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1.
Past mining, processing, and waste disposal activities have left a legacy of uranium-contaminated soil and groundwater. Phosphate addition to subsurface environments can potentially immobilize U(VI) in-situ through interactions with uranium at mineral-water interfaces. Phosphate can induce the precipitation of low solubility U(VI)-phosphates, and it may enhance or inhibit U(VI) adsorption to iron(III) (oxy)hydroxide surfaces. Such surfaces may also facilitate the heterogeneous nucleation of U(VI)-phosphate precipitates. The interactions among phosphate, U(VI), and goethite (α-FeOOH) were investigated in a year-long series of experiments at pH 4. Reaction time, total U(VI), total phosphate, and the presence and absence of goethite were systematically varied to determine their effects on the extent of U(VI) uptake and the dominant uranium immobilization mechanism. Dissolved U(VI) and phosphate concentrations were interpreted within a reaction-based modeling framework that included dissolution-precipitation reactions and a surface complexation model to account for adsorption. The best available thermodynamic data and past surface complexation models were integrated to form an internally consistent framework. Additional evidence for the uptake mechanisms was obtained using scanning electron microscopy and X-ray diffraction. The formation and crystal growth of a U(VI)-phosphate phase, most likely chernikovite, UO2HPO4·4H2O(s), occurred rapidly for initially supersaturated suspensions both with and without goethite. Nucleation appears to occur homogeneously for almost all conditions, even in the presence of goethite, but heterogeneous nucleation was likely at one condition. The U(VI)-phosphate solids exhibited metastability depending on the TOTU:TOTP ratio. At the highest phosphate concentration studied (130 μM), U(VI) uptake was enhanced due to the likely formation of a ternary surface complex for low (∼1 μM) to intermediate (∼10 μM) TOTU concentrations and to U(VI)-phosphate precipitation for high TOTU (∼100 μM) concentrations. For conditions favoring precipitation, the goethite surface acted as a sink for dissolved phosphate that resulted in higher dissolved U(VI) concentrations relative to goethite-free conditions. Based on the total uranium and available sorption sites, a critical phosphate concentration between 15 μM and 130 μM was required for preferential precipitation of uranium phosphate over U(VI) adsorption.  相似文献   

2.
Pyrite dissolution and interaction with Fe(II), Co(II), Eu(III) and U(VI) have been studied under anoxic conditions by solution chemistry and spectroscopic techniques. Aqueous data show a maximal cation uptake above pH 5.5. Iron (II) uptake can explain the non-stoichiometric [S]aq/[Fe]aq ratios often observed during dissolution experiments. Protonation data corrected for pyrite dissolution resulted in a proton site density of 9 ± 3 sites nm−2. Concentration isotherms for Eu(III) and U(VI) sorption on pyrite indicate two different behaviours which can be related to the contrasted redox properties of these elements. For Eu(III), sorption can be explained by the existence of a unique site with a saturation concentration of 1.25 × 10−6 mol g−1. In the U(VI) case, sorption seems to occur on two different sites with a total saturation concentration of 4.5 × 10−8 mol g−1. At lower concentration, uranium reduction occurs, limiting the concentration of dissolved uranium to the solubility of UO2(s).Scanning electron microscopy and micro-Raman spectrometry of U(VI)-sorbed pyrite indicate a heterogeneous distribution of U at the pyrite surface and a close association with oxidized S. X-ray photoelectron spectroscopy confirms the partial reduction of U and the formation of a hyperstoichiometric UO2+x(s). Our results are consistent with a chemistry of the pyrite surface governed not by Fe(II)-bound hydroxyl groups, but by S groups which can either sorb cations and protons, or sorb and reduce redox-sensitive elements such as U(VI).  相似文献   

3.
The rate of chemical weathering of rocks has been determined by using uranium as a natural isotopic tracer. The concentration of uranium and 234U/238U ratio in natural waters, rocks, and soils of the Preto river basin (Bahia State, Brazil) was measured by alpha-ray spectroscopy.The activity ratio U234/U238 measured in the various samples indicates the uranium fraction which is dissolved from rocks during the weathering process. The results obtained show that 1 m of rock needs 25,000 yr to be weathered in this region under present climatic conditions.  相似文献   

4.
Sedimentary units deposited during the post-rift stage of the Erlian Basin located in northeast China present an alternation of sandstone and mudstone layers. This sedimentological architecture is at the origin of confined permeable reservoirs hosting sandstone-type uranium deposits. The study of the Nuheting deposit offered the opportunity to identify synsedimentary/early diagenetic uranium concentrations and diagenetic mineralization hosted in mudstone-dominated layers of the Erlian Formation, indicating that a stock of uranium was present in the basin prior to the genesis of sandstone-hosted uranium deposits. Therefore, this pre-existing stock may constitute a significant source of uranium for the formation of roll front deposits present in other parts of the Erlian Basin.Detailed petrographic and geochemical study of drill-core samples from the Nuheting deposit led to the characterization of different stages related to the formation of the uranium ore bodies and allowed to propose a new metallogenic model. Uranium mineralization of the Nuheting deposit is mainly hosted in dark gray silty mudstone of wetland depositional environment of the Late Cretaceous Erlian Formation. Petrographic observations and EMP analyses evidenced that a significant amount of uranium was associated with clay minerals (interstratified clays, smectite, chlorite, palygorskyte, illite and kaolinite), either adsorbed on mineral surfaces as U (VI) ions or reduced mainly as UO2 nano to microcrystals disseminated in the clayey matrix, which corresponds to synsedimentary/early diagenetic concentrations. Trace elements on pyrite analyzed by LA-ICPMS, petrographic observations and whole-rock geochemical data led to the characterization of a diagenetic uranium mineralization. High As (1–50 ppm), Mo (10–500 ppm) and Se concentrations in the whole rock and the incorporation of these elements in pyrite highlight reducing conditions within the host-rocks during the diagenesis of the Erlian Formation. During the early diagenetic stage, uranium was either desorbed from clay minerals and organic materials to be reduced or directly reduced and precipitated as P-rich coffinite and pitchblende on pyrite crystals. During the late diagenetic stage, uranium was redistributed in situ and locally deposited mainly as coffinite on pyrites. Finally, an epigenetic stage of cementation was identified with sulfate and carbonate minerals, which may enclose some uranium minerals. This epigenetic stage of fluid circulation may be responsible for a minor uranium remobilization. Therefore, the Nuheting deposit experienced three main stages: (i) a synsedimentary/early diagenetic uranium concentration and mineralization, (ii) a late diagenetic in situ uranium remobilization and deposition on pyrite and (iii) an epigenetic cementation. Rock-Eval pyrolysis indicates that the organic matter contained in host-rocks of the Nuheting deposit is of type IV, inherited from land plant, and do not contain free hydrocarbons (very low S1). Therefore, our results do not support that migrated hydrocarbons were involved as a reducing agent for uranium mineralization.  相似文献   

5.
龙虎泡铀矿化区的发现是近年来根据油田资料二次开发和钻探验证而取得的重要创新成果之一,矿化区位于松辽盆地北部龙虎泡-大安阶地北,西与泰康隆起区和西部超覆区相邻。本文在详实的野外工作基础之上,利用偏光显微镜、电子显微镜、能谱、背散射、点化学分析及元素面扫描分析等手段,对龙虎泡地区含铀砂岩中以钛铁矿及其相关蚀变矿物为代表的铁钛氧化物与砂岩型铀矿化之间的关系进行了研究探讨,结果表明:①以富铀-铁钛氧化物-钛氧化物-黄铁矿为代表的蚀变矿物共生组合记录和保留了有关砂岩型铀矿成矿流体和成矿环境的重要信息,含矿砂岩中钛铁矿及其蚀变相关的富铀-铁钛氧化物、钛氧化物、黄铁矿等矿物的不同产出类型和不同蚀变矿物共生组合关系对比分析指示,龙虎泡地区铀成矿受到了后期含铀富铁的氧化性流体与富H_2S的还原性流体混合作用影响,成矿环境偏强还原;②与铀矿化关系最为密切的铁钛氧化物是蚀变程度高且富镁的钛铁矿,富铀-铁钛氧化物即是这些强蚀变钛铁矿与后期成矿流体发生氧化还原作用形成的,钛铁矿内部溶蚀裂隙为含矿流体的蚀变和铀的沉淀富集提供了良好的容矿空间,蚀变钛铁矿和黄铁矿为铀的沉淀富集分别提供了良好的矿物尺度上的氧化障和还原障,在含矿流体与富H_2S还原性流体混合过程中,铀得以在蚀变钛铁矿与黄铁矿的氧化还原界面附近沉淀富集。  相似文献   

6.
It has generally been assumed that the bioreduction of hexavalent uranium in groundwater systems will result in the precipitation of immobile uraninite (UO2). In order to explore the form and stability of uranium immobilized under these conditions, we introduced lactate (15 mM for 3 months) into flow-through columns containing sediments derived from a former uranium-processing site at Old Rifle, CO. This resulted in metal-reducing conditions as evidenced by concurrent uranium uptake and iron release. Despite initial augmentation with Shewanella oneidensis, bacteria belonging to the phylum Firmicutes dominated the biostimulated columns. The immobilization of uranium (∼1 mmol U per kg sediment) enabled analysis by X-ray absorption spectroscopy (XAS). Tetravalent uranium associated with these sediments did not have spectroscopic signatures representative of U-U shells or crystalline UO2. Analysis by microfocused XAS revealed concentrated micrometer regions of solid U(IV) that had spectroscopic signatures consistent with bulk analyses and a poor proximal correlation (μm scale resolution) between U and Fe. A plausible explanation, supported by biogeochemical conditions and spectral interpretations, is uranium association with phosphoryl moieties found in biomass; hence implicating direct enzymatic uranium reduction. After the immobilization phase, two months of in situ exposure to oxic influent did not result in substantial uranium remobilization. Ex situ flow-through experiments demonstrated more rapid uranium mobilization than observed in column oxidation studies and indicated that sediment-associated U(IV) is more mobile than biogenic UO2. This work suggests that in situ uranium bioimmobilization studies and subsurface modeling parameters should be expanded to account for non-uraninite U(IV) species associated with biomass.  相似文献   

7.
《Applied Geochemistry》2000,15(8):1219-1244
Arsenian pyrite, formed during Cretaceous gold mineralization, is the primary source of As along the Melones fault zone in the southern Mother Lode Gold District of California. Mine tailings and associated weathering products from partially submerged inactive gold mines at Don Pedro Reservoir, on the Tuolumne River, contain ∼20–1300 ppm As. The highest concentrations are in weathering crusts from the Clio mine and nearby outcrops which contain goethite or jarosite. As is concentrated up to 2150 ppm in the fine-grained (<63 μm) fraction of these Fe-rich weathering products.Individual pyrite grains in albite-chlorite schists of the Clio mine tailings contain an average of 1.2 wt.% As. Pyrite grains are coarsely zoned, with local As concentrations ranging from ∼0 to 5 wt.%. Electron microprobe, transmission electron microscope, and extended X-ray absorption fine-structure spectroscopy (EXAFS) analyses indicate that As substitutes for S in pyrite and is not present as inclusions of arsenopyrite or other As-bearing phases. Comparison with simulated EXAFS spectra demonstrates that As atoms are locally clustered in the pyrite lattice and that the unit cell of arsenian pyrite is expanded by ∼2.6% relative to pure pyrite. During weathering, clustered substitution of As into pyrite may be responsible for accelerating oxidation, hydrolysis, and dissolution of arsenian pyrite relative to pure pyrite in weathered tailings. Arsenic K-edge EXAFS analysis of the fine-grained Fe-rich weathering products are consistent with corner-sharing between As(V) tetrahedra and Fe(III)-octahedra. Determinations of nearest-neighbor distances and atomic identities, generated from least-squares fitting algorithms to spectral data, indicate that arsenate tetrahedra are sorbed on goethite mineral surfaces but substitute for SO4 in jarosite. Erosional transport of As-bearing goethite and jarosite to Don Pedro Reservoir increases the potential for As mobility and bioavailability by desorption or dissolution. Both the substrate minerals and dissolved As species are expected to respond to seasonal changes in lake chemistry caused by thermal stratification and turnover within the monomictic Don Pedro Reservoir. Arsenic is predicted to be most bioavailable and toxic in the reservoir’s summer hypolimnion.  相似文献   

8.
We determined the association of uranium in yeast cells S. cerevisiae grown in medium containing high (1 g · L-1) or low (0.2 g · L-1) concentrations of phosphate after exposure for 96 h to a 4 × 10-4 mol · L-1 U(VI) solution at pH 3.2 or 4.7. The analysis was made using a field emission scanning electron microscope equipped with energy dispersive spectroscopy (FESEM-EDS), transmission electron microscopy (TEM), and visible diffuse reflectance spectrometry. Cells grown in the high-phosphate medium rapidly accumulated U(VI) from solution at pH 3.2 over the first 24 h, followed by a slow uptake until 96 h, whereas in cells grown in low-phosphate medium, U(VI) accumulation reached a steady state within 24 h. FESEM-EDS analyses revealed the formation of a U(VI)-bearing precipitate on the yeast cells grown in high-phosphate medium after only 48 h exposure; no precipitate was detected on cells grown in low-phosphate medium up to 96 h. These results suggest that sorption onto the cell surfaces was the dominant process initially. Analysis of the U(VI)-bearing precipitates by all three methods demonstrated the presence of H-autunite, HUO2PO4 · 4H2O. Thermodynamic calculations suggest that the chemical compositions of the solutions containing yeast grown in high-phosphate medium were undersaturated with respect to H-autunite, but were supersaturated with ten times more U(VI) and P than were actually observed. Apparently, the sorbed U(VI) on the cell surfaces reacts with P released from the yeast to form H-autunite by local saturation. The U(VI) uptake by yeast cells grown in high phosphate medium at pH 4.7, along with the thermodynamic calculation, indicated that more H-autunite is precipitated in neutral pH solution than in acid solution. Thus, U(VI)-phosphate mineralization on the cells of microorganisms should be taken into account for predicting U(VI) mobility in the environment.  相似文献   

9.
竹山下铀矿床是粤北下庄铀矿田内大型铀矿床之一,铀矿化类型为"交点"型和硅化带型。在详细的野外地质调查基础上,对竹山下铀矿床4种不同类型黄铁矿进行元素含量分析及硫同位素测试,结果表明:"交点"型矿石中黄铁矿相对富集Pb、 Cu、 Co、 As、 Ni、 Se、 Bi、 U、 Sb、 Zn等微量元素;"交点"型铀矿化形成于中深部高温环境,成矿热液具有地幔流体特征,成矿过程硫来源与该区花岗岩中黄铁矿的硫来源一致或者相似,花岗岩中的黄铁矿可能为该期成矿事件的产物;竹山下矿床在垂向上表现出越往深部硫逸度越低的特征;"交点"型和硅化带型中黄铁矿具有相似的微量元素配分曲线,表明二者具有相同的成矿热液来源,且与辉绿岩中黄铁矿配分曲线相似,表明该区成矿热液具有深源性。  相似文献   

10.
The adsorption of gold(I) hydrosulphide complexes by iron sulphide surfaces   总被引：4，自引：0，他引：4  
The adsorption of gold by pyrite, pyrrhotite, and mackinawite from solutions containing up to 40 mg/kg (8 μm) gold as hydrosulphidogold(I) complexes has been measured over the pH range from 2 to 10 at 25°C and at 0.10 m ionic strength (NaCl, NaClO4). The pH of point of zero charge, pHpzc, has been determined potentiometrically for all three iron sulphides and shown to be 2.4, 2.7, and 2.9 for pyrite, pyrrhotite, and mackinawite, respectively. In solutions containing hydrogen sulphide, the pHpzc is reduced to values below 2. The surface charge for each sulphide is therefore negative over the pH range studied in the adsorption experiments. Adsorption was from 100% in acid solutions having pH < 5.5 (pyrite) and pH < 4 (mackinawite and pyrrhotite). At alkaline pH’s (e.g., pH = 9), the pyrite surface adsorbed 30% of the gold from solution, whereas the pyrrhotite and mackinawite surfaces did not adsorb.The main gold complex adsorbed is AuHS°, as may be deduced from the gold speciation in solution in combination with the surface charge. The adsorption of the negatively charged Au(HS)2− onto the negatively charged sulphide surfaces is not favoured. The X-ray photoelectron spectroscopic data revealed different surface reactions for pyrite and mackinawite surfaces. While no change in redox state of adsorbent and adsorbate was observed on pyrite, a chemisorption reaction has been determined on mackinawite leading to the reduction of the gold(I) solution complex to gold(0) and to the formation of surface polysulphides. The data indicate that the adsorption of gold complexes onto iron sulphide surfaces such as that of pyrite is an important process in the “deposition” of gold from aqueous solutions over a wide range of temperatures and pressures.  相似文献   

11.
Mesozoic and Cenozoic sandstone-hosted copper deposits in South China are confined to the variegated rock formation of the faulted basins, the intermontane basins and piedmont basins around a copper-bearing old land. The variegated rock formation is generally of fluviolacustrine delta facies, shore facies and shore-cauce facies. The ore bodies are stratiform, occurring in the light-coloured beds of the variegated rock formation. The mineralization comprises chalcocite, bornite, chalcopyrite, native copper, covellite, pyrite and hematite, showing obvious zonation. The associated profitable elements in the ore are mainly silver, lead, zinc, molybdenum, selenium and uranium. The copper deposits are believed to have been formed through three processes of enrichment, i.e. weathering (copper-bearing weathered crust was formed as a result), deposition (source bed formed) and diagenesis (ore body formed). The variegated rocks with Cu, Ag, Pb, Zn, U, Mo, Cl and organic carbon anormalies and a great deal of pyrite, distributed in the faulted basins around the Cu-bearing old land, are recognized as the most favourable area for copper ore exploration.  相似文献   

12.
The minimum age of a zone of secondary uranium mineralization, located at the Austatom Prospect in the Alligator Rivers region of Australia, is estimated to be 3.6 × 105y. This is derived from a geochronological model based on retarded leaching of 234U with respect to 238U and on ratios within the ore of these members of the 238U decay series. Although kaolinite is a dominant mineral in the weathered schist-host-rocks, retarded dissolution of 234U occurs only in the presence of the clay minerals illite and montmorillonite. In their absence the reverse occurs. A model is proposed to explain the results. Ratios of 230Th to 238U indicate that the mineralization has probably remained stationary within the weathered schist for at least 1 to 2 × 105y. Future use of clay minerals as buffers in radioactive waste repositories is supported by the excellent long-term retention obtained for oxidized uranium, probably due in part to isomorphic substitution into the clay crystal lattice.  相似文献   

13.
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   

14.
Evaluation of the long-term health risks of uranium contamination in soils, sediments, and groundwater requires a fundamental understanding of the various processes affecting subsurface transport of uranium, including adsorption processes at mineral/water interfaces. In this study, the sites of binding and surface complexation of U(VI) adsorbed on the (11?02) surfaces of α-Al2O3 and α-Fe2O3 have been determined using crystal truncation rod (CTR) diffraction and grazing incidence extended X-ray absorption fine structure (GI-EXAFS) spectroscopy. The available binding sites on the (11?02) surfaces were constrained through bond valence and steric analyses. On both surfaces, U(VI) forms uranyl-carbonato ternary complexes to surface oxygens that are singly coordinated to aluminum or iron. On the α-Al2O3 (11?02) surface, a monodentate complex results, whereas on the α-Fe2O3 (11?02) surface, the binding is bidentate to adjacent singly coordinated oxygen sites (i.e., binuclear). Differences in protonation of the singly coordinated oxygen atoms, surface charging, U(VI) aqueous speciation, substrate structure, or the electronic structure of surface functional groups may be the cause of these differences in adsorption geometry. Both XPS and CTR diffraction reveal higher U(VI) surface coverages on the α-Fe2O3 (11?02) surface than on the α-Al2O3 (11?02) surface. This difference cannot be the result of differences in defect concentration alone as CTR diffraction is not sensitive to U(VI) sorbed to defect sites, implying that the α-Fe2O3 (11?02) surface has an intrinsically higher affinity for U(VI). The surface complexes observed in this study are different from the bidentate, mononuclear complexes typically derived for U(VI) on powdered aluminum- and iron-(oxyhydr)oxides and clay minerals using U LIII-edge EXAFS spectroscopy. However, the presence of monodentate, mononuclear and bidentate, binuclear complexes may have been overlooked in past EXAFS studies on such substrates, as these complexes have U-Al or U-Fe interatomic distances that are too large to be easily detected by EXAFS spectroscopy.  相似文献   

15.
张麻井铀钼矿床是中国北方最大的与火山岩有关的热液铀矿床，围岩蚀变广泛发育，其中黄铁矿化在该矿床分布虽 较为局限，但是与铀钼成矿关系密切。为了研究黄铁矿化蚀变与铀、钼成矿的亲缘关系，文章对张麻井的黄铁矿化蚀变岩 进行主、微量元素分析，并选择Yb作为不活动组分，使用质量平衡迁移计算方法， 利用Grant公式对其组分迁移进行定量 计算。岩石地球化学特征显示，黄铁矿化蚀变岩的TFeO含量极高，介于11.24%~24.57%之间(平均18.45%)，其中Fe2O3含量 10.78%~25.25% （平均18.64%）、FeO含量1.43%~1.90% （平均1.69%），Fe2O3/FeO比值平均为10.99，有可能受到后期氧 化。黄铁矿化蚀变岩在Isocon图解上等浓度线斜率小于1，表明整体发生了组分的带入，带入的主要组分为大量的TFeO （131倍），成矿元素Mo（884倍）、Pb（11倍）、U（4.9倍）、V（2.8倍）、Ta（0.44倍）、Cu（0.64倍），碱金属Na2O（0.45 倍），以及Cd（424倍）、Bi（13倍） 等；带出的主要组分有碱金属Li（-0.73）、K2O（-0.17），成矿元素Zn（-0.38）、Cr （-0.37），以及Eu（-0.58）、Sc（-0.25） 等。其中SiO2略微减少（-0.03），带入的Mo含量远大于U的含量，据此认为黄铁 矿化与钼成矿关系更为密切。  相似文献   

16.
张麻井铀钼矿床是中国北方最大的与火山岩有关的热液铀矿床,围岩蚀变广泛发育,其中黄铁矿化在该矿床分布虽 较为局限,但是与铀钼成矿关系密切。为了研究黄铁矿化蚀变与铀、钼成矿的亲缘关系,文章对张麻井的黄铁矿化蚀变岩 进行主、微量元素分析,并选择Yb作为不活动组分,使用质量平衡迁移计算方法, 利用Grant公式对其组分迁移进行定量 计算。岩石地球化学特征显示,黄铁矿化蚀变岩的TFeO含量极高,介于11.24%~24.57%之间(平均18.45%),其中Fe2O3含量 10.78%~25.25% （平均18.64%）、FeO含量1.43%~1.90% （平均1.69%）,Fe2O3/FeO比值平均为10.99,有可能受到后期氧 化。黄铁矿化蚀变岩在Isocon图解上等浓度线斜率小于1,表明整体发生了组分的带入,带入的主要组分为大量的TFeO （131倍）,成矿元素Mo（884倍）、Pb（11倍）、U（4.9倍）、V（2.8倍）、Ta（0.44倍）、Cu（0.64倍）,碱金属Na2O（0.45 倍）,以及Cd（424倍）、Bi（13倍） 等;带出的主要组分有碱金属Li（-0.73）、K2O（-0.17）,成矿元素Zn（-0.38）、Cr （-0.37）,以及Eu（-0.58）、Sc（-0.25） 等。其中SiO2略微减少（-0.03）,带入的Mo含量远大于U的含量,据此认为黄铁 矿化与钼成矿关系更为密切。  相似文献   

17.
通过野外采样、化学分析、电子探针(EPMA)和X射线衍射(XRD)分析等手段,研究了贵州织金地区黑色页岩矿物成分、化学组分、微量元素、稀土元素特征。研究区矿样化学成分以SiO_2和Al_2O_3为主,且具有高K低Na的特征。电子探针和X射线衍射分析表明,研究区黑色页岩主要矿物组成有石英、粘土矿物、白云石及黄铁矿等。织金黑色页岩中Pb、Ni、U、V、Cr等金属元素存在不同程度的富集,稀土元素总量为153.2×10~(-6)~224.89×10~(-6),属轻稀土元素富集型。同时从多金属层、页岩气、页岩提钾及近底部含磷铀矿资源等方面讨论了织金黑色页岩资源化利用。织金黑色页岩多金属层含有Mo、V、Ni、Ag及U等多金属元素,具综合利用价值;其中有机碳含量达到页岩气开发大于2%的条件,可进一步开展研究;页岩中伊利石含量较多,可提取黑色页岩中的钾制备含钾复合肥;黑色页岩底部与磷矿层接触带产出磷铀矿,主要为胶状磷铀矿,接触带可作为铀矿找矿的标志层。  相似文献   

18.
Reductive immobilization of uranium by the stimulation of dissimilatory metal-reducing bacteria (DMRB) has been investigated as a remediation strategy for subsurface U(VI) contamination. In those environments, DMRB may utilize a variety of electron acceptors, such as ferric iron which can lead to the formation of reactive biogenic Fe(II) phases. These biogenic phases could potentially mediate abiotic U(VI) reduction. In this work, the DMRB Shewanella putrefaciens strain CN32 was used to synthesize two biogenic Fe(II)-bearing minerals: magnetite (a mixed Fe(II)-Fe(III) oxide) and vivianite (an Fe(II)-phosphate). Analysis of abiotic redox interactions between these biogenic minerals and U(VI) showed that both biogenic minerals reduced U(VI) completely. XAS analysis indicates significant differences in speciation of the reduced uranium after reaction with the two biogenic Fe(II)-bearing minerals. While biogenic magnetite favored the formation of structurally ordered, crystalline UO2, biogenic vivianite led to the formation of a monomeric U(IV) species lacking U-U associations in the corresponding EXAFS spectrum. To investigate the role of phosphate in the formation of monomeric U(IV) such as sorbed U(IV) species complexed by mineral surfaces, versus a U(IV) mineral, uranium was reduced by biogenic magnetite that was pre-sorbed with phosphate. XAS analysis of this sample also revealed the formation of monomeric U(IV) species suggesting that the presence of phosphate hinders formation of UO2. This work shows that U(VI) reduction products formed during in situ biostimulation can be influenced by the mineralogical and geochemical composition of the surrounding environment, as well as by the interfacial solute-solid chemistry of the solid-phase reductant.  相似文献   

19.
The mineralogy and geochemistry of the massive pyrite-pyrrhotite mineralization, which contains minor magnetite, sphalerite and galena, the weathered profile and surface gossan at Mugga Mugga in Western Australia have been examined. Reactions between amphibolite wall rocks and acid waters from the oxidation of the iron sulfides have resulted in distinct mineralogical zonation of the weathered profile which is further modified near the surface by lateritization. At the base of the weathered zone an opaline chert (Opal-CT) has been precipitated from fluctuations of the water table. A gossanous zone from 25.14–68.80 m with boxworks after massive pyrite is modified by abundant kaolinite, dickite and an alunite-type mineral derived from amphibolite wall rocks, while above 25.14 m both plinthite and mottled clay zones of a laterite profile are evident. Some characteristics of a mature gossan profile – sulfate-phosphate-arsenate near the base, a carbonate zone higher in the profile, and an oxide zone near the surface – overprint the gross zonation.At the interface between sulfide and weathered rock Mg, Ca, K, S, Zn, Cd, Hg, Ba are depleted, As, Sb, Mo, Cr and V contents increase and in the weathered zone, SiO2, TiO2, P2O5, SO3, Pb, Zn, Hg, Sb, Co, Ni, W, Ba, Sr and Zr decrease up the profile whilst Al2O3, Fe2O3, CO2, Cu and As increase. Of the elements associated with the massive pyrite (Pb, Zn, Cu, Ag, As, Cd, Hg, Sb, Co, Ni) anomalous concentrations of Pb, Cu, Ag, As and Sb occur in the surface gossan despite the possibility of complete leaching by highly acidic solutions. These anomalies are similar to those found in gossans over pyrite mineralization elsewhere in the Yilgarn Block.  相似文献   

20.
Feldspar minerals are thermodynamically unstable in the near-surface environment and their surfaces are well known to react readily with aqueous solutions, leading to incongruent dissolution at low pH values, but congruent dissolution at neutral and high pH values. Interactions with mineral surfaces are an important control on the environmental transport of trace elements and detrital feldspars are abundant in soils and sediments. However, the interactions of metal ions in solution with the reacting feldspar surface have not been widely explored. The interactions of Pb(II), U(VI) and Np(V) ions with the feldspar surface have therefore been studied. Lead is taken up by the microcline surface at pH 6 and 10, but no uptake could be measured at pH 2. There was measurable uptake of Pb(II) on the plagioclase surface at pH 2, 6 and 10. Uptake always increased with pH. In most conditions, Pb(II) reacts through cation exchange process although, at high pH, a discrete phase, probably hydrocerrusite, is observed by atomic force microscopy (AFM) to precipitate on the plagioclase surface. Supersaturation with hydrocerrusite in these conditions is expected from thermodynamic calculations. Uptake of uranyl ion , generally through surface complex formation, could only be measured at pH 6 and 10. At pH 6 and an initial U(VI) concentration above 21.0 μM, precipitation of becquerelite (Ca[(UO2)3O2(OH)3]2·8H2O), identified by AFM and characterised by grazing incidence X-ray diffraction and X-ray photoelectron spectroscopy, is observed on plagioclase. The U(VI) concentration range in which becquerelite precipitation begins (dissolved U(VI) 1-5 μM) is consistent with that predicted from thermodynamic modelling. On plagioclase feldspar, secondary ion mass spectrometry showed diffusion of uranium into the altered surface layer. Uptake of the neptunyl ion (Np(V)) was found at pH 6 and 10 for microcline and at pH 2, 6 and 10 for plagioclase, and was generally lower than uptake of U(VI). By combining batch sorption experiments with imaging and surface analysis, and thermodynamic modelling, it has been possible to gain a mechanistic insight into the reactions of the feldspar surface with metal ions in solution.  相似文献   

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