges at the German North Sea coast are possible even without taking effects from rising mean sea level into account. The work presented is part of the ongoing project “Extreme North Sea Storm Surges and Their Consequences” (EXTREMENESS) and represents the first step towards an impact assessment for very severe storm surges which will serve as a basis for development of adaptation options and evaluation criteria.  相似文献   

Spatial and temporal characteristics of nutrient and phytoplankton dynamics in the York River Estuary, Virginia: Analyses of long-term data   总被引：1，自引：0，他引：1  

Yongsik Sin  Richard L. Wetzel  Iris C. Anderson 《Estuaries and Coasts》1999,22(2):260-275

Ten years (1985–1994) of data were analyzed to investigate general patterns of phytoplankton and nutrient dynamics, and to identify major factors controlling those dynamics in the York River Estuary, Virginia. Algal blooms were observed during winter-spring followed by smaller summer blooms. Peak phytoplankton biomass during the winter-spring blooms occurred in the mid reach of the mesohaline zone whereas peak phytoplankton biomass during the summer bloom occurred in the tidal fresh-mesohaline transition zone. River discharge appears to be the major factor controlling the location and timing of the winter-spring blooms and the relative degree of potential N and P limitation. Phytoplankton biomass in tidal fresh water regions was limited by high flushing rates. Water residence time was less than cell doubling time during high flow seasons. Positive correlations between PAR at 1 m depth and chlorophylla suggested light limitation of phytoplankton in the tidal fresh-mesohaline transition zone. Relationships of salinity difference between surface and bottom water with chlorophylla distribution suggested the importance of tidal mixing for phytoplankton dynamics in the mesohaline zone. Accumulation of phytoplankton biomass in the mesohaline zone was generally controlled by N with the nutrient supply provided by benthic or bottom water remineralization.  相似文献