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1.
M.P. Collings J.W. Dever H.J. Fraser M.R.S. McCoustra 《Astrophysics and Space Science》2003,285(3-4):633-659
The interaction of carbon monoxide (CO) with vapour-deposited water(H2O) ices has been studied using temperature programmed desorption (TPD) and Fourier transform reflection-absorption infrared
spectroscopy (FT-RAIRS) over a range of astrophysically relevant temperatures. Such measurements have shown that CO desorption
from amorphous H2Oices is a much more complex process than current astrochemical models suggest. Re-visiting previously reported laboratory
experiments (Collings et al., 2003), a rate model has been constructed to explain, in a phenomenological manner, the desorption
of CO over astronomically relevant time scales. The model presented here can be widely applied to a range of astronomical
environments where depletion of CO from the gas phase is relevant. The model accounts for the two competing processes of CO
desorption and migration, and also enables the entrapment of some of the CO in the ice matrix and its subsequent release as
the water ice crystallises and then desorbs. The astronomical implications of this model are discussed.
This revised version was published online in July 2006 with corrections to the Cover Date. 相似文献
2.
David M. Sherman Caroline L. Peacock Christopher G. Hubbard 《Geochimica et cosmochimica acta》2008,72(2):298-310
Sorption of U(VI) to goethite is a fundamental control on the mobility of uranium in soil and groundwater. Here, we investigated the sorption of U on goethite using EXAFS spectroscopy, batch sorption experiments and DFT calculations of the energetics and structures of possible surface complexes. Based on EXAFS spectra, it has previously been proposed that U(VI), as the uranyl cation , sorbs to Fe oxide hydroxide phases by forming a bidentate edge-sharing (E2) surface complex, >Fe(OH)2UO2(H2O)n. Here, we argue that this complex alone cannot account for the sorption capacity of goethite (α-FeOOH). Moreover, we show that all of the EXAFS signal attributed to the E2 complex can be accounted for by multiple scattering. We propose that the dominant surface complex in CO2-free systems is a bidentate corner-sharing (C2) complex, (>FeOH)2UO2(H2O)3 which can form on the dominant {101} surface. However, in the presence of CO2, we find an enhancement of UO2 sorption at low pH and attribute this to a (>FeO)CO2UO2 ternary complex. With increasing pH, U(VI) desorbs by the formation of aqueous carbonate and hydroxyl complexes. However, this desorption is preceded by the formation of a second ternary surface complex (>FeOH)2UO2CO3. The three proposed surface complexes, (>FeOH)2UO2(H2O)3, >FeOCO2UO2, and (>FeOH)2UO2CO3 are consistent with EXAFS spectra. Using these complexes, we developed a surface complexation model for U on goethite with a 1-pK model for surface protonation, an extended Stern model for surface electrostatics and inclusion of all known UO2-OH-CO3 aqueous complexes in the current thermodynamic database. The model gives an excellent fit to our sorption experiments done in both ambient and reduced CO2 environments at surface loadings of 0.02-2.0 wt% U. 相似文献
3.
Martin R. Lee Mark E. Hodson Maureen MacKenzie Caroline L. Smith 《Geochimica et cosmochimica acta》2008,72(20):4962-4975
Our ability to identify thin non-stoichiometric and amorphous layers beneath mineral surfaces has been tested by undertaking X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM) work on alkali feldspars from pH 1 dissolution experiments. The outcomes of this work were used to help interpret XPS and TEM results from alkali feldspars weathered for <10,000 years in soils overlying the Shap Granite (north-west England). The chemistry of effluent solutions indicates that silica-rich layers a few nanometers in thickness formed during the pH 1 experiments. These layers can be successfully identified by XPS and have lower Al/Si, Na/Si, K/Si and Ca/Si values than the outermost ∼9 nm of unweathered controls. Development of Al-Si non-stoichiometry is coupled with loss of crystal structure to produce amorphous layers that are identifiable by TEM where >∼2.5 nm thick, whereas the crystallinity of albite is retained despite leaching of Na to depths of tens to hundreds on nanometers. Integration of XPS data over the outermost 6-9 nm of naturally weathered Shap feldspars shows that they have stoichiometric Al/Si and K/Si ratios, which is consistent with findings of previous TEM work on the same material that they lack amorphous layers. There is some XPS evidence for loss of K from the outermost couple of nanometers of Shap orthoclase, and the possibility of leaching of Na from albite to greater depths cannot be excluded using the XPS or TEM results. This study demonstrates that the leached layer model, as formulated from laboratory experiments, is inapplicable to the weathering of alkali feldspars within acidic soils, which is an essentially stoichiometric reaction. 相似文献
4.
Jos M. Marques Paula M. Carreira Maria Rosrio Carvalho Maria J. Matias Fraser E. Goff Maria J. Basto Rui C. Graa Luís Aires-Barros Luís Rocha 《Applied Geochemistry》2008,23(12):3278-3289
This paper reviews the geochemical, isotopic (2H, 18O, 13C, 3H and 14C) and numerical modelling approaches to evaluate possible geological sources of the high pH (11.5)/Na–Cl/Ca–OH mineral waters from the Cabeço de Vide region (Central-Portugal). Water–rock interaction studies have greatly contributed to a conceptual hydrogeological circulation model of the Cabeço de Vide mineral waters, which was corroborated by numerical modelling approaches. The local shallow groundwaters belong to the Mg–HCO3 type, and are derived by interaction with the local serpentinized rocks. At depth, these type waters evolve into the high pH/Na–Cl/Ca–OH mineral waters of Cabeço de Vide spas, issuing from the intrusive contact between mafic/ultramafic rocks and an older carbonate sequence. The Cabeço de Vide mineral waters are supersaturated with respect to serpentine indicating that they may cause serpentinization. Magnesium silicate phases (brucite and serpentine) seem to control Mg concentrations in Cabeço de Vide mineral waters. Similar δ2H and δ18O suggest a common meteoric origin and that the Mg–HCO3 type waters have evolved towards Cabeço de Vide mineral waters. The reaction path simulations show that the progressive evolution of the Ca–HCO3 to Mg–HCO3 waters can be attributed to the interaction of meteoric waters with serpentinites. The sequential dissolution at CO2 (g) closed system conditions leads to the precipitation of calcite, magnesite, amorphous silica, chrysotile and brucite, indicating that the waters would be responsible for the serpentinization of fresh ultramafic rocks (dunites) present at depth. The apparent age of Cabeço de Vide mineral waters was determined as 2790 ± 40 a BP, on the basis of 14C and 13C values, which is in agreement with the 3H concentrations being below the detection limit. 相似文献
5.
Geologic relations indicate that silica phases transformed in the Monterey Formation in two zones that persist over a narrow
depth/temperature range and do not stratigraphically overlap. The wide and overlapping range of reported temperatures of these
transformations is mainly a result of the many uncertainties inherent in the different methods used to estimate temperature
and does not indicate that phases transform throughout these ranges. Our approach to a reliable temperature scale for silica
diagenesis combines as empirical zonation of silica phases with temperature calibration from a sequence at maximum temperature
and depth of burial. 相似文献
6.
The Global Programme of Action for the Protection of the Marine Environment from Land-based Activities (GPA) represents an ambitious attempt to make the leap between the rhetoric of protecting and preserving the marine environment and action. With degradation of the marine environment from land based activities posing one of the most serious threats to the quality and productivity of the coastal and marine environment, the GPA can only be viewed as a milestone rather than a destination, as so much work remains to be done in this field.States supporting the GPA are entering the most challenging phase of the program, that of implementation. But the international community in taking on this challenge is not without a few signposts. The failure of the Montreal Guidelines to be implemented, provides States with many important lessons. This paper suggests that if the GPA is to have an impact on the complex problem of land-based activities then several tasks need to be grappled with. Substantial financial support needs to be generated, a proactive and cooperative secretariat established and the nexus between the GPA and United Nations Environment Programme Regional Seas Programme examined. The importance of people and training to the capacity building process needs to be recognised and a wider variety of stakeholders engaged in the follow up phase. Pivotal to the aforementioned is the need to generate political will to address the problem, without which the GPA will become yet another dusty volume on the bookshelf. 相似文献
7.
Caroline M. Isaacs 《Geo-Marine Letters》1985,5(1):25-30
Although best known as a deposit rich in silica and organic matter, the Miocene Monterey Formation actually had long-term
rates of silica and organic Matter accumulation equal to or lower than values in the underlying and overlying detritus-rich
formations in the Santa Barbara coastal area. The factor Mainly influencing the composition of the Monterey Formation in this
area was the slow accumulation of terrigenous debris. In contrast, with greater than average silica abundance within the Monterey
Formation probably resulted from rapid short-term silica accumulation (of hundreds to tens of thousands years duration) rather
than from especially slow accumulation of diluting debris. 相似文献
8.
Mark A. Engle Fraser Goff David G. Jewett Gregory J. Reller Joel B. Bauman 《Hydrogeology Journal》2008,16(3):559-573
Boron, chloride, sulfate, δD, δ18O, and 3H concentrations in surface water and groundwater samples from the Sulphur Bank Mercury Mine (SBMM), California, USA were
used to examine geochemical processes and provide constraints on evaporation and groundwater flow. SBMM is an abandoned sulfur
and mercury mine with an underlying hydrothermal system, adjacent to Clear Lake, California. Results for non-3H tracers (i.e., boron, chloride, sulfate, δD, and δ18O) identify contributions from six water types at SBMM. Processes including evaporation, mixing, hydrothermal water input
and possible isotopic exchange with hydrothermal gases are also discerned. Tritium data indicate that hydrothermal waters
and other deep groundwaters are likely pre-bomb (before ~1952) in age while most other waters were recharged after ~1990.
A boron-based steady-state reservoir model of the Herman Impoundment pit lake indicates that 71–79% of its input is from meteoric
water with the remainder from hydrothermal contributions. Results for groundwater samples from six shallow wells over a 6–month
period for δD and δ18O suggests that water from Herman Impoundment is diluted another 3% to more than 40% by infiltrating meteoric water, as it
leaves the site. Results for this investigation show that environmental tracers are an effective tool to understand the SBMM
hydrogeologic regime.
Electronic supplementary material The online version of this article (doi:) contains supplementary material, which is available to authorized users.
Electronic supplementary material The online version of this article (doi:) contains supplementary material, which is available to authorized users.
Résumé Les concentrations en bore, chlorure, sulfate, δD, δ18O, et 3H d’échantillons d’eaux de surface et souterraine prélevés dans le banc de soufre de la mine de mercure (SBMM en anglais) en Californie, USA, ont été utilisées pour étudier les processus géochimiques et pour fournir des contraintes à l’évaporation et à l’écoulement des eaux souterraines. La SBMM est une mine de soufre et de mercure abandonnée, adjacente au lac Clear en Californie et sous laquelle se trouve un système hydrothermal.Les résultats des traceurs autres que le tritium (bore, chlorure, sulfate, δD, et δ18O) ont permis d’identifier des contributions de six types d’eaux à SBMM. Des processus tels que l’évaporation, le mélange, l’entrée d’eau hydrothermale et de possibles échanges isotopiques avec des gaz hydrothermaux ont également été identifiés. Les données de tritium montrent que les eaux hydrothermales et d’autres eaux profondes sont probablement d’age antérieure à la bombe (avant ~1952), alors que la plupart des autres eaux sont issues de la recharge après ~1990. Un modèle de réservoir représentant le lac situé dans la partie Herman Impoundment de l’ancienne mine, en régime permanent et basé sur le bore, montre que 71–79% de l’eau provient des précipitations, le reste provenant de contributions hydrothermales. Les résultats de δD et δ18O pour des échantillons d’eau souterraine de six puits peu profonds sur une période de 6 mois suggèrent que l’eau de Hermann Impoundment est encore diluée entre 3% jusqu’à plus de 40% lorsqu’elle quitte le site du fait de l’infiltration d’eau météorique. Les résultats de cette étude montrent que les traceurs environnementaux constituent un outil efficace pour comprendre le régime hydrogéologique de la SBMM.
Resumen Se han utilizado datos de concentraciones de boro, cloruros, sulfatos, δD, δ18O, y 3H en muestras de aguas superficiales y subterráneas procedentes de la Mina de Mercurio Sulphur Bank (SBMM), California, USA, para estudiar los procesos geoquímicos y caracterizar la evaporación y el flujo del agua subterránea. SBMM es una mina abandonada de azufre y mercurio con un sistema hidrotermal subyacente, cercano al Lago Clear, California.Los resultados de los trazadores que no son 3H (por ejemplo, boro, cloruros, sulfatos δD, y δ18O) identifican las contribuciones de seis tipos de agua en la SBMM. Se han identificado diversos procesos, como evaporación, mezcla, entrada de agua hidrotermal y la posibilidad de intercambios isotópicos con gases hidrotermales. Los datos de tritio indican que las aguas hidrotermales y otras aguas subterráneas profundas son probablemente pre-bombas (previas a ~1952) en edad mientras que la mayoría de las otras aguas se han recargado después de ~1990. Un modelo estacionario basado en el boro de la fosa del lago Herman Impoundment indica que el 71–79% de su entrada procede de agua meteórica con restos de contribución hidrotermal. Los resultados para las muestras de aguas subterráneas procedentes de seis pozos superficiales en un periodo de 6 meses para δD y δ18O sugieren que el agua procedente de Herman Impoundment se diluye en otro 3% hasta más del 40% debido a la infiltración de agua meteórica., que sale del sitio. Los resultados de esta investigación muestran que los trazadores ambientales son una herramienta efectiva para entender el régimen hidrogeológico de la SBMM.相似文献
9.
Fragmentation, or the "coming apart" of magma during a plinian eruption, remains one of the least understood processes in
volcanology, although assumptions about the timing and mechanisms of fragmentation are key parameters in all existing eruption
models. Despite evidence to the contrary, most models assume that fragmentation occurs at a critical vesicularity (volume
percent vesicles) of 75–83%. We propose instead that the degree to which magma is fragmented is determined by factors controlling
bubble coalescence: magma viscosity, temperature, bubble size distribution, bubble shapes, and time. Bubble coalescence in
vesiculating magmas creates permeability which serves to connect the dispersed gas phase. When sufficiently developed, permeability
allows subsequent exsolved and expanded gas to escape, thus preserving a sufficiently interconnected region of vesicular magma
as a pumice clast, rather than fully fragmenting it to ash. For this reason pumice is likely to preserve information about
(a) how permeability develops and (b) the critical permeability needed to insure clast preservation. We present measurements
and calculations that constrain the conditions (vesicularity, bubble size distribution, time, pressure difference, viscosity)
necessary for adequate permeability to develop. We suggest that magma fragments explosively to ash when and where, in a heterogeneously
vesiculating magma, these conditions are not met. Both the development of permeability by bubble wall thinning and rupture
and the loss of gas through a permeable network of bubbles require time, consistent with the observation that degree of fragmentation
(i.e., amount of ash) increases with increasing eruption rate.
Received: 5 July 1995 / Accepted: 27 December 1995 相似文献
10.
Ruminations of a Dyspeptic Ex-Editor* 总被引:1,自引:0,他引:1
John Fraser Hart 《The Professional geographer》1976,28(3):225-232