Influence of microorganisms on the behavior of technetium and other elements in paddy soil surface water

Insolubilization patterns of technetium (Tc) and other trace elements (Sc, Co, Zn, Se, Rb, Sr, Y, Nb, Ce, Pm, Gd, Lu, Hf, and Re) in surface water covering paddy fields were compared to gain insight into the behavior of Tc in an agricultural environment. The insolubilization of Tc, which did not pass through a 0.2-microm-pore-size filter, was mainly caused by bacteria. Among the 14 other elements investigated, Nb was insolubilized by bacteria and the amounts of insoluble Nb were positively correlated with those of Tc. Although Re is a chemical analog of Tc, no similarity was observed. These results suggest that Tc behaves similarly to Nb in the insolubilization in surface water covering paddy fields.     

Determination of bioavailable rhenium fraction in agricultural soils

Rhenium (Re) mobility in agricultural soils was studied in order to obtain information relevant to (99)Tc mobility in soil-to-plant systems. Since water soluble Tc and Re are highly bioavailable, extraction of Re with water was carried out in addition to a total Re determination in the soils. The geometric means of total Re for paddy field, upland field and other soils were 0.34, 0.23, and 0.28 ng g(-1), respectively, while those of water soluble Re (<0.45 microm membrane filterable) were 0.053, 0.015 and 0.008 ng g(-1), respectively. There were no differences for total Re among soil uses; however, the water soluble Re/total Re ratio was significantly higher in paddy field soils (16%) than in other soil uses (6% for upland fields and 3% for other uses). Rhenium mobility and plant availability were higher in paddy fields than in other agricultural fields, and similar phenomena would be expected for (99)Tc.     

Redox reaction of iodine in paddy soil investigated by field observation and the I K-Edge XANES fingerprinting method

In order to elucidate the cause for the leaching of iodine in a flooded paddy field, we investigated the transformation of an iodine species affected by the water management of the paddy field. The increased concentration of iodide (I(-)) in soil solution of a flooded paddy field suggested that I(-) was leached from the soil under anaerobic conditions. The post-edge feature of X-ray absorption near-edge structure (XANES) for iodate (IO(3)(-)) spiked to soil totally disappeared after anaerobic incubation of the soils, and I(-) was dissolved in the solution. On the other hand, I(-) in contact with the soil was not likely to be oxidized to IO(3)(-) under aerobic incubation. Iodine was leached out in soil solution as I(-) under anaerobic conditions, whereas part of the iodine species was retained by soil as I(2) or organoiodine both under anaerobic and aerobic conditions.     

Technetium species induced in maize as measured by phosphorimager

Leaves of plants have the ability to accumulate the long-lived fission product (99)Tc. In the present work, an attempt was made to separate and characterize technetium species formed in maize grown on soil contaminated with Tc(VII)O(4)(-) solution. Data obtained from selective extraction, a Phosphorimager and liquid scintillation were employed.     

Influence of climatic conditions and soil type on 99TcO4- uptake by rye grass

Climatic changes over the long term will modify significantly the biosphere, with glaciation events probably taking place in the next 100 000 years. This is important to safety assessments of nuclear waste disposal facilities that contain high-level and long-lived waste.The soils will evolve toward new situations, and their properties will be consequently modified (e.g. an increase of soil organic matter may be expected in a cooler climate). These changes in soil properties would affect the mobility and the soil-to-plant transfer of radionuclides such as (99)Tc. This study aimed at simulating the cooling of climatic conditions for soils representative of a Jurassic limestone plateau, and the effect on transfer parameters of (99)TcO(4)(-) in the soil-plant systems was investigated. The cooler conditions were simulated by increasing elevation, a surrogate for climate change. Soils were sampled in similar geological background and topography at different elevations in the north east of France (Lorraine and Jura). Soil/solution distribution coefficients (K(d)) of (99)TcO(4)(-) were measured on soil samples in short-term batch experiments with 1:10 soil:solution ratio. Rye grass was grown on the soils spiked with (99)TcO(4)(-) at temperature regimes adapted to each soil. Also, two different temperature regimes (cold and temperate) were applied to one soil to test the effect of plant physiology and evapotranspiration on (99)TcO(4)(-) uptake. K(d) values did not show significant differences among soils in aerobic conditions, and were not significantly different from 0. During plant culture, reduction of (99)Tc was never totally achieved in soils, including in a peaty OM soil. Concentration ratios (CR) were calculated on a dry weight basis and ranged from 20 to 370. CR were always higher in high temperature regimes than in cold temperatures. They were also inversely correlated with soil organic matter (OM) content. A decrease of CR values from 5 to 10-fold was observed with increasing soil OM. Results suggested that the water holding capacity, in which (99)Tc is diluted, the nitrification potential of the soils and the evapotranspiration of plants (efficiency of uptake of soluble (99)TcO(4)(-)) were strongly involved in these differences.     

富营养水体中浮游植物生长的营养限制研究

选取位于武汉城郊汤逊湖畔的30个养殖池塘作为研究对象,运用营养盐加富试验评价了浮游植物生长的氮磷限制类型。研究发现这些池塘的氮磷含量均较高,尤其是TP,绝大部分都在0.4 mg/L以上,TN/TP(原子比)变化范围为1.7~20.3。相关分析显示,浮游植物的生物量与氮素(TN,TDN,NO3-,NH4+,NO2-)显著正相关(r=0.402~0.677,P<0.05);但与磷素(TP,TDP,PO43-)无显著相关性(P>0.05)。营养盐加富试验显示浮游植物群落对加N的响应程度要显著大于加P;受N限制的池塘数量占50%;P限制的占13.3%;N、P共同限制的占23.3%;而不受N、P影响的仅占13.3%。这些结果表明:在富营养的水体中,当TP浓度>0.4 mg/L且TN/TP<20时,N是限制浮游植物生长的主要因子,P处于第二位。     

Soil migration and plant uptake of technetium from a fluctuating water table

Soil columns (50x15 cm) were used to determine the potential for 95mTc (as a surrogate for 99Tc which is an important component of some radioactive waste) to migrate from a contaminated, fluctuating water table, through sandy loam soil and into perennial ryegrass. Upward migration was significantly retarded with, generally, only the bottom few centimetres of soil becoming contaminated over the 6 months of the experiment. This is thought to have been due to the presence of anoxic conditions within the water table leading to the reduction of pertechnetate to Tc(IV) species which are relatively insoluble. However, some evidence of very slow upward migration over time was found. Only a small and inconsistent transfer of activity into the perennial ryegrass was observed. Whilst these observations would suggest that 99Tc is less important than radionuclides such as 129I and 36Cl in terms of the risk associated with radioactive waste disposal, the potential for a slow upward migration, and/or a pulse-release following the re-oxidation of reduced soil in which 99Tc has accumulated should not be overlooked.     

Availability of 99Tc in undisturbed soil cores

Models for safety assessment of radioactive waste repositories need accurate values of the soil-to-plant transfer of radionuclides. In oxidizing environments, (99)Tc is expected to occur as pertechnetate ((99)TcO(4)(-)). Due to its high mobility, leaching of this element in the field might be important, potentially affecting the reliability of estimated transfer parameters of (99)Tc as measured in closed experimental systems such as hydroponics or pot experiments. The aim of this experiment was to measure the leaching of (99)Tc in undisturbed irrigated soil cores under cultivation as well as plant uptake and to study the possible competition between the two transfer pathways. Undisturbed soil cores (50 x 50 cm) were sampled from a Rendzic Leptosol (R), a colluvial Fluvic Cambisol (F) and a Dystric Cambisol (D) using PVC tubes (three cores sampled per soil type). Each core was equipped with a leachate collector at the bottom, allowing the monitoring of (99)Tc leaching through the cores. Cores were placed in a greenhouse and maize (Zea mays L., cv. DEA, Pioneer) was sown. After 135 d, maize was harvested and radioactivity determined in both plant and water samples. Results showed that during the growing period, leaching of (99)Tc was limited, due to the high evapotranspiration rate of maize. After harvest, leaching of (99)Tc went on because of the absence of evapotranspiration. Effective uptake (EU) of (99)Tc in leaves and grains was calculated. EU reached 70% of the input in the leaves and was not significantly different among soils. These results confirmed those obtained from pot experiments, even though leaching was allowed to occur in close-to-reality hydraulical conditions. As a consequence, it was concluded that pot experiments are an adequate surrogate for more complex "close-to-reality" experimental systems for measuring transfer factors.     

Distribution of pesticides, PAHs and heavy metals in prawn ponds near Kolleru lake wetland, India

This paper discussed the distribution of pesticides, polycyclic aromatic hydrocarbons (PAHs) and heavy metals in water, sediment and prawn from intensive prawn ponds (n=8) near the Kolleru lake wetland, India and assessed the quality of prawn for human consumption and also discussed the possible effects of these pollutants on pond environment and aquatic environment. The chemicals and other products used in prawn ponds near the Kolleru lake wetland were documented. The sediment, prawn and water samples were collected six times from selected prawn ponds during the production period of 3 months. Water samples were analyzed for selected physico-chemical parameters. The levels of pesticides, PAHs and heavy metals were found to decrease in the order sediment followed by prawn and water. The maximum concentrations of pesticides in sediment, prawn and water were alpha-BHC (174.2 microg g(-)(1)), gamma-BHC (234 microg g(-)(1)), malathion (256 microg g(-)(1)), chloripyrifos (198.5 microg g(-)(1)), endosulfan (238 microg g(-)(1)), dieldrin (19.6 microg g(-)(1)) and p,p'-DDT (128.6 microg g(-)(1)). Isodrin was found below detectable limit. The maximum concentrations of PAHs in sediment, prawn and water are anthracene (0.901 microg kg(-)(1)), fluranthene (0.601 microg kg(-)(1)), pyrene (0.786 microg kg(-)(1)), chrysene (0.192 microg kg(-)(1)), benzo(a)pyrene (0.181 microg kg(-)(1)) and benzo(ghi)perylene (227 microg kg(-)(1)). Benzo(e)pyrene, perylene, isomers of dibenzoanthracene and coronene were found below detectable limits. The maximum concentrations of heavy metals in sediment, prawn and water and also in prawn feed are Cu (791 microg g(-)(1)), Pb (270 microg g(-)(1)), Cd (1.07 microg g(-)(1)), Mn (4417 microg g(-)(1)), Ni (8.1 microg g(-)(1)), Co (5.8 microg g(-)(1)), Zn (1076 microg g(-)(1)), Cr (36.4 microg g(-)(1)), As (2.9 microg g(-)(1)), Se (6.3 microg g(-)(1)), Th (2.1 microg g(-)(1)) and Mo (0.762 microg g(-)(1)).     

2000~2010年汉江流域湿地动态变化及其空间趋向性

基于面向对象分类方法建立汉江流域2000年、2005年和2010年湿地景观数据库。运用湿地景观动态变化指数、强度指数及多度指数等方法分析近10a来汉江流域湿地景观变化的时空分异特征及空间趋向性。结果表明：2000年以来，汉江流域湖泊、河流、水田湿地面积大幅度减少，其中前5a（2000~2005年）湿地变化强度明显高于后5a（2005~2010年）。空间趋向性以湿地景观内部转变和湿地向其他用地转移为主要特征，内部转变以水田与水库坑塘间的转变为主，在空间上呈现3种趋向特征：湖泊周围[0-12]km两者之间转化强度随距离拉大而增大；河流周围两者转变趋势明显，在[4-6] km变化尤为突出；交通用地附近[0-4] km水田与水库坑塘间转变强度高。水田、湖泊和水库坑塘湿地向建设用地的转变是引起区域湿地面积萎缩的重要原因，10a间湿地向建设用地转变总量约为470.43 km²，占湿地变化总量的22.55%。     

Sea-to-land transfer of technetium-99 through the use of contaminated seaweed as an agricultural soil conditioner

The use of seaweed as an agricultural soil conditioner gives rise to a potential pathway for the transfer of Technetium-99 ((99)Tc) from marine to terrestrial ecosystems and thence to man. However, to date there is little information on the extent of the release of (99)Tc from seaweed into soil and the mechanisms involved. This pot experiment has shown that (99)Tc is released fairly rapidly from Fucus vesiculosus into a sandy coastal soil. Despite low temperature conditions, 60% of the (99)Tc added with the seaweed had accumulated in the soil 15 weeks after addition. Concurrent CO(2) monitoring (used as a measure of microbial decomposition or catabolism) suggested that the initial (99)Tc release (up to 40% in the first 8 weeks) was due to leaching from the seaweed and that microbial decomposition was responsible for the release of the remaining (99)Tc in the latter phase (12-15 weeks).     

X-ray absorption spectroscopy studies of reactions of technetium, uranium and neptunium with mackinawite

Technetium, uranium and neptunium may all occur in the environment in more than one oxidation state (IV or VII, IV or VI and IV or V respectively). The surface of mackinawite, the first-formed iron sulfide phase in anoxic conditions, can promote redox changes so a series of laboratory experiments were carried out to explore the interactions of Tc, U and Np with this mineral. The products of reaction were characterised using X-ray absorption spectroscopy. Technetium, added as TcO4(-), is reduced to oxidation state IV and forms a TcS(2)-like species. On oxidation of the mackinawite in air to form goethite, Tc remains in oxidation state IV but in an oxide, rather than a sulfide environment. At low concentrations, uranium forms uranyl surface complexes on oxidised regions of the mackinawite surface but at higher concentrations, the uranium promotes surface oxidation and forms a mixed oxidation state oxide phase. Neptunium is reduced to oxidation IV and forms a surface complex with surface sulfide ions. The remainder of the Np coordination sphere is filled with water molecules or hydroxide ions.     

Assessing field-scale migration of radionuclides at the Nevada Test Site: "mobile" species

Many long-lived radionuclides are present in groundwater at the Nevada Test Site (NTS) as a result of 828 underground nuclear weapons tests conducted between 1951 and 1992. In conjunction with a comprehensive geochemical review of radionuclides ((3)H, (14)C, (36)Cl, (99)Tc and (129)I) that are presumably mobile in the subsurface, we synthesized a body of radionuclide activity data measured from groundwater samples collected at 18 monitoring wells, to qualitatively assess their migration at the NTS over distances of hundreds of meters and over timescales of decades. Tritium and (36)Cl showed little evidence of retardation, while the transport of (14)C may have been retarded by its isotopic exchange with carbonate minerals in the aquifer. Observed local reducing conditions (either natural or test-induced) will impact the mobility of certain redox-sensitive radionuclides (especially (99)Tc) that were otherwise soluble and readily transported under oxidizing conditions. Conversely, strongly oxidizing conditions may impact the mobility of (129)I which is mobile under reducing conditions. The effect of iodine speciation on its transport deserves further attention. Indication of delayed transport of some "mobile" radionuclides (especially (99)Tc) in the groundwater at the NTS suggested the importance of redox conditions of the natural system in controlling the fate and transport of radionuclides, which has implications in the enhanced performance of the potential Yucca Mountain repository, located adjacent to the NTS, to store high-level nuclear wastes as well as management of radionuclide contamination in legacy nuclear operations facilities.     

Effect of low continuous 99Tc intake on its absorption and metabolism in young rats

A continuous daily oral dose of (99)TcO(4)(-) (5 Bq g(-1) day(-1)) was given to young rats for 56 days. In one group the intake was continued for 98 days, while in the other the intake was stopped to facilitate the determination of biological half lives in different organs and tissues. The absorbed fraction of (99)Tc increased from 0.7 to 0.9 during the experimental period (m=0.85 sigma=0.02). The whole body retained fraction (m=0.15 sigma=0.05) indicated a storage in the tissues. The liver and kidneys showed increasing concentrations of (99)Tc until a plateau was reached after 6 and 9 weeks, then a rapid decline after the intake was stopped (half life of 6 and 5 days respectively). In hair and thyroid tissue, the accumulation of (99)Tc increased linearly then declined very slowly after the intake was stopped and did not reach a plateau during the experiment. No significant amounts of (99)Tc were detected in the muscular tissues or in the walls of the digestive tract. After the contamination period, urinary and fecal excretions fell off very quickly (1 week), but significant, though low, quantities of urinary and fecal excretions were still observed 6 weeks after stopping intake.     

Effect of indigenous bacterial activity on arsenic mobilization under anaerobic conditions

Batch biochemical leaching tests were carried out to investigate the mobility of arsenic from a contaminated soil collected from a French gold mining site. The specific objective of this research was to examine the effect of indigenous bacterial activity on arsenic mobilization under anaerobic conditions. In a first step, physical and chemical characterizations were performed to provide data concerning the liquid-solid partitioning and mobility of arsenic and other inorganic constituents. In a second step, batch bioleaching tests were conducted in shaker flasks to determine the effect of indigenous bacterial activity under different anaerobic conditions (i.e., addition of mineral nutrients and carbon sources) on arsenic mobilization. Results indicated that arsenic release during contact with deionized water was limited by its very low solubility in the interstitial solution and by the stability of the different arsenic compounds formed with the amorphous solid phases of the soil (mainly iron (oxy)hydroxides). However, an increased mobilization potential was observed over the long term under anaerobic conditions with indigenous bacterial activity enhanced by the addition of carbon sources.     

Effect of tetracycline residues in pig manure slurry on tetracycline-resistant bacteria and resistance gene tet(M) in soil microcosms

Effects of tetracycline residues from pig manure slurry on the prevalence of tetracycline-resistant bacteria and the tetracycline resistance gene, tet(M), were studied in soil microcosms. Four types of soil microcosms were established for a period of 152 days, supplemented with combinations of pig manure slurry and a tetracycline-resistant Enterococcus faecalis, CG110, containing the tetracycline resistance gene tet(M) (on the conjugative transposon, Tn916). The prevalence of both tetracycline-resistant aerobic bacteria and tetracycline-resistant enterococci declined rapidly until day 45 where no significant differences in the levels of tetracycline-resistant bacteria in any of the four types of microcosms could be detected. tet(M) could be detected in microcosms supplemented with either pig manure slurry and/or E. faecalis CG110 (tet(M)) for the whole period (152 days). tet(M) could be detected longer than tetracycline-resistant enterococci could be isolated (limit of detection 100 CFU/g soil) probably due to viable but not culturable (VBNC) bacteria with tet(M), horizontal gene transfer of tet(M) to indigenous soil bacteria or presence of "free" DNA. The concentration of chlortetracycline and oxytetracycline were almost stable through out the experimental period, but the tetracycline concentrations had no effect on prevalence of tetracycline-resistant bacteria. The presented microcosm approach simulated natural farmland conditions well and supported results from previous field studies.     

Bioremediation of coastal areas 5 years after the Nakhodka oil spill in the Sea of Japan: isolation and characterization of hydrocarbon-degrading bacteria

Five years after the 1997 Nakhodka oil spill in the Sea of Japan, seven bacterial strains capable of utilizing the heavy oil spilled from the Nakhodka Russian oil tanker were isolated from three coastal areas (namely Katano Seashore of Fukui Prefecture, Osawa and Atake seashores of Ishikawa Prefecture) and the Nakhodka Russian oil tanker after a 5-year bioremediation process. All bacterial strains isolated could utilize long-chain-length alkanes efficiently, but not aromatic, and all of them were able to grow well on heavy oil. Using 16S rDNA sequencing, most of the strains were affiliated to Pseudomonas aeruginosa. Comparing between the year 1997 (at the beginning of bioremediation process) and the year 2001 (after 5 years of bioremediation), there was no significant change in morphology and size of hydrocarbon-degrading bacteria during the 5-year bioremediation. Scanning and transmission electron microscopic observations revealed that a large number of hydrocarbon-degrading bacteria still existed in the sites consisting of a variety of morphological forms of bacteria, such as coccus (Streptococcus and Staphylococcus) and bacillus (Streptobacillus). On the application of bioremediation processes on the laboratory-scale, laboratory microcosm experiments (containing seawater, beach sand, and heavy oil) under aerobic condition by two different treatments (i.e., placed the inside building and the outside building) were established for bioremediation of heavy oil to investigate the significance of the role of hydrocarbon-degrading bacteria on them. There was no significant bacterial activity differentiation in the two treatments, and removal of heavy oil by hydrocarbon-degrading bacteria in the outside building was slightly greater than that in the inside building. The values of pH, Eh, EC, and dissolved oxygen (DO) in two treatments indicated that the bioremediation process took place under aerobic conditions (DO: 1-6 mg/l; Eh: 12-300 mV) and neutral-alkaline conditions (pH 6.4-8) with NaCl concentrations of 3-15% (ECs of 45-200 mS/cm).     

Assessing field-scale migration of radionuclides at the Nevada Test Site: “mobile” species

Many long-lived radionuclides are present in groundwater at the Nevada Test Site (NTS) as a result of 828 underground nuclear weapons tests conducted between 1951 and 1992. In conjunction with a comprehensive geochemical review of radionuclides (³H, ¹⁴C, ³⁶Cl, ⁹⁹Tc and ¹²⁹I) that are presumably mobile in the subsurface, we synthesized a body of radionuclide activity data measured from groundwater samples collected at 18 monitoring wells, to qualitatively assess their migration at the NTS over distances of hundreds of meters and over timescales of decades. Tritium and ³⁶Cl showed little evidence of retardation, while the transport of ¹⁴C may have been retarded by its isotopic exchange with carbonate minerals in the aquifer. Observed local reducing conditions (either natural or test-induced) will impact the mobility of certain redox-sensitive radionuclides (especially ⁹⁹Tc) that were otherwise soluble and readily transported under oxidizing conditions. Conversely, strongly oxidizing conditions may impact the mobility of ¹²⁹I which is mobile under reducing conditions. The effect of iodine speciation on its transport deserves further attention. Indication of delayed transport of some “mobile” radionuclides (especially ⁹⁹Tc) in the groundwater at the NTS suggested the importance of redox conditions of the natural system in controlling the fate and transport of radionuclides, which has implications in the enhanced performance of the potential Yucca Mountain repository, located adjacent to the NTS, to store high-level nuclear wastes as well as management of radionuclide contamination in legacy nuclear operations facilities.     

Radiosensitivity of subterranean bacteria in the Hungarian Upper Permian Siltstone Formation

The main purpose of this work was to study the radioresistance of subterranean aerobic and anaerobic isolates from the Hungarian Upper Permian Siltstone (Aleurolite) Formation, in order to assess the safety of potential sites of future underground repositories for nuclear waste. A total of 93 isolates were studied. The radiosensitivities of these aerobic and anaerobic bacteria isolates were determined: the D10 values (decimal reducing doses) of the aerobic spore-formers lay in the range 0.80 -2.44 kGy, and those of the anaerobic spore-formers lay in the range 1.86 4.93 kGy. The D10 values of the aerobic and anaerobic vegetative isolates were much lower, in the ranges 0.11 0.57 and 0.22-0.40 kGy. respectively. The variability in bacterial radioresistance indicates the biodiversity at this potential disposal site. These results can affect the construction of a future underground repository, since knowledge of the most resistant microorganism may be of importance as concerns calculation of the time required to inactivate the bacteria surrounding the containers.     

Assessment of natural or enhanced in situ bioremediation at a chlorinated solvent-contaminated aquifer in Italy: a microcosm study

A microcosm study was used to assess the potential for in situ natural or enhanced bioremediation at a chloroethane- (i.e., tetrachloroethane, TeCA) and chloroethene-contaminated (i.e., tetrachloroethene, PCE; trichloroethene, TCE) groundwater in Northern Italy. All the live microcosms were positive for dechlorination, indicating the presence of an active native dechlorinating population in the subsurface. All the tested electron donors (i.e., yeast extract, lactate, butyrate, hydrogen) promoted enhanced dechlorination of chlorinated contaminants. Lactate- and butyrate-amended microcosms performed the best, and also dechlorinated the solvents past cis-dichloroethene (cis-DCE). The microcosm bioaugmented with a PCE-dechlorinating mixed culture containing Dehalococcoides spp. dechlorinated groundwater contaminants to DCE, vinyl chloride (VC), and ethene (ETH). In conclusion, results from this microcosm study indicate the potential for enhancing full dechlorination at the contaminated site, through a proper addition of a suitable electron donor (e.g., lactate or butyrate) and/or through bioaugmentation with a Dehalococcoides-containing culture.