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《Applied Geochemistry》2001,16(9-10):1067-1082
Thermodynamic data for all fate-determining processes are needed in order to predict the fate and transport of metals in natural systems. The surface complexation properties of a synthetic MnO2, δ-MnO2, have accordingly been investigated using glass electrode potentiometry. Experimental data were interpreted according to the surface complexation model in conjunction with the diffuse double layer model of the solid/solution interface. Adsorption constants were determined using the non-linear optimisation program FITEQL. Surface complexation parameters determined in this way were validated against results obtained from the literature. Best fits of alkalimetric titration data were obtained with a 2-site, 3 surface-species model of the δ-MnO2 surface. Site concentrations of 2.23×10−3 mol g−1 and 7.66×10−4 mol g−1 were obtained. Corresponding logarithms of formation constants for the postulated surface species are −1.27 (≡XO−), −5.99 (≡YO−) and 3.52 (≡YOH2+) at I=0.1 M. The surface speciation of δ-MnO2 is dominated by ≡XO− over the pH range investigated. Metal adsorption was modelled with surface species of the type ≡XOM+, ≡XOMOH, ≡YOM+, ≡YOMOH (M=Cu, Ni, Zn, Cd and Pb) and ≡XOM2OH2+ (M=Pb). For Cu, Ni and Zn, titration data could be modelled with ≡XOM+, ≡XOMOH, ≡YOM+ and ≡YOMOH, whereas for Cd, ≡XOM+ and ≡YOM+ were sufficient. Lead data were best modelled by assuming the dinuclear species ≡XOM2OH2+ to be the only surface species to form. Adsorption constants determined for Ni, Cu and Zn follow the Irving-Williams sequence. The model suggests an adsorption order of (Pb, Cu) > (Ni, Zn) > Cd. The discrepancy between model predictions and published adsorption results is similar to the variability observed in experimental results from different laboratories.  相似文献   

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4.
研究海水体系(即Na+,K+,Mg2+,Ca2+∥Cl-,$SO_{4}^{2-}$-H2O六元体系)中杂卤石的形成条件不仅有助于理解海相蒸发盐成因,对开发杂卤石钾资源利用技术也具有重要的指导作用。但杂卤石以及其他含有硫酸钙矿物(如二水石膏、半水石膏、无水石膏、钾石膏、多钙钾石膏、钙芒硝和水钙芒硝)的相平衡,无论是在实验研究方面还是在热力学模拟方面都仍然存在很多争议。由于缺乏杂卤石在复杂水溶液体系中可靠的相平衡数据,使人们对认识杂卤石成因和利用杂卤石钾资源带来巨大障碍。本工作对海水体系中杂卤石的形成条件进行了热力学模拟和实验研究。超过一年的长时间固液平衡实验表明25 ℃下Na+,K+,Mg2+,Ca2+∥Cl-,$SO_{4}^{2-}$-H2O六元体系中杂卤石的形成区域极为可观,且较前人实验结果均大数倍;同时证实了热力学模型预测结果的可靠性。这些结果为讨论盐矿床中杂卤石的形成条件提供了物理化学依据。25 ℃下可靠的热力学信息表明:杂卤石与其他盐类矿物的共生情况丰富多样,并且与前人看法不同,杂卤石的形成并不需要极高的钾、镁浓度。这给以杂卤石为指示寻找可溶性固体钾盐带来了挑战,但却指示了以杂卤石为线索更容易找到钾、镁盐未饱和的富钾卤水。  相似文献   

5.
采用溶胶-凝胶法在低温、还原气氛下制备了长余辉发光材料SrAl2O4∶Eu2+,Dy3+.用X射线粉晶衍射对其进行了物相鉴定,表明在1 050 ℃已经得到纯相的SrAl2O4产物,1 150～1 400 ℃物相没有改变,仍是SrAl2O4相.研究了灼烧工艺、铕和锶的比值、硼酸的加入量、激活剂铕和镝的比值、基质元素铝和锶的比值等条件对SrAl2O4∶Eu2+,Dy3+长余辉发光材料的相对发光强度的影响.结果表明:采用H2作还原气氛,灼烧温度为1 200 ℃,恒温2 h,然后随炉自然降温的生产工艺,可制备出发光性能优良的长余辉发光材料.  相似文献   

6.
沸石对放射性核素Cs+,Sr2+的吸附阻滞作用   总被引：7，自引：0，他引：7  
通过对新疆乌鲁木齐浅水河地区沸石的物化性质和工程特性(包括阳离子交换容量、孔结构、粒度组成、击实密度、渗透系数等)、活化处理以及对放射性核素C s ,S r2 吸附性能的研究,结果表明:该沸石的阳离子交换容量(CEC)达到97.9 m eq/100 g,在中性条件下最高为195.4 m eq/100 g;击实后的渗透系数为8.7×10-4m/s。沸石对溶液中的C s ,S r2 吸附量分别达到162.6×1-0 3和74.9×1-0 3,吸附效果优于内蒙高庙子膨润土矿。经过钠改性和铵改性处理后的沸石,对C s 的吸附量有不同程度的提高,最高达234.5×1-0 3;但对S r2 的吸附效果影响不大。溶液pH值对C s ,S r2 的吸附量有明显影响,中性和碱性环境更有利于沸石吸附作用的进行。  相似文献   

7.
Mineralogical analysis, electrical conductivity and thermopower are reported for monocrystalline heterosite (Fe3+, Mn3+)PO4 with the orthorhombic olivine-type structure. The 57Fe Mössbauer spectrum could be adequately described using two Fe3+ doublets. By impedance spectroscopy (20 Hz–1 MHz) the electrical DC conductivity σDC and AC conductivity σAC were determined parallel (∥) and perpendicular to the [001] direction (space group Pnma) in the range ～160–440 K. The graph log σDC?1/T shows a slightly bent curve in both directions with activation energies of E A ～0.30 and ～0.15 eV in the high and low temperature ranges, respectively. The reduced E A is associated with electronic conduction; σDC ∥ [001] follows Mott’s T 1/4 variable range hopping law at lower temperatures with hopping between localized levels. The values of σAC are increased relative to σDC at high frequencies and low temperatures, obeying Jonscher’s universal dynamic response law; for σAC ∥ [001], the variation with temperature of the frequency exponent is in fair agreement with the model of small polaron hopping. The absolute thermopower Θ is negative and low between ～295 and ～440 K, Θ does hardly vary with temperatures in both directions; the temperature independency of Θ ∥ [001] is consistent with the small polaron hopping model.  相似文献   

8.
在对河南油田下二门矿区油田污水进行全面分析的基础上，研究了污水中Fe^2 ，S^2-，溶解氧（DO）及污水的pH值对无机交联体系聚丙烯酰胺（HPAM）－Cr^3 胶成分散凝胶（CDG）成胶性能的影响。研究结果表明，对于HPAM－Cr^3 体系，污水中Fe^2 ，DO对其成胶性能没有影响；S^2-和污水的pH值对其成胶性能有影响。pH值增大，凝胶强度增强；S^2-浓度增加，则凝胶强度减弱。  相似文献   

9.
电气石吸附Cu2+,As(Ⅲ),F-影响因素及机理研究   总被引：1，自引：0，他引：1  
以新疆电气石为原料,通过原子荧光光谱仪、原子吸收分光光度研究电气石的不同粒度、用量、吸附时间、热处理温度等对水中Cu2 ,As(Ⅲ)吸附的影响;进而探讨分析电气石的吸附机理。研究结果表明:(1)电气石对Cu2 ,As(Ⅲ),F-离子的去除率随着电气石粒径的减小而增加。随着电气石用量的增加,去除率逐渐提高,增至一定值后下降。热处理温度为300℃,500℃时,可提高电气石吸附Cu2 ,As(Ⅲ)的效率。加热预处理未改善电气石对F-离子吸附能力。(2)电气石对带电性质不同的阴、阳离子都具有较好的吸附作用。电气石的极性和表面性质使其对离子可能存在络合吸附和静电吸附两种形式。电气石对Cu2 ,As(Ⅲ)吸附为表面络合吸附与静电吸附共同作用,吸附效果好。对F-吸附只存在静电吸附,吸附效果差。  相似文献   

10.
Summary Crystals of K2[Co2(SeO3)3]-2H2O and K2[Ni2(SeO3)3]-2H2O were synthesized under low-hydrothermal conditions. Their structures were determined using single crystal X-ray data up to sin / = 0.7Å-1. [Space group P63/m; a = 9.091(3),9.016(2)Å; c = 7.562(2), 7.476(2)Å; Z = 2; RW = 1.6, 2.5%]. The investigations confirmed that K2[Co2(SeO3)3].2H2O and K2[Ni2(SeO3)3]-2H2O represent the first selenites belonging to the zemannite structure type, a framework structure with wide channels running parallel [0001]. In both compounds four maxima were clearly located in the channel by Fourier summations and attributed to two K atoms and two H2O molecules, each with an occupancy factor of 1/6; a possible ordering scheme (full occupancy) with local symmetry 1 and [6]-coordinated K atoms could be derived for the channel atoms.Zusammenfassung Kristalle von K2[Co2(SeO3)3]-2H2O und K2[Ni2(SeO3)3]-2H2O wurden unter niedrig-hydrothermalen Bedingungen synthetisiert. Die Strukturen wurden unter Verwendung von Einkristallröntgendaten bis sin /= 0.7Å-1 bestimmt. [Raumgruppe P63/m; a = 9.091(3), 9.016(2)Å; c = 7.562(2), 7.476(2)Å; Z = 2; RW = 1.6, 2.5%] Die Untersuchungen bestätigten, daß K2[Co2(SeO3)3] - 2H2O und K2 [Ni2(SeO3)3] - 2H2O als erste Selenite dem Strukturtyp des Zemannits angehören, einer Gerüststruktur mit weiten, parallel [0001] verlaufenden Kanälen. In beiden Verbindungen wurden im Kanal vier Maxima durch Fourier-Summationen eindeutig lokalisiert und zwei Kalium-atomen sowie zwei H2O Molekülen, jeweils mit einem Besetzungsfaktor von 1/6, zugeschrieben. Für die Kanalatome konnte ein möglicher Ordnungszustand (volle Besetzung) mit lokaler Symmetrie 1 und [6]-koordinierten Kaliumatomen abgeleitet werden.
Selenite des Zemannittyps: Kristallstrukturen von K2[Co2(SeO3)3] - 2H2O und K2[Ni2(SeO3)3]-2H2O

Dedicated to Prof. Dr. Josef Zemann at the occasion of his 70th birthday

With 2 Figures  相似文献   

11.
采用等温溶解平衡法研究了288K时Li+, Mg2+//SO2-4, B4O2-7- H2O四元体系的固液相平衡关系,测定了该四元体系在288K时平衡液相的溶解度和密度.依据实验测定的平衡溶解度数据及对应的平衡固相,绘制了该四元体系的平衡相图及密度组成图.研究结果表明:交互四元体系Li+, Mg2+//SO2-4, B4O2-7- H2O 288K时平衡相图中有2个共饱点,5条单变量曲线,4个结晶区对应的平衡固相分别为Li2B4O7·3H2O,Li2SO4·H2O,MgB4O7·9H2O和MgSO4·7H2O.  相似文献   

12.
Polarized single crystal absorption spectra, in the spectral range 40 000–5 000 cm-1, were obtained on Co2+ in trigonally distorted octahedral oxygen fields of buetschliite-type K2Co(SeO3)2 (I), K2Co2(SeO3)3 (II) and zemannite-type K2Co2(SeO3)3 · 2H2O (III). Site symmetries of Co2+ are m (D3d) in I, 3m (C3v) in II, and 3 (C3) in III. The spectra can be interpreted on the basis of an electric dipole mechanism, wherein transitions of Co2+ in the centrosymmetric site in I gain intensity from dynamic removal of the inversion centre by vibronic coupling. In accordance with the elongation of the CoO6 octahedra along the trigonal axis, the split component E(g) of the ground state 4T1g in octahedral fields is the ground state in all three compounds. Trigonal field parameters Dq(trig), D, D and the Racah parameters B have been fitted to the energies of spin allowed transitions (293 K) as follows: I: 744, 94, -16, and 838 cm-1, resp.; II: 647, 227, 42, and 798 cm-1, resp.; III: 667, 181, 21, and 809 cm-1, respectively. Racah parameters C were estimated from the energy of some observed spin-forbidden transitions to be 3770 (I), 3280 (II), and 3465 cm-1 (III). Values of Dq and of the Racah parameters B and C indicate slight differences of Co2+-O bonding in I as compared to II and III, with somewhat higher covalency in compounds II and III which contain face-sharing CoO6 octahedra with short Co-Co contacts. Also, in II and III the observed D values do not agree with theoretical D values, predicted from the magnitude of the mean octahedral distortions.  相似文献   

13.
用等温溶解平衡法研究了四元体系K+,Na+∥Clˉ,Brˉ-H2O 348 K条件下的相平衡关系,测定了该交互四元体系在相应温度条件下平衡溶液的溶解度和密度,并根据相平衡实验数据绘制了相应的相图.研究结果表明:四元体系K+,Na+∥Clˉ,Brˉ-H2O348 K条件下属于固溶体型,相图中含有1条单变量曲线,2个平衡固相结晶区,无共饱和点.其平衡固相分别为固溶体K(Cl,Br)和Na(Cl,Br),其中固溶体K(Cl,Br)结晶区较大,固溶体Na(Cl,Br)结晶区较小.与同体系313 K条件下的相图相比,348 K时固溶体Na(Cl,Br)·2H2O结晶区消失.  相似文献   

14.
We define and calibrate a new model of molar volume as a function of pressure, temperature, ordering state, and composition for spinels in the supersystem (Mg, Fe2+)(Al, Cr, Fe3+)2O4 ? (Mg, Fe2+)2TiO4. We use 832 X-ray and neutron diffraction measurements performed on spinels at ambient and in situ high-P, T conditions to calibrate end-member equations of state and an excess volume model for this system. The effect on molar volume of cation ordering over the octahedral and tetrahedral sites is captured with linear dependence on Mg2+, Al3+, and Fe3+ site occupancy terms. We allow standard-state volumes and coefficients of thermal expansion of the end members to vary within their uncertainties during extraction of the mixing properties, in order to achieve the best fit. Published equations of state of the various spinel end members are analyzed to obtain optimal values of the bulk modulus and its pressure derivative, for each explicit end member. For any spinel composition in the supersystem, the model molar volume is obtained by adding excess volume and cation order-dependent terms to a linear combination of the five end-member volumes, estimated at pressure and temperature using the high-T Vinet equation of state. The preferred model has a total of 9 excess volume and order-dependent parameters and fits nearly all experiments to within 0.02 J/bar/mol, or better than 0.5 % in volume. The model is compared to the current MELTS spinel model with a demonstration of the impact of the model difference on the estimated spinel-garnet lherzolite transition pressure.  相似文献   

15.
The thermodynamic properties of the copper carbonates malachite and azurite have been studied by adiabatic calorimetry, by heat-flux Calvet Calorimetry, by differential thermal analysis (DTA) and by thermogravimetrie (TGA) analysis. The heat capacities, C p 0 of natural malachite and azurite have been measured between 3.8 and 300 K by low-temperature adiabatic calorimetry. The heat capacity of azurite exhibits anomalous behavior at low temperatures. At 298.15 K the molar heat capacities C p 0 and the third law entropies S 298.15 0 are 228.5±1.4 and 254.4±3.8 J mol?1 K?1 for azurite and 154.3±0.93 and 166.3±2.5 J mol?1 K?1 for malachite. Enthalpies of solution at 973 K in lead borate 2PbO·B2O3 have been measured for heat treated malachite and azurite. The enthalpies of decomposition are 105.1±5.8 for azurite and 66.1±5.0 kJ mol? for malachite. The enthalpies of formation from oxides of azurite and malachite determined by oxide melt solution calorimetry, are ?84.7±7.4 and ?52.5±5.9 kJ mol?1, respectively. On the basis of the thermodynamic data obtained, phase relations of azurite and malachite in the system Cu2+-H2O-CO2 at 25 and 75 °C have been studied.  相似文献   

16.
本文用抽空石英管法对三元硫化物体系Ag_2S-PbS-Bi_2S_3和Cu_2S-PbS-Bi_2S_2的500℃相关系进行了研究。Cu_2S-PbS-Bi_2S_3体系的相图特征是Bi_2S_3-CuPbBiS_3。之间完全固溶关系,以及它与二元系Cu_2S-Bi_2S_3和PbS-Bi_2S_3各相之间双变关系。Ag_2S-PbS-Bi_2S_3体系相图被PbS-AgBi_S_2之间的完全固溶关系分成两部分:富铋与富银。富银部分仅有辉银矿与PbS-AgBiS_2固溶体之间简单双变关系,而富铋部分却包含丰富的银、铅铋硫盐。在抽空石英管法500℃下合成成功的有块硫铋银矿固溶体、铜银铅铋矿、硫铋铅矿固溶体、富硫铋铅矿和辉铅铋矿。 以上两个体系中矿物之间共生长关系及稳定范围也作了简短讨论。  相似文献   

17.
离子色谱法测定水样中S2-、SO2-3、SO2-4、S2O2-3   总被引：1，自引：0，他引：1  
时艳  刘江潮 《吉林地质》2001,20(2):64-71
该种方法利用离子色谱仪的电导检测器与电化学检测器串联,十几分钟即可连续完成水中S2-、SO2-3、SO2-4、S2O2-3的测定,方法具有快速、高效、方便、灵敏、选择性好等特点.方法的检出限分别为S2-12.5μg/L;SO2-3 22.4μg/L;SO2-4 5.0μg/L;S2O2-3 5.0μg/L.相对标准偏差在1.5%～6.9%之间,能够满足水中S2-、SO2-3、SO2-4、S2O2-3四种阴离子分析测试的需要.  相似文献   

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19.
从对固溶体中离子的扩散机制研究中发现：保温温度为773K－1023K时，斜方顽火辉石－正铁辉石固溶液中Fe^2 ，Mg^2 发生有序－无序扩散；扩散机制有两种类型：等价于spinadal分解机制或等价于“成核－生长”机制；并对扩散条件进行了探讨。  相似文献   

20.
《Geochimica et cosmochimica acta》1999,63(19-20):3105-3119
A comprehensive low-temperature thermodynamic model for the geochemically important Na2CO3−MgCO3−CaCO3−H2O system is presented. The model is based on calorimetrically determined ΔfH°298 values, S°298 values and C°p(T) functions taken from the literature as well as on μ°298 values of solids derived in this work from solubility measurements obtained in our laboratories or by others. When these thermodynamic quantities were combined with temperature-dependent Pitzer parameters taken from the literature, solubilities calculated for a wide range of conditions agree well with experimental data. The results for several subsystems were summarized by depicting the respective phase diagrams. For the MgO−CO2−H2O subsystem, it was found that the commonly believed stability relations must be revised, i.e., in the temperature range covered, nesquehonite never becomes more stable than hydromagnesite at pCO2 ≤ 1 atm. Although the recommended set of thermodynamic data on sparingly soluble solids was derived from experimental results on mainly NaClO4 systems, it can be incorporated in databanks containing additional Pitzer parameters for modeling more complex fresh- or seawater systems.  相似文献   

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