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1.
137Cs was dispersed globally by cold war activities and, more recently, by the Chernobyl accident. Engineered extraction of 137Cs from soils and groundwaters is exceedingly difficult. Because the half-life of 137Cs is only 30.2 years, remediation might be more effective (and less costly) if 137Cs bioavailability could be demonstrably limited for even a few decades by use of a reactive barrier. Essentially permanent isolation must be demonstrated in those few settings where high nuclear level wastes contaminated the environment with 135Cs (half-life 2.3×106 years) in addition to 137Cs. Clays are potentially a low-cost barrier to Cs movement, though their long-term effectiveness remains untested. To identify optimal clays for Cs retention, Cs desorption was measured for five common clays: Wyoming Montmorillonite (SWy-1), Georgia Kaolinites (KGa-1 and KGa-2), Fithian Illite (F-Ill), and K-Metabentonite (K-Mbt). Exchange sites were pre-saturated with 0.16 M CsCl for 14 days and readily exchangeable Cs was removed by a series of LiNO3 and LiCl washes. Washed clays were then placed into dialysis bags and the Cs release to the deionized water outside the bags measured. Release rates from 75 to 139 days for SWy-1, K-Mbt and F-Ill were similar; 0.017% to 0.021% sorbed Cs released per day. Both kaolinites released Cs more rapidly (0.12% to 0.05% of the sorbed Cs per day). In a second set of experiments, clays were Cs-doped for 110 days and subjected to an extreme and prolonged rinsing process. All the clays exhibited some capacity for irreversible Cs uptake. However, the residual loading was greatest on K-Mbt (0.33 wt.% Cs). Thus, this clay would be the optimal material for constructing artifical reactive barriers.  相似文献   

2.
《Chemosphere》2002,49(10)
The distribution coefficients (Kd) and desorption rates of 137Cs and 241Am radionuclides in bottom sediments at different locations in the Black Sea were studied under laboratory conditions. The Kd values were found to be 500 for 137Cs and 3800 for 241Am at the steady state and described exponential curves. Rapid uptake of the radionuclides occurred during the initial period and little accumulation happened after four days. The desorption rates for 137Cs in different bottom sediments were best described by a three-component exponential model. The desorption half-times of 137Cs ranged from 26 to 50 d at the slow components. However, the desorption rate of 241Am described one component for all sediment samples and desorption half-time was found to be 75 d. In general, the results showed that the 241Am radionuclide is more effectively transferred to bottom sediment and has longer turnover time than 137Cs under Black Sea conditions.  相似文献   

3.
Results are reported for a series of migration experiments performed in a hydraulically characterized, single, natural fracture in a block of granite with overall dimensions of 1 × 1 × 0.7 m (all approximate), using the conservative, poorly sorbing and strongly sorbing radionuclides 3H20, 131I, 22Na, 85Sr, 137Cs, 60Co, 154,155Eu, 237Np, and 238Pu. The volumetric flow velocity of the transport solution was 3 ml h−1, giving a residence time in the fracture of approximately 50 h. Elution profiles were obtained for 3H20, 131I, 22Na, 85Sr and 137Cs but no evidence of the other radionuclides was observed in the eluent. Results from supporting static sorption measurements on crushed geological materials and granite coupons showed in general higher sorption on alteration minerals than on granite. Sorption was lowest for 22Na and 85Sr.The migration of 131I, 22Na, 85Sr through the fracture in real time was followed using end-window Geiger-Müller probes located in unused boreholes. Additional information, obtained by alpha and gamma scanning of the fracture surfaces after separating the block along the fracture, confirmed that transport had occurred along the flow path predicted from the hydraulic characterization of the fracture and that, over a 5.5 month period, the bulk of the injected 137Cs had migrated only 75 cm along the flow path. The 60Co, the rare earths and the actinides had not moved beyond the location of the injection borehole, suggesting that fracture infilling minerals played a major role in retarding radionuclide transport. Additional confirmation of the role of secondary minerals in radionuclide retardation was obtained using selective sequential extraction on the fracture surfaces. These observations support the inclusion of sorption data for fracture infilling minerals in the sorption database developed for the geosphere model for the Canadian Nuclear Fuel Waste Management Program.  相似文献   

4.
We present results from experiments on the migration of 137Cs through columns containing quartz sand. Times for 137Cs movement through these columns and the quantity of 137Cs adsorbed by the sand decreased as the ionic strength of the pore water increased from 0.002 to 0.1 m. The breakthrough curves were characterized by a slow approach towards steady-state concentrations as well as by long tails, indicating that 137Cs adsorption to the sand grains was, at least in part, controlled by rate-limited reactions. Various formulations for solute mass transfer were tested for their ability to fit the experimental breakthrough curves. Based on a statistical analysis, a nonlinear, two-site model was identified as the most appropriate for describing the suite of experimental data. Variation in the model parameter that describes the rate of 137Cs adsorption to the sand showed no consistent pattern with changes in ionic strength. In contrast, model parameters describing the sorption capacity of the sand grains and the fraction of kinetic sorption sites on the sand decreased with increasing ionic strength. The parameter describing the rate of 137Cs desorption varied directly with changes in ionic strength.  相似文献   

5.
The present study focuses on the exceptional Saharan dust event that affected most of France in February 2004. Activity levels of various artificial radionuclides (90Sr, 137Cs, uranium, thorium and plutonium isotopes, 241Am) were examined. Activity or isotopic ratios are discussed in the context of atmospheric nuclear weapons tests, among them French tests performed in Sahara in the 1960s. The daily evolution of 137Cs activity levels in the atmosphere was compared to daily PM10 change. A link between airborne 137Cs and PM10, is given. It is estimated that this 2-day event deposited as much 137Cs as would be deposited on average over a 10-month period. The amount of deposited 137Cs and 239+240Pu represents respectively about 0.1 and 1% of the activity already present in the soil. Such Saharan dust events correspond to an extreme type of “feeder” process of artificial radionuclides in the atmosphere. Therefore, they contribute to the long term background level of artificial radionuclides kept at trace levels in the atmosphere.  相似文献   

6.
Decades-long monitoring of anthropogenic radionuclides in the atmospheric deposition in Tsukuba, Japan suggests not only the substantial impacts of the Asian dust (Kosa) on the deposition but also the possible change of the Kosa source region, especially during springs of the 2000s. In order to know more about such change, 4 single wet deposition events occurred in the spring of 2007 were scrutinized. The largest anthropogenic radionuclides wet deposition was supplied by the April 2–4 event. It brought several tens % of the monthly depositions (April 2007) of the dust (residue) mass (4.5 g m?2) and anthropogenic radionulides (90Sr: 16, 137Cs: 97 and Pu: 3 mBq m?2). None of the events observed fulfilled both criteria of the specific activities and 90Sr/137Cs activity ratio to the Tsukuba soil; they did not exhibit local soil dust signature. The Kosa events in fact have extensive impacts on the atmospheric environment over Japan in spring season. Considering the elevated specific activities as well as greater 137Cs/90Sr activity ratio in the deposited dust, it is hypothesized that the dust source areas in Asian continent would be shifting from the arid zone to the desert-steppe zone suffering from desertification during the 2000s. This type of the Kosa may be called as the ‘new-regime Kosa’. Chemical observation in the far downwind region of the Kosa dust could allow us to know possible shift in the source regions.  相似文献   

7.
Zusammenfassung Ziel und Schwerpunkte  Um das Verhalten des künstlichen Radionuklids137Cs im Landschaftshaushalt der Saar-Lor-Lux Region zu klaren, wurdend die r?umliche Verteilung sowie das deszendente Migrationsverhalten und die Tiefenfunktionen des Radioisotops in den wichtigsten Bodensubstraten saarl?ndischer Wald?kosysteme untersucht. Ergebnisse  Demnach finden sich die h?chsten137Cs-Aktivit?ten im Norden des Landes, w?hrend die Gebiete im Süden und Südosten deutlich geringere Konzentrationen aufweisen. Es konnten deszendente Migrationsraten zwischen 0,25 cm/a und 1,0 cm/a festgestellt werden. Durchschnittlich treten die h?chsten Migrationsraten in den tonig-schluffigen Substraten des Muschelkalks auf (0,66 cm/a), gefolgt von den lehmig ausgepr?gten Substraten des Unterrotliegenden (0,53 cm/a) und den sandigen Substraten des Buntsandsteins (0,41 cm/a). In den tonarmen Bodensubstraten des Unterrotliegenden und des Buntsandsteins lassen sich 90–95% der Aktivit?ten in den oberen 10 cm der humusreichen Oberb?den nachweisen, wohingegen in den tonreichen Substraten des Muschelkalks bis zur gleichen Tiefe nur etwa 70–76% zu finden sind. Schlussfolgerungen  Mit einem Abnehmen der als Leitbahnen fungierenden Prim?r-und Sekund?rporen in zunehmender Tiefe ist künftig mit einer deutlichen Reduzierung der Verlagerungsgeschwindigkeit von137Cs in den Substraten des Muschelkalks zu rechnen. Insbesondere bei geringm?chtigen B?den auf kluftreichem Ausgangsgestein impliziert die maximale Eindringtiefe des Isorops von 40 cm in den Unterboden jedoch eine m?gliche Kontamination des oberfl?chennahen Grundwassers, ebenso wie an Standorten mit hohem Grundwasserstand. Ausblick  Aufgrund der hier vorgestellten Ergebnisse wurde ein137Cs-Monitoring in das Boden-Dauerbeobachtungsprogramm des Landesamts für Umweltschutz des Saarlandes aufgenommen Online-First: 25. April 2000  相似文献   

8.
The adsorption behavior of 241Am, 60Co, 137Cs and 85Sr in the presence and absence of chelating ligands (ethylenediaminetetraacetic acid, ethylenediaminediacetic acid, hydroxyethyliminodiacetic acid, iminodiaceiticacid and methyliminodiacetic acid) was investigated. Sorption affinity in the absence of chelating ligands followed: Am(III) > Co(II) > Cs(I) > Sr(II). The presence of chelating ligands generally had little effect on sorption of 85Sr and 137Cs with Kd values 110 and 690 mL g−1, respectively. But at 0.02 M of ethylenediaminetetraacetic or hydroxyethyliminodiacetic, the Kd decreased to 5 or 63 mL g−1, respectively, where thermochemical modeling indicated almost all 85Sr is complexed with these ligands. The Kd values for 241Am and 60Co generally decreased with increasing chelating agent concentrations. In notable cases, the Kd values for Am increased at specific concentrations of 10−3 M for IDA, MIDA and 10−4 M for EDDA. This is proposed to be due to formation of a ternary surface complex.  相似文献   

9.
以煤矸石为原料,采用碱熔后水热合成法制备X型分子筛并进行XRD、SEM、BET和Zeta电位分析。研究其对水中Co2+、Cu2+、Cd2+和Cr3+4种离子的吸附性能,包括吸附等温线、吸附动力学以及初始金属离子浓度、pH值对吸附性能的影响。所合成的矸石基X型分子筛的BET比表面积为676.02 m2/g,微孔孔容为0.263 cm3/g。吸附实验表明,矸石基X型分子筛能有效去除上述4种离子,同时实现煤矸石的资源化和金属离子的去除。4种离子的平衡吸附量均随初始浓度的增大而增大,相同条件下平衡吸附量的大小顺序为Cd2+>Cr3+>Cu2+>Co2+。准二级动力学模型能很好地描述4种离子的吸附动力行为。Langmuir模型对Co2+、Cu2+和Cd2+吸附的拟合较Freundlich模型高,说明其主要表现为物理吸附过程。4种离子的吸附速率均由液膜扩散和颗粒内扩散共同控制。  相似文献   

10.
Concentrations of 32 elements, Ag, As, Au, Ba, Ca, Ce, Co, Cr, Cs, Eu, Fe, Hf, K, La, Lu, Mo, Na, Nd, Ni, Rb, Sb, Sc, Se, Sm, Sr, Ta, Tb, Th, U, W, Yb, and Zn were determined by instrumental neutron activation analysis (INAA) in the early preserved epiphytic lichens (Parmotrema recticulatum) from the remote southwestern China area in the 1960s, 1980s and 1990s. The concentrations of Ag, As, Ce, Cr, Cs, Eu, Fe, Hf, La, Nd, Ni, Sc, Se, Sm, Tb, U, Yb and Zn were dropped down by the temporal prolongation. The elemental concentration levels obtained from the organisms indicate that the extent of heavy metal atmospheric deposition among the sampling sites has been declining during the past decades.  相似文献   

11.
满江红干体对锌离子的生物吸附   总被引:2,自引:1,他引:1  
以满江红干体为生物吸附剂,研究了不同条件下对废水中Zn2+的净化作用。结果表明,满江红干体对Zn2+的吸附是一个快速的过程,前5 min的吸附量达到最大吸附量的62.9%,30 min达到吸附平衡;初始pH值对Zn2+的吸附有显著的影响,最适pH值为6;随着干体量的增加,吸附率逐渐提高而吸附量则降低;随着Zn2+初始浓度的增加,吸附率逐渐降低而吸附量则提高。满江红干体对Zn2+的吸附符合Langmuir吸附等温线方程,最大吸附容量达57.5 mg/g。5次吸附解吸循环实验数据表明,重复次数和再生处理对满江红干体的吸附能力没有产生显著影响。因此,满江红干体在处理含Zn2+废水中的重复使用是可行的。  相似文献   

12.
Functionalized magnetic core–zeolitic shell nanocomposites were prepared via hydrothermal and precipitation methods. The products were characterized by vibrating sample magnetometer, X-ray powder diffraction, Fourier transform infrared spectroscopy, nitrogen adsorption–desorption isotherms, and transmission electron microscopy analysis. The growth of mordenite nanocrystals on the outer surface of silica-coated magnetic nanoparticles at the presence of organic templates was well approved. The removal performance and the selectivity of mixed metal ions (Pb2+ and Cd2+) in aqueous solution were investigated via the sorption process. The batch method was employed to study the sorption kinetic, sorption isotherms, and pH effect. The removal mechanism of metal ions was done by chem–phys sorption and ion exchange processes through the zeolitic channels and pores. The experimental data were well fitted by the appropriate kinetic models. The sorption rate and sorption capacity of metal ions could be significantly improved by optimizing the parameter values.  相似文献   

13.
Artificial radionuclides, such as iodine-131 (131I), cesium-134 (134Cs), and cesium-137 (137Cs), as well as natural isotopes of beryllium-7 (7Be) and potassium-40 (40K) have been registered in atmospheric aerosols over Vladivostok selected from 11 March to 17 June 2011. Additionally, 134Cs and 137Cs were detected in atmospheric aerosols over Tomsk selected from 16 March to 17 June 2011. Artificial radionuclides were also discovered in atmospheric wet depositions sampled in Vladivostok from 3 to 17 May 2011. Moreover, these radionuclides have been registered in atmospheric aerosols over the sea surface of the Sea of Japan selected from 3 to 31 May 2011 during an expedition of the “Nadezhda” sailing ship. From 18 March to 15 April, an increase in concentrations of atmospheric aerosols over Vladivostok from 108.8 to 321.5 μg/m3 has been registered. It was accompanied by increased activity concentrations of 134Cs, 137Cs, and the 131I. During the period from 18 March to 15 April, activity concentrations of 137Cs and 134Cs in atmospheric aerosols increased 100 times compared with the minimum detectable concentration (MDC) level and peaked in the weekly sample gathered from 8 to 15 April (145.0 and 105.3 μBq/m3, respectively). Variability of concentrations of natural isotopes of 7Be and 40K was not greater than 1 order of magnitude throughout the sampling period. Maximal values of 137Cs and 134Cs concentrations (1,281.5?±?141 and 384.4?±?42.3 μBq/m3, respectively) in Tomsk were reached in samples taken from 1 to 2 April. For the atmospheric aerosol samples from the Sea of Japan, the largest concentration of 131I (392.3?±?215.7 μBq/m3) was detected from 13 to 19 May, while all other samples had much lower concentration values. Synoptic analysis of back trajectories movement of air masses showed that the radioactive cloud came to Vladivostok from the regions of Siberia and northeastern part of China. Synoptic analysis for Tomsk showed that during the period of maximal activity concentrations (1–9 April), air masses were arriving from the European part of Russia and north of Kazakhstan.  相似文献   

14.
Retardation capacity of organophilic bentonite for anionic fission products   总被引:7,自引:0,他引:7  
Sorption and diffusivity of iodide and pertechnetate (I- and TcO4-) on MX-80 bentonite with different hexadecylpyridinium (HDPy+) loadings were studied using equilibrium solutions of different ionic strengths. In HDPy(+)-modified bentonite, iodide and pertechnetate ions exhibited increasing sorption (characterized by the distribution ratio, Rd), while Cs+ and Sr2+ showed decreasing sorption with increasing organophilicity. In case of medium-loading levels, the simultaneous sorption of anions (I- and TcO4-) and cations (Cs+ and Sr2+) was observed. Sorption of ions was influenced by the composition of the electrolytes employed. It decreased gradually with increasing ionic strength of the electrolyte solutions. The experiments revealed the general tendency that the diffusivity (Da [cm2.s-1]) for iodide and pertechnetate decreases with increasing organophilicity and increases with increasing ionic strength of the equilibrium solutions, confirming the results of the sorption experiments. Additionally, some mineralogical and chemical investigations, like IR spectral analysis of the organo-bentonite samples and exchange behavior of HDPy+, were performed. On the basis of these analyses, it was concluded that the alkylammonium ions are sorbed as (1) HDPy+ cations, (2) HDPyCl molecules and (3) micelles with decreasing binding intensities in this order.  相似文献   

15.
In case of an accident at a nuclear power plant with liberation of radioactive material into the atmosphere, knowledge about the behavior of plant species when in contact with radionuclides is indispensable for safety reasons. The leaf-fruit translocation is an important route through which agricultural products are contaminated by radionuclides. To quantify the leaf-fruit translocation factors for 137Cs and 90Sr in common beans (Phaseolus vulgaris) an experiment was carried out in a greenhouse with a randomized block design. 137Cs activity was determined by gamma-ray spectrometry, while chemical separation followed by beta counting of 90Y was used for 90Sr determination. The model applied for translocation indicated functional dependence between the moment of tracer application and the physiological development of the bean plant. Translocation factors obtained for 137Cs and 90Sr were 0.16 and less than 0.005, respectively.  相似文献   

16.
Background, Aims and Scope Advances in radioecology can support improvements in environmental remediation technologies, especially by illuminating interaction processes between polymorphic metal radionuclides and various materials and their ions in aqueous solutions. This study modeled interaction processes of 90Sr with transitive metals to delineate the behavior of polymorphic metal radionuclides. Experimental and modeling results confirmed Sr sedimentation was sensitive to the physical impact of radionuclides on various sorbents and possible chemical reactions occurring between the radionuclides and sorbents. Methods Models were developed to simulate 90Sr sedimentation process, and the potential physical and chemical reactions accompanying the process. Models were verified, inorganic salts were used as sorbents to absorb metal cations, activity levels were recorded before and after mixing the inorganic salts while the efficiency of sedimentation using the heavy metals composites was quantified. Results and Discussion This research demonstrates that the process of the sedimentation is complex and occurs in several stages. Micro-structural analysis shows that zones of interaction between the sorbent and source metal are formed during the irradiation of the target’s metal surface. Electrical-microscopic analysis indicates that the composition of the formed zones of interaction of Ti (Sr) with target metals has various structures. Roentgenophase analysis indicates that the interaction of the ions of a precipitable source and a target occurs according to constitution diagrams of equilibrium systems. The results indicate that application of inorganic salts composites based on modeling increases the efficiency of the deactivation of aqueous solutions when compared to standard aluminum sulfate composite. Conclusions Experimental and modeling results confirm 90Sr sedimentation is sensitive to the physical impact of radionuclides on various sorbents and possible chemical reactions occurring between the radionuclides and sorbents. The models support estimation of the physical impact of polymorphic metal radionuclides on various components of sorbents and possible chemical reactions occurring between the radionuclides and sorbents during the interaction. Inorganic salt composites deactivate and clear 90Sr and Sr+2 from water. This paper is openly accessible!  相似文献   

17.
为了开发新型廉价生物吸附剂,以高效吸附去除水体中全氟辛烷磺酸盐(PFOS),对小球藻提取生物柴油后的藻渣吸附酸性水体中的PFOS进行了吸附行为及机理的研究。小球藻提取生物质柴油后,比表面积、孔容、孔径几乎没有变化;等电点由3.3降低至2.7;蛋白质含量由51.45%提高到57.35%。在酸性条件下(pH≤3),小球藻和藻渣对PFOS的吸附率均达到99%以上;随着pH值增加至7,二者的吸附去除率迅速降低,但仍保持在22%~26%。小球藻和藻渣对PFOS的最大吸附容量分别为353.69 mg/g和444.83 mg/g。Freundlich模型能较好地拟合二者对PFOS的吸附数据,表明为多层吸附,即小球藻以静电吸引的形式吸附PFOS阴离子,并疏水分配至所含蛋白质中;而藻渣中含量较高的蛋白质对PFOS的疏水性分配作用是导致藻渣吸附量增高的主要原因。  相似文献   

18.
A three-site cation exchange model is proposed to describe the concentration dependent uptake of Cs on natural argillaceous rock systems. Major premises in the model are that the sorption of Cs is dominated by the illite mineral component in the rock and that there is a fixed relationship between the site capacities of the three site types denoted as frayed edge, type II and planar sites. The definition of a “reference illite” with a cation exchange capacity of 0.2 equiv. kg-1 allows the three site capacities to be fixed in the model calculations over the weight fraction of illite in the argillaceous rocks. Up to Cs equilibrium concentrations of 10-3 M sorption occurs predominantly on the frayed edge and type II sites (higher affinity sites), with the planar site type playing only a minor role. Competition with Cs for sorption on the former two site types arises predominantly from monovalent cations such as K, Rb and NH4 which have low hydration energies. H and Na (except at high concentrations) are considerably less competitive and bivalent cations such as Mg, Ca and Sr are effectively non-competitive. A consistent set of selectivity coefficients for Cs with respect to K, Rb, NH4 and Na was derived from analyses and modelling of a wide range of Cs sorption data available in the open literature on pure illites from many different sources. The model was tested against four Cs sorption isotherm data sets determined on argillaceous rocks: Boom clay, Oxford clay, Palfris marl and Opalinus clay. The water chemistries and illite contents given in these experiments allowed the Cs sorption isotherms to be predicted. It is concluded that the Cs sorption model presented here, in which there are no free parameters, can be used to predict the uptake of Cs at equilibrium concentrations below 10-3 M to within a factor of 2 to 3 in natural argillaceous rock systems.  相似文献   

19.
《Chemosphere》2013,90(11):1316-1322
Carbon nanotubes (CNTs), as a type of superior adsorbents for both organic and inorganic contaminants, are increasingly introduced into the environment. Ubiquitous natural organic matter (NOM) would coat on the released CNTs and change their physicochemical properties and sorption of contaminants. The effects of four sequentially extracted humic acids (HAs, as a model NOM) from a peat soil on the physicochemical properties and Cd(II) sorption of three multiwalled CNTs (MWNTs) with different surface areas were investigated. The MWNTs as purchased with very few oxygen-containing functional groups had relatively low sorption capacities (0.93–1.49 mg g−1) for Cd(II) and the sorption capacity increased with increasing surface area of the MWNTs. Surface-coating with the HAs lowered surface areas of the MWNTs but greatly increased their sorption capacities (5.42–18.4 mg g−1). The MWNT-bound HAs introduced oxygen-containing functional groups and negative charges to the MWNT surfaces, which could thus increase the apparent sorption of Cd(II) through chemical complexation and electrostatic attraction, respectively. The later-extracted HAs with lower polarity were more favorable for the surface-coating but increased less Cd(II) sorption by the MWNTs. The results are expected to shed light on understanding the underlying mechanism of the effect of NOM on the sorption of heavy metal ions by CNTs.  相似文献   

20.
Following the Chernobyl accident in late April 1986, central Finland was subjected to considerable radioactive fallout. The radioactive isotope of caesium, (137)Cs, was potentially the most harmful isotope in the fallout because of its long half-life (30 years). (137)Cs activities remained unexpectedly low within the biota (algae, zooplankton, aquatic moss, fish) of some humic forest lakes in southern Finland compared to the clear water lakes within the same district. This observation suggested that humic substances, by binding (137)Cs chemically, may reduce its bioavailability in lake water. Our laboratory experiments (throughflow systems; gel chromatography) demonstrated that binding of (137)Cs by humic substances was negligible in untreated lake waters; only when most of the alkali metals had been removed with an ion exchange resin was any binding of (137)Cs by low molecular humic fractions apparent. Instead, the concentrations of cations (especially potassium) were of overwhelming importance for the bioavailability of (137)Cs within the lacustrine ecosystems. The concentrations of (137)Cs within food chains are expected to stay at a high level for many years especially in lakes with long water renewal times.  相似文献   

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