Impact of water quality parameters on the sorption of U(VI) onto hematite

In this study, the sorption of U(VI) from aqueous solution on hematite was studied as a function of various water quality parameters such as contact time, pH, ionic strength, soil humic acid (HA) or fulvic acid (FA), solid content and temperature by using a batch technique. The results demonstrated that the sorption of U(VI) was strongly dependent on ionic strength at pH < 6.0, and outer-sphere surface complexation may be the main sorption mechanism. The sorption was independent of ionic strength at pH > 6.0 and the sorption was mainly dominated by inner-sphere surface complexation. The presence of HA/FA increases U(VI) sorption at low pH, whereas decreases U(VI) sorption at high pH. The thermodynamic parameters (ΔH⁰, ΔS⁰, and ΔG⁰) were calculated from the temperature dependent sorption isotherms, and the results suggested that U(VI) sorption was a spontaneous and endothermic process. The results might be important for the application of hematite in U(VI) pollution management.     

Removal of uranium(VI) from aqueous solutions and nuclear industry effluents using humic acid-immobilized zirconium-pillared clay

Removal of uranium [U(VI)] from aqueous solutions with humic acid-immobilized zirconium-pillared clay (HA-Zr-PILC) was investigated using a batch adsorption technique. The adsorbent was characterized using XRD, FTIR, SEM, TG/DTG, surface area analyzer and potentiometric titration. The effects of pH, contact time, initial concentration, adsorbent dose, and adsorption isotherm on the removal process were evaluated. A maximum removal of 97.6 ± 2.1 and 94.7 ± 3.3% was observed for an initial concentration of 50 and 100 mg L⁻¹, respectively at pH 6.0 and an adsorbent dose of 2.0 g L⁻¹. Equilibrium was achieved in approximately 180 min. The mechanism for the removal of U(VI) ions by HA-Zr-PILC was based on an ion exchange reaction. The experimental kinetic and isotherm data were analyzed using a second-order kinetic equation and Langmuir isotherm model, respectively. The monolayer adsorption capacity for U(VI) removal was found to be 132.68 ± 5.04 mg g⁻¹. An increase of temperature of the medium caused an increase in metal adsorption. Complete removal (≅100%) of U(VI) from 1.0 L of a simulated nuclear industry effluent sample containing 10.0 mg U(VI) ions was possible with 1.5 g of HA-Zr-PILC. The adsorbent was suitable for repeated use (over 4 cycles) without any noticeable loss of capacity.     

Removal of uranium(VI) from aqueous solutions by manganese oxide coated zeolite: discussion of adsorption isotherms and pH effect

This paper discusses the adsorption properties for uranium(VI) by manganese oxide coated zeolite (MOCZ). The removal of uranium(VI) from aqueous solution by adsorption onto MOCZ in a single-component system with various contact times, pH, competitive ions, temperatures and initial concentrations of uranium(VI) was investigated. The experimental results were fitted to the Langmuir, Freundlich and the three-parameter Redlich-Peterson model isotherms to obtain the characteristic parameters of each model. Both the Langmuir and Redlich-Peterson isotherms were found to best represent the measured adsorption data. According to the evaluation using the Langmuir equation, the maximum adsorption capacity of uranium(VI) ions onto MOCZ was 15.1 mg g(-1) at 293K and pH 4.0. Using the thermodynamic equilibrium constants obtained at different temperatures, various thermodynamic parameters, such as DeltaG(0), DeltaH(0) and DeltaS(0), have been calculated. The thermodynamics of uranium(VI) ion/MOCZ system indicates the spontaneous and endothermic nature of the process. It was noted that an increase in temperature resulted in a higher uranium loading per unit weight of the adsorbent.     

Microbial removal of uranyl by sulfate reducing bacteria in the presence of Fe (III) (hydr)oxides

Microbiological reduction of uranyl by sulfate reducing bacteria (SRB) has been proposed as a promising method for removal of radionuclide from groundwater. In this study, we examined the effect of two naturally occurring Fe(III) (hydr)oxides, hematite and goethite, on the bioreduction of U(VI) by a mixed culture of SRB via laboratory batch experiments. The biogenic precipitate from U(VI) bioreduction was determined using X-ray absorption near edge structure (XANES) analysis, showing a typical feature of uraninite (UO₂). In the presence of either hematite or goethite-containing Fe(III) ranging from 10 to 30 mM, the reduction of U(VI) was retarded by both minerals and the retardatory effect was enhanced with increasing amount of Fe(III) (hydr)oxide. When exposed to a mixture of hematite and goethite with the total Fe(III) kept constant at 20 mM, the retardatory effect on U(VI) reduction by the minerals were directly correlated with the fraction of hematite present. A slow increase in U(VI) concentration was also found in all Fe(III) (hydr)oxide treatments after 10-13 days, accompanied by the release of Fe(II) into the solution. The presence of Fe(III) (hydr)oxide can cause the eventual incomplete bioreduction of U(VI). However, it was not the case for the control without minerals. When mixing biogenic uraninite with hematite or goethite without SRB, Fe(II) was also detected in the solution. These findings suggest that the U(VI) remobilization after 10～13 days may be due to reoxidation of the uraninite by the solid-phase Fe(III) (hydr)oxide.     

Diffusive gradient in thin FILMS (DGT) compared with soil solution and labile uranium fraction for predicting uranium bioavailability to ryegrass

The usefulness of uranium concentration in soil solution or recovered by selective extraction as unequivocal bioavailability indices for uranium uptake by plants is still unclear. The aim of the present study was to test if the uranium concentration measured by the diffusive gradient in thin films (DGT) technique is a relevant substitute for plant uranium availability in comparison to uranium concentration in the soil solution or uranium recovered by ammonium acetate. Ryegrass (Lolium perenne L. var. Melvina) is grown in greenhouse on a range of uranium spiked soils. The DGT-recovered uranium concentration (C_DGT) was correlated with uranium concentration in the soil solution or with uranium recovered by ammonium acetate extraction. Plant uptake was better predicted by the summed soil solution concentrations of UO₂²⁺, uranyl carbonate complexes and UO₂PO₄⁻. The DGT technique did not provide significant advantages over conventional methods to predict uranium uptake by plants.     

Assessment of surface area normalisation for interpreting distribution coefficients (Kd) for uranium sorption

Adsorption of radionuclides on soils and sediments is commonly quantified by distribution coefficients (K_d values). This paper examines the relationship between K_d values for uranium(VI) adsorption and the specific surface area (SSA) of geologic materials. We then investigate the potential applicability of normalising uranium (U) K_d measurements using the SSA, to produce ‘K_a values’ as a generic expression of the affinity of U for the surface. The data for U provide a reasonably coherent set of K_a values on various solid phases, both with and without ligands. The K_a representation provides a way of harmonising datasets obtained for materials having different specific surface areas, and accounting for the effects of ligands in different systems. In addition, this representation may assist in developing U sorption models for complex materials. However, a significant limitation of the K_a concept is that sorption of radionuclides at trace levels can be dominated by interactions with specific surface sites, whose abundances are not reflected by the SSA. Therefore, calculated K_a values should be interpreted cautiously.     

Adsorption of thorium from aqueous solutions by perlite

The use of expanded perlite for the adsorption of thorium from aqueous solution by batch technique is presented. The effects of particle size, pH of the solution, initial thorium concentration, shaking time, V/m ratio and temperature were determined. It was found that the adsorption capacity increases by the increase in the pH of the suspensions. The rate of thorium adsorption on expanded perlite was observed to be fast in the first hour of the reaction time. Adsorption isotherms were expressed by Langmuir and Freundlich adsorption models and the adsorption experiments conducted at 30 ± 1 °C showed that the adsorption isotherms correlated well with the Langmuir model. From the adsorption data, thermodynamic parameters such as ΔG^o, ΔH^o and ΔS^o were calculated as a function of temperature.     

Distribution of uranium isotopes in surface water of the Llobregat river basin (Northeast Spain)

A study is presented on the distribution of ²³⁴U, ²³⁸U, ²³⁵U isotopes in surface water of the Llobregat river basin (Northeast Spain), from 2001 to 2006. Sixty-six superficial water samples were collected at 16 points distributed throughout the Llobregat river basin. Uranium isotopes were measured by alpha spectrometry (PIPS detectors). The test procedure was validated according to the quality requirements of the ISO17025 standard. The activity concentration for the total dissolved uranium ranges from 20 to 261 mBq L⁻¹. The highest concentrations of uranium were detected in an area with formations of sedimentary rock, limestone and lignite. A high degree of radioactive disequilibrium was noted among the uranium isotopes. The ²³⁴U/²³⁸U activity ratio varied between 1.1 and 1.9 and the waters with the lowest uranium activity registered the highest level of ²³⁴U/²³⁸U activity ratio. Correlations between uranium activity in the tested water and chemical and physical characteristics of the aquifer were found.     

Uranium isotopes in groundwater from the continental intercalaire aquifer in Algerian Tunisian Sahara (Northern Africa)

The disequilibrium between ²³⁴U and ²³⁸U is commonly used as a tracer of groundwater flow. This paper aims to identify uranium contents and uranium isotopic disequilibria variation in groundwater sampled from deep Continental Intercalaire aquifer (southern Algeria and Tunisia). Large variations in both U contents (0.006–3.39 ppb) and ²³⁴U/²³⁸U activity ratios (0.4–15.38) are observed. We conduct a first assessment in order to verify whether the results of our investigation support and complete previous hydrogeological and isotopic studies. The dissolved U content and ²³⁴U/²³⁸U activity ratio data were plotted on a two-dimensional diagram that was successfully utilized on sharing the CI aquifer into different compartments submitted to different oxidising/reducing conditions and leads also to distinguished two preferential flow paths in the Nefzaoua/Chott Fejej discharge area. Uranium isotopes disequilibrium indicate that ranium chemistry is mainly controlled by water–rock interaction enhanced by long residence time recognised for this aquifer.     

Spatial distribution of natural radioactivity levels in topsoil around the high-uranium mineralization zone of Kylleng-Pyndensohiong (Mawthabah) areas, West Khasi Hills District, Meghalaya, India

A study of background radiation and the distribution of radionuclides in the environment of the proposed uranium mining sites of Kylleng-Pyndensohiong (Mawthabah) areas, West Khasi Hills District, Meghalaya, India, has been carried out with the objective of establishing a baseline radiation level of the region. Topsoil samples collected from the region are analysed for radioactivity measurements of primordial radionuclides by gamma-spectrometry technique. Direct dose measurement using a survey meter was also carried out simultaneously. Measurement carried out in the region shows that the activity concentration of (238)U and (232)Th in soil samples is found to be highest in Kylleng with respective median values of 335.3Bqkg(-1) and 283.9Bqkg(-1) followed by Syngkai with activity concentration of 285.3Bqkg(-1) and 257.4Bqkg(-1) for (238)U and (232)Th, respectively. The distribution of (40)K concentration in the study area is found to be in the range of 173.1-359.0Bqkg(-1) which is below the global and Indian average values of 420Bqkg(-1) and 394Bqkg(-1), respectively. The contribution of the primordial radionuclides to the total dose of the study area is found to be very high with a range of 136.8-334.5nGyh(-1) in comparison to the global as well as Indian average values.     

Adsorption models of Cs radionuclide and Sr (II) on some Egyptian soils

Distribution of cesium (¹³⁴Cs and ¹³⁷Cs) and strontium (Sr-II) between soil/water phases depends on many factors such as concentration of these ions between phases, the cation exchange capacity (CEC) of the soil as well as its clay content, chemical composition (especially Na, K, Ca, and Mg ions), grain size distribution, calcite, iron oxide content, and organic coatings. Distribution coefficients (Kd) of cesium (labeled with ¹³⁷Cs) and strontium were measured on the grain size distributions ≥32 μm of four soil samples. These soils were obtained from four different locations within Inshas site in Egypt and three groundwater samples were obtained from the same site locations. X-ray diffraction showed that the soil samples consisted mainly of quartz mixed with the minor amounts of kaolonite and clay minerals. Sorption experiments were carried out at strontium aqueous concentrations range 10⁻⁷ to 10⁻⁴ mol l⁻¹. The CEC and Kds for cesium and strontium were measured at the same metal concentrations range. Distribution coefficients of cesium were found to be influenced by the composition of the soil, while the distribution coefficients of strontium were found to depend on calcium concentrations in the soil/groundwater system. The aim of this study was to determine the safety assessment of disposal ¹³⁷Cs radionuclide and Sr(II) in the aquifer regions inside the Inshas site. Sequential extraction tests showed that, strontium was associated with the carbonate fractions and majority of cesium was sorbed on the iron oxides and the residue.     

Gamma radiation measurements and dose rates in commercially-used natural tiling rocks (granites)

The gamma radiation in samples of a variety of natural tiling rocks (granites) imported in Cyprus for use in the building industry was measured, employing high-resolution gamma-ray spectroscopy. The rock samples were pulverised, sealed in 1-l plastic Marinelli beakers, and measured in the laboratory with an accumulating time between 10 and 14 h each. From the measured gamma-ray spectra, activity concentrations were determined for (232)Th (range from 1 to 906 Bq kg(-1)), (238)U (from 1 to 588 Bq kg(-1)) and (40)K (from 50 to 1606 Bq kg(-1)). The total absorbed dose rates in air calculated from the concentrations of the three radionuclides ranged from 7 to 1209 nGy h(-1) for full utilization of the materials, from 4 to 605 nGy h(-1) for half utilization and from 2 to 302 nGy h(-1) for one quarter utilization. The total effective dose rates per person indoors were determined to be between 0.02 and 2.97 mSv y(-1) for half utilization of the materials. Applying dose criteria recently recommended by the EU for superficial materials, 25 of the samples meet the exemption dose limit of 0.3 mSv y(-1), two of them meet the upper dose limit of 1 mSv y(-1) and only one clearly exceeds this limit.     

Equilibrium,kinetics and thermodynamics studies on adsorptive removal of cobalt ions from wastewater using MIL-100(Fe)

This study describes experiments in which MIL-100(Fe) was used to remove Co²⁺ ions from the waste water. The synthesised adsorbent was characterised by Fourier-transform infrared spectroscopy (FTIR), X-ray diffraction, Brunauer–Emmett–Teller (BET) and scanning electron microscope. Statistical analysis was used to investigate the effects of different parameters. From the obtained results, the removal efficiency was enhanced with increasing contact time and pH but decreased with increasing cobalt initial concentration. The maximum removal efficiency of Co⁺² was 93.4% under optimum conditions. The equilibrium adsorption data were best fitted to linearly transformed Freundlich isotherm. Adsorption kinetic data followed the pseudo second-order kinetic model. The maximum adsorption capacity of Co⁺² on to the MIL-100(Fe) was found to be 119 mg g^?1. The results showed that ?G of adsorption was negative, while ?H was positive which showed that the adsorption process was spontaneous and endothermic. The positive value of ?S showed that disordering and randomness increased at the solid–solution interface of cobalt ions with MIL-100(Fe) particles.     

Bioaccumulation and trophic transfer of polybrominated diphenyl ethers (PBDEs) in biota from the Pearl River Estuary, South China

Two hundred and fifty-four biota samples (four species of invertebrates and ten species of fish) were collected from the Pearl River Estuary between 2005 and 2007 and one hundred and twenty four individual or composite samples were analyzed for polybrominated diphenyl ethers (PBDEs). The concentrations of PBDEs in organisms varied from 6.2 to 208 ng/g lipid weight. This PBDE level was significantly lower than those collected in 2004, showing a decreasing trend of PBDEs in biota in the study area. Trophic magnification factors (TMFs) for nine BDE congeners were calculated with values ranging from 0.78 to 3.0. TMFs of BDE47, 66, 100, 99, 154, and 153 were statistically greater than one, indicating a biomagnifcation potential for these congeners. Significant positive correlations were also found between concentrations of the total PBDEs, BDE28, 47, 66, 100, 99, 154, and153 and lipid content in biota, indicating the that bioconcentration also played an important role in the accumulation of PBDEs. No correlation between trophic level and lipid content was found, suggesting that biomagnification was not the result of lipid content effect but indeed occurred. The concentration ratios of BDE99 to BDE100 were much lower in biota than that in water implying that potential congener-specific biotransformation of PBDEs occurred and influenced the biomagnification of BDE congeners.     

Environmental and economic viability of Alkali Activated Material (AAM) comprising slag,fly ash and spent coffee ground

ABSTRACT

This paper presents a concept of reusing spent coffee ground (CG) as a construction material. Through creating a CG-filled Alkali Activated Material (AAM) with industrial wastes such as fly ash (FA) and slag (S), a strong recycled material was synthesised and found suitable to be used as a road subgrade fill material. Potential groundwater contamination tests were done in accordance to the Australian Standard Leaching Procedure (ASLP). The environmental analysis done on this green material shows that albeit being composed of various industrial wastes and chemicals, CG-filled AAMs in the ground will not cause adverse environmental impacts to surrounding soils and groundwater. Heavy metals and cyanide leached from the AAMs were well below hazardous thresholds. Comparing the carbon footprint of CG, it is found that recycling CG into a construction material would reduce the nett global carbon emission by reducing dependency on quarried material. Cost analyses done on CG-filled AAMs show that these AAMs are expensive to produce relative to traditional construction materials. However, as recycling technology is progressively advancing, in the future the economic value of CG-filled AAM may increase to match those of contemporary construction materials.     

中国碳捕集、利用与封存技术研发与示范

碳捕集、利用与封存(CCUS)是一项新兴的、具有大规模减排潜力的技术,有望实现化石能源使用的CO2近零排放,被认为是进行温室气体深度减排最重要的技术路径之一.开展CCUS技术的研发和储备,将为中国未来温室气体减排提供一种重要的战略性技术选择,受到政府、企业和学术界的广泛关注.本文从CCUS技术产生和发展的背景出发,概括了该技术的特点及存在的主要同题,总结了当前中国CCUS技术政策,介绍了中国CCUS技术研发、试点示范、国际合作等的开展情况,并通过与欧美等发达国家CCUS技术发展与示范活动现状的对比,初步分析了中国CCUS技术发展方面存在的主要不足.为进一步推动我国CCUS技术的研发与示范,文章提出应加强国家层面的技术政策指导和宏观协调、引导资源有效配置;推动建设行业间的CCUS技术合作平台;重视CCUS来来技术应用软环境建设等有针对性的建议.     

天津市节能减排绩效及经济效益协调性研究

利用节能绩效-减排绩效关系图,以及节能绩效、减排绩效与经济效益协调关系三角图,研究了2006-2008年天津市17个区县及滨海新区的节能减排绩效关系及其经济协调性状态和趋势.结果如下:①2006-2008年,天津市17个区县及滨海新区的节能减排绩效整体上较差,河西区、西青区、津南区、北辰区、宝坻区、静海县和蓟县的节能减排绩效呈现变差趋势,东丽区和滨海新区(塘沽区、汉沽区和大港区)节能减排绩效很差且无明显变好趋势;其他6个区县的节能减排绩效呈现变好趋势.②2008年,北辰区、武清区、静海县3个区县的经济协调性很强,河西区、河北区、汉沽区、蓟县处于强不经济协调性状态,滨海新区处于弱不协调性状态;2006年,大部分区县(包括滨海新区)处于弱不经济协调性状态,且按强协调趋势发展,其协调性增强主要来自经济效益驱动.③天津市17个区县及滨海新区的节能减排绩效及经济协调性评估权重选择较为合理,能准确地反映节能减排现状.