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1.
L. Prez del Villar J. Bruno R. Campos P. Gmez J. S. Czar A. Garraln B. Buil D. Arcos G. Carretero J. Ruiz Snchez-Porro P. Hernn 《Chemical Geology》2002,190(1-4):395-415
In the frame of the ENRESA natural analogue programme, the uranium ore from the “Mina Fe” (Salamanca, Spain) has been studied as a natural analogue of radioactive spent fuel behaviour. This uranium mine is hosted in highly fractured schistose rocks, a geological setting that has not been envisaged in the Spanish options for radioactive waste burial. However, some analogies with the processes that might be involved in the evolution of these geological repositories suggested this investigation.
The pitchblende–pyrite–carbonate paragenesis has been studied “in situ” as natural analogue of the nuclear spent fuel behaviour under extremely oxidative dissolution conditions. Similarly, secondary Fe oxyhydroxides and clay minerals have also been considered as relevant analogue materials for the retention of uranium and other analogous trace metals. A multidisciplinary characterisation of the site has been performed in order to study these processes.
Though the intense mining activities in the site hindered precise determination of the original hydrogeological and hydrochemical features of the investigated zone (Boa fault zone), the mineralogy and geochemistry of fracture fillings, mineralisation and associated clayey materials have allowed the geochemical evolution of the system to be established. Three geochemical zones have been clearly differentiated: (i) the oxidised zone, from the surface to approximately 20 m depth, (ii) the redox transition zone, from 20 to 50 m depth, and (iii) the reduced zone, located below the transition zone.
The oxidised zone is characterised by the presence of the typical mineral association resulting from the strong acid conditions caused by the total oxidation of pyrite and other sulphides. The total oxidation, dissolution and leaching of U(IV), as uranyl–sulphate aqueous complexes, prevailed in this oxidised zone. The redox transition zone is characterised by the coexistence of the primary uranium paragenesis, oxidised minerals, as well as numerous secondary solid phases as a result of the physico-chemical changes in the environment. The optimal physico-chemical conditions for the coffinitisation of pitchblende and the co-precipitation of Fe(III)–U(VI) took place in this zone. In the reduced zone, where the primary uranium paragenesis is present, we currently find the necessary physico-chemical conditions to stabilise pitchblende, pyrite and carbonates.
The physico-chemical conditions of the oxidised zone are not relevant to disposal conditions. In the transition zone, two main geochemical processes take place: (i) the coffinitisation of pitchblende, which may be an important process for the stability of spent fuel in reducing conditions, and (ii) the co-precipitation of the Fe(III) and U(VI) as oxyhydroxides, another relevant mechanism for the retention of uranium. The physico-chemical conditions that prevail below 50 m depth should be sufficient to stabilise a spent nuclear fuel repository, in the same way as they have been able to preserve the 34-Ma-old uranium deposit of the Mina Fe. 相似文献
2.
特征矿物是地质作用的直接记录,研究铀矿物伴生组合类型和特征为探讨铀矿床成因提供直接信息。本文以鄂尔多斯盆地东北部杭锦旗?纳岭沟地区含铀岩系中侏罗统直罗组为研究对象,通过岩心观察、显微观察、扫描电镜和电子探针分析等,系统研究了含铀砂岩中铀矿物种类、赋存特征及典型矿物伴生组合类型,在此基础上,结合铀成矿过程中流体作用探讨了铀成矿机理。取得的主要成果和认识如下:(1)研究区含矿目的层最主要的矿物类型为铀石,与铀矿物相关的矿物组合包括:莓球状黄铁矿?铀石、黑云母?它形黄铁矿?铀石、胶状黄铁矿?铀石、钛铁矿?锐钛矿?铀石、高岭石?铀石、蒙脱石/伊蒙混层?铀石、方解石?铀石、有机质?铀石和石英?铀石9种;(2)研究区成矿环境经历了成岩期的中性?弱碱性氧化环境→弱酸性氧化环境→成矿早期的弱酸性还原环境→成矿中?晚期的弱碱性还原环境→成矿期后的碱性还原环境的转变;(3)铀矿物的富集可以分为5个阶段:①早期预富集的碎屑铀;②石英颗粒边缘富集的沥青铀矿;③莓球状、它形、胶状黄铁矿、高岭石、钛铁矿边缘沉淀富集,与酸性还原流体有关的铀石;④与石英、方解石、蒙脱石/伊蒙混层等伴生,与碱性还原流体有关的铀石;⑤与莓球状黄铁矿、胶状黄铁矿、方解石伴生的受中低温热液改造的铀石。综上所述,研究区主成矿作用受酸性和碱性还原流体共同控制。 相似文献
3.
黄铁矿与沥青铀矿的共生条件及在沥青铀矿形成过程中所起作用的实验研究 总被引：5，自引：0，他引：5
高价铁与高价铀混合溶液在还原场中形成了共生的黄铁矿与沥青铀矿,该过程必须在弱酸性-中性-碱性介质中进行,其中在弱酸性至中性介质中易形成大的黄铁矿单晶。高价铀溶液流经黄铁矿矿区时,若在高温高压条件下,有新生的黄铁矿或白铁矿与沥青铀矿共生。黄铁矿还原六价铀形成沥青铀矿时,起还原作用的是二价硫。赤铁矿常与沥青铀矿共生,但它们是热液演化过程中不同阶段的产物,赤铁矿形成于体系氧逸度高的氧化环境,沥青铀矿形成于体系氧逸度低的还原环境,赤铁矿形成于沥青铀矿之前。 相似文献
4.
《Applied Geochemistry》2005,20(7):1268-1283
A geochemical model is developed for the immobilization of U in the presence of metallic Fe. Zero-valent iron (ZVI) serves as a reducing agent inducing the reductive-precipitation of U, and ZVI corrosion products can serve as absorbing agents for U. The numerical model developed allows the complex interactions of U in solution in differing concentrations to be examined, under variable pH and redox conditions, with or without carbonate, in the presence of ZVI of different size and surface area. It incorporates Fe corrosion, Fe(II) and Fe(III) corrosion product formation, reductive-precipitation of U from the soluble U(VI) valence to the poorly soluble U(IV) valence, adsorption/de-sorption of U onto the Fe oxide corrosion products, and aqueous speciation. The processes of Fe corrosion and reductive precipitation of U are simulated as non-equilibrium, an improvement over other geochemical models. The reductive-precipitation process may use either ZVI or Fe(II) as the reducing agent. The model is calibrated using 3 separate sets of experimental data from published literature that cover a wide range of redox conditions. Sensitivity of the model predictions to variations in input parameters is examined. The simulation results show that the different published experimental results can be explained by different solution chemistries in the studies, specifically O2 and CO2 availability and pH, and the amount and surface area of the metallic Fe. With this numerical model the behavior of U in ZVI containing systems over a range of conditions realistic for groundwater can be investigated. By synthesizing observations across several experimental studies, it will lead to a broader understanding of the processes controlling U immobilization under varied geochemical conditions. 相似文献
5.
The systematic sampling of the chemical composition of the groundwater from five karst springs (including an overflow spring) and one outflowing borehole have permitted to determine distinctive chemical changes in the waters that reflect the geochemical processes occurring in a carbonate aquifer system from southern Spain. The analysis of the dissolution parameters revealed that geochemical evolution of the karst waters basically depends on the availability of the minerals forming aquifer rocks and the residence time within the aquifers. In the three proposed scenarios in the aquifers, which include the preferential flow routines, the more important geochemical processes taking place during the groundwater flow from the recharge to the discharge zones are: CO2 dissolution and exsolution (outgassing), calcite net dissolution, calcite and dolomite sequential dissolution, gypsum/anhydrite and halite dissolution, de-dolomitization and calcite precipitation. A detailed analysis of the hydrochemical data set, saturation indices of the minerals and partial pressure of CO2 in the waters joined to the application of geochemical modelling methods allowed the elaboration of a hydrogeochemical model of the studied aquifers. The developed approach contributes to a better understanding of the karstification processes and the hydrogeological functioning of carbonate aquifers, the latter being a crucial aspect for the suitable management of the water resources. 相似文献
6.
Final disposal of high-level radioactive waste in deep repositories in clay formations is being considered by several countries. Repository safety assessment requires the use of numerical models of groundwater flow, solute transport and chemical processes. These models are being developed from data and knowledge gained from in situ experiments such as the CERBERUS experiment carried out at the HADES facility excavated in the Boom clay formation at Mol (Belgium). This long-term experiment is aimed at evaluating the effect of heating and radiation in Boom clay. The test was performed in a cased well drilled at 223 m depth and lasted from 1989 to 1994. A 60Co source of 400 TBq and two heaters were emplaced inside the well. Dose rate, temperature, porewater pressure and pH/Eh were measured in situ during the experiment and gas and porewater samples were taken for chemical analyses. Here a coupled thermo-hydro-geochemical (THC) model of the CERBERUS experiment is presented which accounts simultaneously for heating, radiation, solute diffusion and a suite of geochemical reactions including: aqueous complexation, acid–base, redox, mineral dissolution/precipitation, cation exchange and gas dissolution/ex-solution. Computed results indicate that heating and radiation causes a slight oxidation, a decrease in pH, slight changes in porewater chemistry and pyrite dissolution near the well. THC model results follow the general evolution of chemical data, but cannot fit SO4 data. Model discrepancies are partly overcome when microbially-mediated Fe and SO4 reduction are taken into account in a coupled thermo-hydro-bio-geochemical (THBC) model. This THBC model captures the trends of geochemical data, improves the fit to dissolved SO4 and predicts pyrite precipitation, a process observed near the CERBERUS well. The ability of the THBC numerical model to reproduce the overall trends of geochemical data of the CERBERUS experiment provides confidence in such a model as a suitable tool for the long-term prediction of geochemistry in the near field of a HLW repository in clay. However, the small number of available chemical data throughout the experiment and the lack of DOC and microbial data allow only a partial validation of the THBC model. 相似文献
7.
Effect of the addition of granitic powder to an acidic soil from Galicia (NW Spain) in comparison with lime 总被引：1，自引：1，他引：0
The impact of diffuse pollution, agricultural land use and climate change on the long-term response of subsurface–surface water quality is not well understood, but is a prerequisite for evaluation of water management options. The goal of this study is to model geochemical evolution of water chemistry from the infiltration through soil into the unsaturated zone, transport through bedrocks and granular aquifers to a river in order to identify zones of steep concentration gradients and high dynamics under transient flow conditions. A numerical model was constructed comprising a 2-D 1,500 m × 150 m vertical cross-section of typical sedimentary rock formations, a glacio-fluvial quaternary gravel aquifer in the valley and soil layers. The model coupled saturated/un-saturated flow and reactive transport under steady state and transient conditions. Geochemical interactions, include intra-aqueous kinetic reactions of oxygen with dissolved organic matter, as well as kinetics of carbonate dissolution/precipitation. This model section was chosen to provide insight in to the principal processes and time scales affecting water chemistry along different flow paths. The numerical simulator MIN3P was used, a finite volume program for variably saturated subsurface flow and multi-component reactive transport. The results show that subsurface water residence times range from approximately 2 to 2,000 years. Different zones are to be expected with respect to the development of mineral equilibria; namely, purely atmospherically influenced, as well as open and closed system carbonate dissolution. Short-term responses to daily averaged changes in precipitation, however, are only visible to some extent in the shallower and near-river parts of flow system and solute loads. This can most likely be explained by directional changes in flow paths, indicating that equilibrium geochemical condition predominate at the hillslope scale, i.e. water quality depends on transport pathways rather than on kinetic effects. The extent of reducing conditions is controlled by the presence of organic-rich layers (i.e. peat deposits), the dissolution kinetics of aquifer organic matter and the subsequent mixing with oxygenated water by hydrodynamic dispersion. 相似文献
8.
冷湖地区砂岩型铀矿是近年柴北缘新发现的具有工业价值的铀矿床,为了进一步研究该地区砂岩型铀成矿岩石学及矿物学特征、铀成矿条件等问题,本文在野外地质调查的基础上,利用偏光显微镜结合电子探针分析手段,对该区内大煤沟组中含矿岩石进行了系统研究。结果表明:研究区中侏罗统大煤沟组含矿岩石类型主要为(粉)砂质泥岩、薄层煤及细粒石英杂砂岩,整体发育一系列后生蚀变。研究区北东侧安南坝山古元古界达肯达坂群及赛什腾山海西期花岗岩为区内砂岩型铀成矿提供了丰富的铀源。砂岩型铀矿中铀主要以独立铀矿物沥青铀矿的形式赋存,其次含有少量分散吸附态铀,沥青铀矿总体呈不规则粒状、星点状、"串珠状、线状"及粉末状赋存于黄铁矿边缘、裂隙部位或黄铁矿与方解石的接触部位,吸附态铀主要赋存于炭屑及煤线内;区内沥青铀矿为柴北缘地区首次揭露并发现的独立铀矿物,总体上填补了柴北缘地区无独立铀矿物出露的空白。铀成矿条件方面,含矿目的层中方解石的发育,显示了铀成矿流体富含CO_2、H_2O等挥发分和矿化剂,其次出露的众多还原性介质(油气、炭屑及黄铁矿等)为区内砂岩型铀成矿提供了氧化还原反应必需的还原剂,最终将U~(6+)还原成U~(4+)以沥青铀矿等形式沉淀成矿。 相似文献
9.
Geochemical and mineralogical investigation of domestic archaeological soil features at the Tiel-Passewaaij site,The Netherlands 总被引：2，自引：0，他引：2
Archaeological soil features can be defined as areas of staining in ancient cultural soil horizons and are frequently used in surveys to locate sites and activity areas. Visual observation of these features, however, provides only limited information on their origin and the processes leading to their formation and this limits site interpretation. This paper presents the results of geochemical and mineralogical analyses of domestic archaeological soil features in order to assess their composition, formation pathway and origin. The greenish soil features studied here belong to a house plan from a Roman farmhouse located at the Tiel-Passewaaij site in the Netherlands. The soils were investigated using a range of techniques, including X-ray Fluorescence (XRF) spectroscopy, sequential soil extractions, Fourier-transformed infrared (FT-IR) spectroscopy, X-ray Diffraction (XRD) and microprobe analysis. The results indicate that the studied soil features can chemically be distinguished from off-site soils e.g. based on their phosphate and carbonate content. Mineralogical analysis of aggregate samples from soil features further reveal that quartz and feldspar minerals are coated with Ca–Fe–P phases that closely resemble anapaite and mitridatite mineral forms. The formation of these mineral phases probably resulted from periodic reductive dissolution of Fe-oxide phases and subsequent precipitation of Fe–P phases, with inclusion of Ca from anthropogenic carbonates or groundwater. The combined presence of (Ca)-carbonates, P-phases and some anthropogenic trace elements (Cu, Zn) suggests that the greenish soil features stem from manure inputs. 相似文献
10.
《International Geology Review》2012,54(10):930-944
At sites of groundwater contamination, predictions of contaminant behavior and evaluation of remedial strategies depend on identification and characterization of the geochemical processes affecting contaminant migration. Heavy-metal loadings to waters and sediments by leachate from the Golbasi waste disposal site in Ankara, Turkey, have been evaluated quantitatively using hydrogeochemical modeling. The groundwater of the waste disposal area, characterized by high concentrations of Ca, K, Cl, Cd, Pb, Zn, Cu, B, Ni, SO4, and NO3, contaminates the waters and sediments in the down-gradient area, Eymir Lake and a swamp along the flow path. An advective mass transport duration is ～15 years for unretarded contaminants to move from the waste disposal well area to the southern shoreline of Eymir Lake. Mixing calculations suggest that the down-gradient groundwater is formed by mixing of 40 to 72% upgradient groundwater and 28 to 60% waste-disposal-area groundwater, as well as Eymir Lake surface-water ion concentrations formed by mixing of down-gradient groundwater (3%-25%) and swamp-water ion concentrations (75-97%) along the flow path. An evaluation of the changes in concentration of trace ion-related precipitation/dissolution and exchange reactions between water and sediments for the formation of both Eymir Lake surface-water composition and the down-gradient groundwater composition indicate considerable trace-ion content of the clays (exchangers) and related reactions in the system. These results suggest that the amounts of contaminants removed from or added both to the down-gradient groundwater and to surface waters through mixing, dilution, and evaporation processes are rather small. The amounts of ions in the waters at the present stage of the contamination process are predominantly governed by exchange and dissolution/precipitation reactions. 相似文献
11.
氧化还原障在热液铀矿成矿中的作用 总被引：5，自引：0，他引：5
铀是变价元素,氧化还原条件控制铀的迁移和沉淀。铀在氧化环境中呈U~(6+)形式存在,在还原条件下则以U~(4+)形式存在。氧化态六价铀主要以可溶的碳酸铀酰/氟化铀酰络合物形式在水溶液中迁移,还原态四价铀主要以沥青铀矿和铀石等形式富集沉淀成矿。热液铀矿的形成需要一对空间上密切共生的氧化障/氧化剂和还原障/还原剂,二者缺一不可。首先,氧化障中氧化剂将富铀岩石中的铀大量氧化形成U~(6+),溶解进入水溶液迁移;第二,高氧化性富铀溶液遇到还原障,U~(6+)还原成U~(4+)沉淀下来,富集形成铀矿。前人虽然对铀的地球化学性质及氧化还原反应在铀成矿中作用已比较了解,但如何在实际铀矿成矿系统中准确识别氧化还原障,有效利用氧化还原障的控矿机理指导找矿,还存在一些模糊认识,制约了铀成矿理论的发展和找矿方法的提升。本文以我国最重要的砂岩型铀矿、火山岩型铀矿、花岗岩型铀矿和变质型铀矿为例,总结了与铀矿化有关的氧化还原障的主要类型,探讨了红层等蒸发盐地层(氧化障),有机质、煌斑岩等中基性岩脉(还原障)与铀矿之间的关系及控矿机制,揭示了成矿盆地中铀-煤、铀-气(油)共生的机制,阐明了翁泉沟硼、铁、铀矿共生原因,建立了不同类型铀矿成矿模型。 相似文献
12.
通过电子显微镜及电子探针分析,对鄂尔多斯盆地东南部店头地区砂岩型铀矿物的赋存状态、主要伴生元素及其沉淀机制进行了初步探讨。研究区主要的铀矿物类型为沥青质铀矿,以显微浸染状充填于砂岩孔隙及胶结物中;与U密切伴生的元素有Fe、Se、Pb、Si、Ti、Cr、S等,与铀矿物伴生的矿物组合有黄铁矿、方铅矿、钛铀矿以及与其关系密切的硒矿化;主要含铀层位富含有机质及黄铁矿,夹有透镜状、条带状煤线,具备丰富的还原物质,有利于铀元素的还原富集,因此认为影响研究区铀沉淀的主要地球化学障是还原障和吸附障。 相似文献
13.
从矿物粉晶表面反应性到矿物晶面反应性——以黄铁矿氧化行为的晶面差异性为例 总被引：1，自引：0，他引：1
地球系统中各种矿物相的物理化学反应大多是从矿物表面或界面开始的。要揭示矿物表面反应性的本质,就需要从控制其反应性的表面结构入手。由于实验条件的限制,绝大多数关于矿物表面物理化学性质的研究主要采用粉晶作为研究对象。尽管粉晶方法在研究诸如硅酸盐、碳酸盐溶解和沉淀结晶等过程中被普遍采用,但这种基于矿物粉晶的研究方法还是有一定的不足。因为形成粉晶的破碎研磨过程会导致晶体高能面的出现,高能面所具有的高活性可能会加速其反应过程,应用于地球化学反应的计算结果就可能高估了实际的地球化学反应速率。本研究以黄铁矿表面氧化反应的晶面差异性为例,从晶面结构制约反应性的角度出发,重新审视了黄铁矿氧化的相关问题,弥补了传统"粉晶研究"中对黄铁矿氧化速率和氧化机理认识的缺陷。黄铁矿宽范围的氧化速率实测值很可能是由不同晶面间较大的反应性差异导致;水在黄铁矿的氧化过程中同时扮演着传递电子的催化剂和反应物的角色,也是黄铁矿氧化反应速控步(rate-limiting step)的核心物质。这些认识首次明确了黄铁矿不同晶面反应性差异的重要性,并提示我们应将传统表面矿物学的研究推向更为精确的晶面矿物学水平。这一从晶面角度考察发生在矿物表面的地球化学反应的研究方法可为构建更为精确的地球化学模型提供理论基础。 相似文献
14.
Nikolay P. Laverov Vasily I. Velichkin Ai Fujiwara Naotatsu Shikazono Alexey P. Aleshin Enver E. Asadulin Vyacheslav N. Golubev Tatiana L. Krylova Alexander A. Pek Igor V. Chernyshev 《Resource Geology》2009,59(4):342-358
It has been shown that the main uranium ore mineral, pitchblende (uranium dioxide), is a natural analog of synthetic uraninite (also uranium dioxide), which constitutes 96% of spent nuclear fuel (SNF). Geochronological studies of the U‐Pb isotope systems in unaltered pitchblende from the orebodies reveal that these systems remained completely closed over the entire period (approximately 135 Ma) since the formation of the deposits. The bulk of the primary uranium ores within the Streltsovskoye ore field was influenced to various degrees by post‐ore hydrothermal solutions that led to pitchblende spherulites being replaced by pseudomorphs of an amorphous phase with a U‐Si composition; this phase also re‐precipitated in veinlets proximal to the pitchblende pseudomorphs. A technique specially developed by the authors was used to carry out quantitative counts of the abundance of uranium minerals by calculating the uranium mass balance in one of the orebodies subjected to hydrothermal alteration. The calculations reveal minimal uranium loss from the orebody. Uranium liberated in the process of the pseudomorphic replacement of pitchblende was immediately fixed, in situ, in the newly formed coffinite‐like amorphous U‐Si phase as a result of the development of an efficient geochemical barrier that prevented the long‐distance migration of uranium. In assessing the long‐term safety of underground SNF repositories, the results of the present study give us confidence that SNF uraninite, in terms of the preservation of its integrity as a mineral phase, provides for the reliable long‐term isolation of uranium, transuranium elements, and fission products that are “sealed” in the uraninite matrix. In the case of the mineral transformation of the uraninite matrix by hydrothermal solutions, the liberated uranium would be efficiently immobilized by the newly formed amorphous U‐Si phase. 相似文献
15.
It is essential that computer-based models used in the safety assessment of radioactive waste repositories accurately represent the processes occurring in real field systems. Confidence in long-term predictions of radionuclide migration will then depend upon the completeness of data available, particularly those obtained from the disposal site, and correct implementation of the model. The study of natural geochemical systems provides information on the adequacy of the underlying “generic” database and enhances our understanding of the transport mechanisms which form the basis of performance assessment. This paper concentrates on speciation-solubility modelling and describes four natural occurrences of uranium, each of which displays a different facet of uranium migration behaviour. The attributes of each site and the means by which uranium is immobilised are described. Retardation is highly species specific and this is illustrated through the use of site data in equilibrium speciation and coupled chemical transport calculations. Oxidation of U(IV) to U(VI) species promotes leaching of uranium ore at all the locations studied, emphasising the need to ensure that reducing conditions persist in a repository dominated by its actinide inventory. 相似文献
16.
Owing to the rapid increase in available data on the natural variations of the 238U/235U ratio, new isotopic geochemical mark of redox processes are beginning to emerge. In this connection, numerical estimates of the 238U and 235U fractionation factor (α(UIV?UVI)) accompanying the reduction UVI → UIV are needed. Such an estimate has been obtained for hydrothermal pitchblende formation based on results of high-precision (±0.06‰) measurements of the 238U/235U ratio in local microsamples of coarse spherulitic pitchblende from carbonate-pitchblende veins at the Oktyabr’sky deposit (Strel’tsovsky uranium ore field, eastern Transbaikal region). For this purpose, we used the formation temperature of hydrothermal pitchblende and a maximum estimate of the fractionation factor for 238U and 235U isotopes in the solution-solid phase system under normal (25°C) conditions (Murphy et al., 2014). The most probable isotopic fractionation factor accompanying pitchblende crystallization from hydrothermal solution at T = 320?250°C falls into the interval α(UIV?UVI) = 1.00020?1.00023. 相似文献
17.
西准噶尔白杨河铀矿床沥青铀矿矿物特征及形成环境 总被引：1，自引：0，他引：1
白杨河铀矿是我国新疆地区典型的铀-多金属矿床,为查明该矿原生铀矿物特征,进一步探究沥青铀矿的形成与保存环境,本文利用偏光显微镜、扫描电镜、电子探针等多种研究手段对该矿床中的沥青铀矿开展了矿物学研究工作,并利用激光拉曼和碳硫仪对与原生矿体空间关系极为密切的黑色断层泥开展了研究。结果表明,本矿床形成的原生沥青铀矿主要赋存在热液脉中,矿石组构包括:碎裂结构、花岗状压碎结构、斑状压碎结构、交代反应边结构;黑色断层泥含有一定量的有机碳(TOC为0.24%～1.07%),拉曼测试结果显示出较强烈的碳质峰。沥青铀矿不同程度地遭受流体改造作用,使得矿物化学成分极其复杂。随着流体改造程度的增加,UO_2、PbO呈现降低的趋势,Nb_2O_5及ZrO_2含量则表现出升高的趋势,显示在后期的流体改造作用过程中,铀被活化迁移的同时,流体还带来了丰富的Nb和Zr等元素。进一步分析认为富有机碳的断层泥在成矿过程中可能为U~(6+)的易溶络合物还原为沥青铀矿沉淀提供了有利条件,并且在沥青铀矿形成后起到了一定程度的保护作用。 相似文献
18.
《Applied Geochemistry》2004,19(6):917-936
Carbon dioxide disposal into deep aquifers is a potential means whereby atmospheric emissions of greenhouse gases may be reduced. However, our knowledge of the geohydrology, geochemistry, geophysics, and geomechanics of CO2 disposal must be refined if this technology is to be implemented safely, efficiently, and predictably. As a prelude to a fully coupled treatment of physical and chemical effects of CO2 injection, the authors have analyzed the impact of CO2 immobilization through carbonate mineral precipitation. Batch reaction modeling of the geochemical evolution of 3 different aquifer mineral compositions in the presence of CO2 at high pressure were performed. The modeling considered the following important factors affecting CO2 sequestration: (1) the kinetics of chemical interactions between the host rock minerals and the aqueous phase, (2) CO2 solubility dependence on pressure, temperature and salinity of the system, and (3) redox processes that could be important in deep subsurface environments. The geochemical evolution under CO2 injection conditions was evaluated. In addition, changes in porosity were monitored during the simulations. Results indicate that CO2 sequestration by matrix minerals varies considerably with rock type. Under favorable conditions the amount of CO2 that may be sequestered by precipitation of secondary carbonates is comparable with and can be larger than the effect of CO2 dissolution in pore waters. The precipitation of ankerite and siderite is sensitive to the rate of reduction of Fe(III) mineral precursors such as goethite or glauconite. The accumulation of carbonates in the rock matrix leads to a considerable decrease in porosity. This in turn adversely affects permeability and fluid flow in the aquifer. The numerical experiments described here provide useful insight into sequestration mechanisms, and their controlling geochemical conditions and parameters. 相似文献
19.
《Applied Geochemistry》2002,17(2):93-103
Mimicking geochemical processes to solve environmental problems was implemented in dealing with waste acidic jarosite and alkaline coal fly ash. By placing these two chemically different materials adjacent to one another, a self-sealing layer was formed at the interface between both wastes, isolating and immobilizing chemical constituents in the process. A series of leaching experiments were performed on each material separately to study the release behavior of the principal constituents. Radiotracer experiments were conducted to explore diffusion and reaction of constituents such as Fe3+ in a combined jarosite/fly ash system. A model has been developed to simulate the coupled processes of diffusion and precipitation taking into account porosity change due to pore filling by precipitates. The formation of a self-sealing isolation layer in a hypothetical jarosite/fly ash disposal site was modelled. Leaching results indicate that the release of elements from jarosite is much larger than that from fly ash, and that the highly pH dependent release of Fe, Al, and Zn was controlled by the solubility of their hydroxides. Leaching results also suggest that precipitation reactions can be expected to occur at the interface between jarosite and alkaline coal fly ash where a large pH gradient exists. Radiotracer experiments showed that accumulation of constituents occurred at the interface. Modeled Fe3+ profiles in layered jarosite/fly ash were well validated by experiments. Modeling results also showed that with the accumulation of constituents at the interface, a new layer with low porosity was formed. Application of this model suggests that there is a potential use to form a self-sealing layer in jarosite/fly ash co-disposal sites. 相似文献
20.
The assessment of the aluminosilicate buffering potential during acid weathering of the Estonian alum shale is provided.
It is found that the stoichiometric interaction between dissolved pyrite oxidation products and illite of the shale best describe
the buffering process and are consistent with earlier field studies. The scheme includes incongruent dissolution of illite
with smectite and K-jarosite precipitating. This complex mechanism involves buffering of 8% of the acidity by K+ and temporary precipitation of 25% of the acidity as K-jarosite. Dissolution proceeds at a low pH (1.5–3) until all pyrite
in the shale particle is oxidised. Hence, if the total amount of illite present is larger than needed for stoichiometric interactions,
only part of it is involved in a buffering process, neutralising a certain percentage of acidity. The next stage in shale
weathering is the incongruent dissolution of K-jarosite with the release of the precipitated acidity and the formation of
ferric oxyhydroxide.
Received: 3 August 1998 · Revised paper: 26 January 1999 · Accepted: 23 February 1999 相似文献