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681.
Gregory K. Druschel Robert J. Hamers George W. Luther III Jillian F. Banfield 《Aquatic Geochemistry》2003,9(2):145-164
The oxidation kinetics of trithionate (S3O62-
) and tetrathionate (S4O
6
2-
) with hydroxyl radicals (OH*) have been investigated in systems analogous to acid mine drainage (AMD) environments. The discovery of hydroxyl radical
(OH*) formation on pyrite surfaces (Borda et al., 2003) suggests hydroxyl radicals may affect the oxidation kinetics of intermediate
sulfur species such as tetrathionate. Cyclic voltammetry experiments in acidic solutions indicate that the reaction of S4O
6
2-
with OH* goes through an unknown intermediate, tentatively assigned as S3O
4
n-
. An outer-sphere electron transfer mechanism for the reaction of S4O
6
2-
with OH* to form S3O
4
n-
is proposed based on experimental results. Oxidation rates for trithionate and tetrathionate in the presence of Fenton's
reagent (which forms hydroxyl radicals) are too fast to be directly measured using UV-Vis spectrophotometry, electrochemical,
or stop-flow spectrophotometry methods. Competitive reaction kinetics within the context of the Haber—Weiss mechanism suggests
that the rate constant for the oxidation of trithionate and tetrathionate with OH* is in excess of 108 M-1 sec-1. 相似文献
682.
K. Pecher D. McCubbery E. Kneedler J. Bargar L. Cox B. Tonner 《Geochimica et cosmochimica acta》2003,67(6):1089-1098
We have applied Scanning Transmission Soft X-ray Microscopy (STXM) to investigate the charge state distribution of Mn in two kinds of Mn-biominerals, Mn nodules collected from Lake Michigan sediments and Mn precipitates formed by spores of a marine bacillus SG-1 under transport limited reaction conditions. A data analysis technique was developed, which allows for extraction of spatially resolved 2-d charge state maps of manganese on a submicron level. We find that the charge state of Mn dominates the spectral shape of L-edge spectra of environmentally important single oxidation state Mn minerals and that spectra of mixed oxidation state oxides can be modelled by a combination of appropriate single oxidation state reference spectra. Two-dimensional maps of charge state distributions clearly reveal domains of different oxidation states within single particles of Mn-micronodules. Spots of preferred accumulation of Mn(II) were found, which indicates biogenic precipitation of Mn(II)-species as a first step of nodule formation. The presence of Mn(III) in the studied sediment samples suggests the involvement of one-electron oxidation processes and reaction conditions which inhibit or slow down the disproportionation of Mn(III)-products. Under transport limited conditions, Mn oxidation products formed by spores of the marine bacillus SG-1 can vary from cell to cell. The presence of significant amounts of Mn(III) containing species points to the involvement of one-electron oxidation reactions as in the case of the micro-nodules. Our technique and the results obtained form a new basis for the mechanistic understanding of the formation of Mn biominerals in the environment. 相似文献
683.
In the first known kinetic application of the technique, synchrotron 57Fe-Mössbauer spectroscopy was used to follow the rate of heterogeneous electron transfer between aqueous reagents and a solid phase containing Fe. The solid, a synthetic 57Fe-enriched Fe(III)-bearing pyroaurite-like phase having terephthalate (TA) in the interlayer [Mg3Fe(OH)8(TA)0.5 · 2H2O], was reduced by Na2S2O4 and then reoxidized by K2Cr2O7 by means of a novel flow-through cell. Synchrotron Mössbauer spectra were collected in the time domain at 30-s intervals. Integration of the intensity obtained during a selected time interval in the spectra allowed sensitive determination of Fe(II) content as a function of reaction time. Analysis of reaction end member specimens by both the synchrotron technique and conventional Mössbauer spectroscopy yielded comparable values for Mössbauer parameters such as center shift and Fe(II)/Fe(III) area ratios. Slight differences in quadrupole splitting values were observed, however. A reactive diffusion model was developed that fit the experimental Fe(II) kinetic data well and allowed the extraction of second-order rate constants for each reaction. Thus, in addition to rapidly collecting high quality Mössbauer data, the synchrotron technique seems well suited for aqueous rate experiments as a result of the penetrating power of 14.4 keV X-rays and high sensitivity to Fe valence state. 相似文献
684.
Geoid determination using adapted reference field, seismic Moho depths and variable density contrast 总被引:4,自引:0,他引:4
The traditional remove-restore technique for geoid computation suffers from two main drawbacks. The first is the assumption
of an isostatic hypothesis to compute the compensation masses. The second is the double consideration of the effect of the
topographic–isostatic masses within the data window through removing the reference field and the terrain reduction process.
To overcome the first disadvantage, the seismic Moho depths, representing, more or less, the actual compensating masses, have
been used with variable density anomalies computed by employing the topographic–isostatic mass balance principle. In order
to avoid the double consideration of the effect of the topographic–isostatic masses within the data window, the effect of
these masses for the used fixed data window, in terms of potential coefficients, has been subtracted from the reference field,
yielding an adapted reference field. This adapted reference field has been used for the remove–restore technique. The necessary
harmonic analysis of the topographic–isostatic potential using seismic Moho depths with variable density anomalies is given.
A wide comparison among geoids computed by the adapted reference field with both the Airy–Heiskanen isostatic model and seismic
Moho depths with variable density anomaly and a geoid computed by the traditional remove–restore technique is made. The results
show that using seismic Moho depths with variable density anomaly along with the adapted reference field gives the best relative
geoid accuracy compared to the GPS/levelling geoid.
Received: 3 October 2001 / Accepted: 20 September 2002
Correspondence to: H.A. Abd-Elmotaal 相似文献
685.
In the present study, an attempt has been made to delineate and characterize the different geomorphic units of Tundiya river
catchment in a part of Lower Maharahstra Metamorphic Plateau, north-eastern part of Nagpur district, Maharashtra. The drainage,
contour and delineated geological units have been overlaid on IRS-ID LISS III satellite imagery (bands 2,3 and 4) in EASI/PACE
analysis system to delineate and characterize different geomorphological units and analysis of their processes based on the
field observations. The study area is basically of metamorphic in origin with different geological formations and is influenced
by the various fluvio-morphological processes. Based on the satellite data analysis, the distinct geomorphological units viz.,
table top summits, structural hills, subdued plateau, linear ridges, shallow, moderate and deeply buried foot slopes, shallow
valley fills and deep valley fills have been delineated and characterized. The information generated from satellite data in
the form of vector layers has been used in GIS to generate geological and geomorphological maps of the study area. The present
study demonstrates that IRS-ID LISS-III data in conjunction with geology, drainage and contour parameters to enable detailed
evaluation of different geomorphological units and analysis of their processes based on the field observations. The delineated
geomorphological units can be utilized for evaluation and management of natural resources and geo-environment on sustainable
basis at river catchment level. 相似文献
686.
The paper discusses the land damage assessment and change detection analysis with reference to a mineral bearing zone in Manjhi,
Manuni and Churan valleys. The area is located in environmentally sensitive and fragile region of Himalaya and constitutes
of nearly 400 small-scale mines of slate, which were operative since last one hundred years and are stopped by court of law
since 1995 on account of environment deterioration. The status of land degradation has been studied using IRS-1B satellite
data of 1988,1992 and 1995. The geo-coded data on 1:50,000 scale has been interpreted and an increase in land degradation
status was noticed. Finally, the management strategy for arresting the further land damage in a broader perspective is suggested. 相似文献
687.
Xiaoli Guo Lars n Vladimir K. Makin Ann-Sofi Smedman 《Journal of Atmospheric & Ocean Science》2003,9(3):97-120
Measurements from the Baltic Sea and a wind-over-wave coupled model are used to study the wave impact on the sea drag. The study has been carried out for different wave conditions, namely a pure wind-sea, following-swell/ mixed sea and cross-swell/ mixed sea. Measurements reveal the fact that the sea drag is dependent on the sea-state. In stationary conditions and in the absence of severe cross-swell, swell reduces drag compared to wind-sea at the same wind speed. The cross-swell enhances the drag as compared to the following-swell case and the magnitude of the drag coefficient is increased with increasing the angle of swell propagation to the wind. It is shown that the agreement between the model results and measurements is good for pure wind-sea and stationary mixed-sea cases. Discrepancies occur at light winds, where most of the data represent pure swell conditions. During these pure swell conditions the data are characterized by a large variation of the drag coefficient. The variation is caused by mesoscale variability in the stress co-spectra, wind-cross-swell effects and nonstationarity in the wave and wind fields not represented in the model. 相似文献
688.
A. Chakraborty H. C. Upadhyaya O. P. Sharma S. K. Deb 《Meteorology and Atmospheric Physics》2003,83(3-4):221-236
Summary ?A newly developed ocean general circulation model has been tested and verified with some idealized experiments. Generally
two types of idealized experiments have been done here. First types are called as “symmetric experiments” and second types
are called as “transport experiments”. The first types of experiment help to correct the model core and any deficiency from
boundary conditions. The second types of experiment are the type of validation experiment. In both the experiments there are
no continents, so in the first type of experiments where symmetric forcings are provided one can expect that model should
maintain the symmetric nature. In the second type of experiments one can expect that model should respond correctly to the
wind forcings, if no wind curl is present in the wind forcing there will be no circulation in the extratropics and if there
is no wind the equator there will be no circulation. The model reproduces the possible envisaged results of these experiments
and gives the confidence for performing the realistic integration.
Received February 20, 2002; accepted July 7, 2002
Published online: February 20, 2003 相似文献
689.
A. Heusel-Waltrop K. Diehl S. K. Mitra H. R. Pruppacher 《Journal of Atmospheric Chemistry》2003,44(2):211-223
Laboratory experiments have been carried out to investigate the uptake of sulfur dioxide by water drops containing heavy metal ions where the metal ions serve as catalysts to oxidise the taken up S(IV) into S(VI). During the gas uptake the drops were freely suspended at their terminal velocity in the airstream of the Mainz vertical wind tunnel. Two series of experiments were carried out, one with large millimeter size water drops containing manganese or iron ions, and the other with small water drops containing manganese ions and having radii in hundreds of micron size range. The experimental results were compared against model computations using the Kronig–Brink model and the fully mixed model, modified for the case that heavy metal ions present in the liquid phase act as catalysts for the oxidising process. The results of the model calculations show that there are only small differences between the predicted gas uptake according to the two models. In addition it was found that the experimental obtained results from the uptake of SO2 by water drops containing heavy metal ions for both, large and small water drops did agree with the model results. 相似文献
690.