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1.
In order to determine the mechanisms of the retention of 60Co, 85Sr and 134Cs in natural silica sand columns, desorption experiments were performed by changes of pH and ionic strength and by injection of natural organic matter (NOM). Injection of KCl (0.1 M) resulted in a high release of 60Co (60-100%) and 85Sr (72-100%) but a smaller release of 134Cs (31-66%). Only limited release of 60Co (66%) and 85Sr (71%) and no release of 134Cs were observed by injection of NOM. The different percentages of desorption were related to the chemical characteristics of the organic colloids previously retained in columns before the desorption step. The results evidenced different sorption processes on energetically heterogeneous surface sites. According to the initial conditions, the binding of the radionuclides to the solid phase resulted from weak and easily reversible sorption processes to strong association probably by inner sphere complexes. The rather weak release of 134Cs by KCl was attributed to the strong retention of 134Cs by clay coatings on the natural silica sand surfaces.  相似文献   

2.
Scenarios of barrier failure and radionuclide release to the near-surface environment are important to consider within performance and safety assessments of repositories for nuclear waste. A geological repository for spent nuclear fuel is planned at Forsmark, Sweden. Conceptual and numerical reactive transport models were developed in order to assess the retention capacity of the Quaternary till and clay deposits for selected radionuclides, in the event of an activity release from the repository. The elements considered were carbon (C), chlorine (Cl), cesium (Cs), iodine (I), molybdenum (Mo), niobium (Nb), nickel (Ni), radium (Ra), selenium (Se), strontium (Sr), technetium (Tc), thorium (Th), and uranium (U). According to the numerical predictions, the repository-derived nuclides that would be most significantly retained are Th, Ni, and Cs, mainly through sorption onto clays, followed by U, C, Sr, and Ra, trapped by sorption and/or incorporation into mineral phases.  相似文献   

3.
Soil contamination with radionuclides and potential remediation   总被引:5,自引:0,他引:5  
Zhu YG  Shaw G 《Chemosphere》2000,41(1-2):121-128
Soils contaminated with radionuclides, particularly 137Cs and 90Sr, pose a long-term radiation hazard to human health through exposure via the foodchain and other pathways. Remediation of radionuclide-contaminated soils has become increasingly important. Removal of the contaminated surface soil (often up to 40 cm) or immobilization of radionuclides in soils by applying mineral and chemical amendments are physically difficult and not likely cost-effective in practicality. Reducing plant uptake of radionuclides, especially 137CS and 90Sr by competitive cations contained in chemical fertilizers has the general advantage in large scale, low-level contamination incidents on arable land, and has been widely practiced in central and Western Europe after the Chernobyl accident. Phytoextraction of radionuclides by specific plant species from contaminated sites has rapidly stimulated interest among industrialists as well as academics, and is considered to be a promising bio-remediation method. This paper examines the existing remediation approaches and discusses phytoextraction of radionuclides from contaminated soils in detail.  相似文献   

4.
Natural colloids in groundwater could facilitate radionuclide transport, provided the colloids are mobile, are present in sufficient concentrations and can adsorb radionuclides. This paper describes the results of a laboratory migration study carried out with combinations of radionuclides and natural colloids within a fracture in a large granite block to experimentally determine the impact of colloids on radionuclide transport. The 85Sr used in this study is an example of a moderately sorbing radionuclide, while the 241Am is typical of a strongly sorbed radionuclide with very low solubility. The natural colloids used in this study were isolated from granite groundwater from Atomic Energy of Canada (AECL) Underground Research Laboratory (URL), and consisted of mostly 1-10 nm organic colloids, along with lesser amounts of 10-450 nm colloids (organics and aluminosilicates). The measured coefficients for radionuclide sorption onto these colloids were between 3 x 10(2) and 1 x 10(3) ml/g for 85Sr, and between 7 x 10(4) and 7 x 10(5) mg/l for 241Am. The 85Sr sorption on the natural colloids appeared to be reversible. Migration experiments in the granite block were carried out by establishing a flow field between two boreholes (out of a total of nine) intersecting a main horizontal fracture. These experiments showed that dissolved 85Sr behaved as a moderately sorbing tracer, while dissolved 241Am was completely adsorbed by the fracture surfaces and showed no evidence of transport. However, when natural colloids were injected together with dissolved 241Am, a small amount of 241Am transport was observed, demonstrating the ability of natural colloids to facilitate the transport of radionuclides with low solubility. Natural colloids had only a minor effect on the transport of 85Sr. In a separate experiment to test the effect of higher colloid concentrations on 85Sr migration, synthetic colloids were produced from Avonlea bentonite. The introduction of a relatively high concentration of bentonite colloids actually reduced 85Sr transport because, compared to natural colloids, the bentonite colloids were less mobile and they sorbed 85Sr more strongly.  相似文献   

5.
Contamination of the environment by radionuclides is usually estimated using soil and grass sampling. However, radionuclides are often not homogeneously distributed in soils. In the alpine Mercantour region (Western Alps, France) a large heterogeneity in Chernobyl 137Cs deposition has been previously observed. Here we report additional 137Cs results together with new 90Sr and Pu data for soil, grass, milk, and cheese samples. The results show that radioisotopes from nuclear weapons tests fallout are more homogeneously distributed than Chernobyl 137Cs. Further, we observe that the 137Cs and 90Sr contents are less variable in milk samples than in grass or soil samples. This can be attributed to the homogenization effect of cow vagrancy during grazing. Hence milk seems to be a more robust sample than soil or grass to evaluate the extent of contamination on a regional scale. We explore this idea by comparing own unpublished 90Sr results and 90Sr results from the literature to establish the relationship between altitude of grazing and contamination of soil and milk for Western Europe. There is a significant positive correlation between soil contamination and altitude and an even closer correlation between milk 90Sr activity (A) and altitude (h): A = A0 + e(k x h) where A0 is the expected activity of milk sampled at sea level (A0 = 0.064 +/- 0.014 Bq g(-1) Ca) and h is the altitude of grazing, k being a constant (k = 0.95 x 10(-3) +/- 0.11 x 10(-3) m(-1) Bq g(-1) Ca). The fact that there is less scattering in the relationship for the 90Sr(milk)-altitude than for 90Sr(soil)-altitude suggests, again, that milk is a well-suited sample for environmental survey. The relationship between the altitude of grazing and the 90Sr content of milk and cheese can also be used to assess the authenticity of dairy products.  相似文献   

6.
Microorganisms play an important role in the fixation of radionuclides in forest soils. In particular, fungi have the capacity to absorb and translocate radionuclides. The role of the ectomycorrhizal fungus Hebeloma crustuliniforme in the uptake of radiocaesium (134Cs) and radiostrontium (85Sr) into seedlings of Norway spruce (Picea abies) was investigated in a pouch test system. Inoculated and non-inoculated seedlings; seedlings inoculated during 8 and 15 weeks; seedlings exposed during 2 and 3 weeks to the radioactive solution; and seedlings grown under low and high ammonium conditions prior to the application of the radionuclides were compared. The final 134Cs and 85Sr activity was determined in fine-roots, main-roots, stems and needles. The results showed that ectomycorrhizae reduced the uptake of 134Cs and 85Sr. The degree of ectomycorrhization was of crucial importance and seemed to be governed by the period during which ectomycorrhizae were allowed to develop and by the ammonium concentration in the nutrient solution. The radionuclide uptake increased with increasing exposure time. Both radionuclides were predominantly accumulated in fine-roots. However, needles proved to describe best the result of net root uptake and translocation to the shoot. The uptake-and and translocation-rates of 85Sr were smaller than those of 134Cs. It is assumed that the translocation is coupled with the intensity of water fluxes through the xylem and that 85Sr is more readily adsorbed into mycelium or plant tissue relative to 134Cs. The effect of high ammonium growth conditions was overcome by the effect of ectomycorrhization, except in needles with a very large biomass which behaved as a strong sink and led to a high accumulation of 134Cs.  相似文献   

7.
The results of seven years lysimeter experiments to determine the uptake of 60Co, 137Cs and 226Ra into agricultural crops (endive, maize, wheat, mustard, sugarbeet, potato, Faba bean, rye grass) are described. The lysimeter consists of twelve monolithic soil profiles (four soil types and three replicates) and is located in Seibersdorf/Austria, a region with a pannonian climate (pronounced differences between hot and semi-arid summers and humid winter conditions, annual mean of precipitation: 517 mm, mean annual temperature: 9.8 degrees C). Besides soil-to-plant transfer factors (TF), fluxes were calculated taking into account biomass production and growth time. Total median values of TF's (dry matter basis) for the three radionuclides decreased from 226Ra (0.068 kg kg(-1)) to 137Cs (0.043 kg kg(-1)) and 60Co (0.018 kg kg(-1)); flux values exhibited the same ranking. The varying physical and chemical properties of the four experimental soils resulted in statistically significant differences in transfer factors or fluxes between the investigated soils for 137Cs and 226Ra, but not for 60Co. Differences in transfer between plant species and plant parts are distinct, with graminaceous species showing, on average, TF values 5.8 and 15 times lower than dicotyledonous species for 137Cs and 60Co, respectively. This pattern was not found for 226Ra. It can be concluded that 137Cs transfer is heavily influenced by soil characteristics, whilst the plant-specific factors are the main source of TF variability for 60Co. The variability of 226Ra transfer originates both from soil properties and plant species behaviour.  相似文献   

8.
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   

9.
The Peach Bottom Atomic Power Station (PBAPS) has contributed measurable quantities of radioactivity to Conowingo Reservoir, an impoundment of the lower Susquehanna River. As part of an ongoing radiological assessment program, concentrations of plant-related radionuclides in sediments have been monitored in spring and fall since 1980. Mass balance estimates derived from grab samples of surface sediments (< 10 cm) indicate that less than 20% of reactor released (60)Co, (65)Zn, (134)Cs and (137)Cs is present in these sediments. Significant seasonal variations in radionuclide trapping efficiency by the reservoir are not apparent. Deep core samples (c. 200 cm) confirm that some, but not all, of this surface sediment radionuclide inventory remains within the reservoir-trapped in discrete locations by subsequent sediment accumulation. The remaining radionuclide mass, in dissolved or particle-associated form, appears to be transported downstream, through Conowingo Dam, to upper Chesapeake Bay. The detection of PBAPS-derived radionuclides in the sediments of upper Chesapeake Bay, primarily the Susquehanna Flats, confirms the transport of these radionuclides from the lower Susquehanna River.  相似文献   

10.
The potential influence of earthworm activity on the mobility of radionuclides in soils and their subsequent availability for uptake by plants and transfer to higher trophic levels is briefly reviewed. The accumulation of caesium by the earthworm Aporrectodea longa from soil and from plant litter was investigated in laboratory experiments, as was the effect of reworking (through burrowing and ingestion) soil and soil with added organic material, on the extractability of caesium (ammonium acetate extraction). Soil was spiked with (134)Cs, organic matter with (137)Cs. In soil-fed worms, most of the radioactivity measured was eliminated with the gut contents; 5-25% of the ingested radioactivity was retained or assimilated. Loss of caesium from soil-fed worms followed a two component curve, with an initial rapid loss due to gut clearance (half-life of loss (Tb1/2) of about 0.2-0.6 days) and a slower loss of assimilated caesium (Tb1/2 of 15-26 days). Loss rates of assimilated caesium from worms fed on fragmented apple leaves were found to have half-lives of 18-54 days. Assimilation of caesium from apple leaves was higher than from soil, ranging from 55-100% of the activity measured before gut clearance. Dry weight transfer factors (concentration in worm tissue/concentration in substrate) for worms cleared of their gut contents were similar for the two substrates 0.04 and 0.04 for two loss experiments with worms fed on radioactive soil, and 0.03 and 0.05 for worms fed on apple leaves. After three months of reworking soil and soil/organic mixtures, A. longa was found to have no measurable effect on the extractable fraction of caesium. If earthworms have any subtle effects they were masked by changes in availability that occurred when the spiked soil and organic substrates were mixed together. Only about half of the extractable fraction in soil was recovered when soil was mixed with organic material suggesting that some of the labile fraction in soil had become complexed with organic material. This exchange occurred in substrate mixtures with and without worms. The limitation of chemical extraction procedures is discussed and suggestions for further work are presented.  相似文献   

11.
Oxalate and root exudates enhance the desorption of p,p'-DDT from soils   总被引:3,自引:0,他引:3  
Luo L  Zhang S  Shan XQ  Zhu YG 《Chemosphere》2006,63(8):1273-1279
The abiotic desorption of p,p'-DDT from seven Chinese soils spiked with p,p'-DDT and the effects of oxalate at 0.001-0.1M and the root exudates of maize, wheat, and ryegrass were evaluated using batch experiments. Soil organic carbon played a predominant role in the retention of DDT. Oxalate significantly increased the desorption of p,p'-DDT, with the largest increments ranging from 11% to 54% for different soils. Oxalate addition also resulted in the increased release of dissolved organic carbon and inorganic ions from soils. Root exudates had similar effects to those of oxalate. Root exudates significantly increased DDT desorption from the soils, and the general trend was similar among the plant species studied for all the soils (p > 0.05). Low molecular weight dissolved organic carbon amendments caused partial dissolution of the soil structure, such as the organo-mineral linkages, resulting in the release of organic carbon and metal ions and thus the subsequent enhanced desorption of DDT from the soils. The enhancing effects of oxalate and root exudates on DDT desorption were influenced by the contents of soil organic carbon and dissolved organic carbon in soils.  相似文献   

12.
The aim of this study was to explore how atmospherically derived soil pollution is affected by environmental processes at two typical boreal catchment landscape type settings: wetlands and forested areas. Measurements of hydrophobic organic compounds (HOCs) in forest soil and peat from an oligotrophic mire at various depths were performed at a remote boreal catchment in northern Sweden. HOCs in peat were evenly distributed throughout the body of the mire while levels of HOCs in the forest soil increased with increased amount of organic matter. Evaluation of HOC composition by principal component analysis (PCA) showed distinct differences between surface soils and deeper soil and peat samples. This was attributed to vertical transport, degradation and/or shifting sources over time. The calculated net vertical transport differed between surface layers (0.3%) and deeper soils (8.0%), suggesting that vertical transport conditions and processes differ in the deeper layers compared to the surface layers.  相似文献   

13.
The influence of dissolved humic substances on the transport of (4-chloro-2-methylphenoxy) acetic acid (MCPA) in a sandy soil with a low organic carbon content was studied in a column experiment. Soil columns were eluted with aqueous solutions containing different fractions of humic substances. More than 70% of the applied compound was found in the leachate in all sandy soil experiments, but distinct differences were obtained depending on the composition of the eluent. The addition of both humic and fulvic acids to the eluent affected the leaching behaviour of MCPA. While the presence of humic acids increased and accelerated the movement of MCPA in the investigated sandy soil, fulvic acids caused the opposite effect: increased retention was observed relative to the control. We concluded that a possible carrier transport or retention strongly depends on the composition of the dissolved organic matter. Thus, changes in the composition of dissolved organic matter may affect MCPA movement into deeper soil layers.  相似文献   

14.
Activity concentrations, inventories and activity ratios of 137Cs, 238Pu, 239?+?240Pu and 241Am in soil profiles were surveyed in the dry tundra and the adjoining proglacial zones of glaciers at a High Arctic site on Svalbard. Vertical profiles of radionuclide activities were determined in up to 14-cm-thick soil sequences. Additionally, soil properties (pH, organic matter, texture, mineral composition and sorption capacity) were analyzed. Results obtained in this study revealed a large range of activity concentrations and inventories of the fallout radionuclides from the undetectable to the uncommonly high levels (inventories of 30,900?±?940, 47?±?6, 886?±?80 and 296?±?19 Bq/m2 for 137Cs, 238Pu, 239?+?240Pu and 241Am, respectively) found in two profiles from the proglacial zone. Concentration of these initially airborne radionuclides in the proglacial zone soils is related to their accumulation in cryoconites that have a large ability to concentrate trace metals. The cryoconites develop on the surface of glaciers, and the material they accumulate is deposited on land surface after the glaciers retreat. The radionuclide inventories in the tundra soils, which effectively retain radionuclides due to high organic matter contents, were comparable to the global fallout deposition for this region of the world. The 238Pu/239?+?240Pu activity ratios for tundra soils suggested global fallout as the dominant source of Pu. The 238Pu/239?+?240Pu and 239?+?240Pu/137Cs activity ratios in the proglacial soils pointed to possible contributions of these radionuclides from other, unidentified sources.  相似文献   

15.
In the Ellen catchment on the Pinjarra Plain, NE of Perth in Western Australia, cadmium from fertilisers is starting to leach from soils. About 70% of surface soils in the Ellen catchment are sandy and often on top of a shallow ephemeral water table. Adsorption of Cd in the sandy soils of the Ellen catchment was studied by batch adsorption and by leaching small columns of soil. Adsorption of Cd increases linearly with increasing soil organic matter content and exponentially with increasing pH. Cadmium is significantly mobilised in the sandy soils by dissolved organic matter.The capacity of most of the sandy soils in the Ellen catchment to adsorb phosphate from fertiliser has been saturated. Resulting concentrations in Ellen Brook average 500 μg L−1 P. Cadmium is adsorbed more strongly in the sandy soils than phosphate and is just starting to leach into Ellen Brook. From a comparison of Cd/P ratios in water, soils and fertiliser, cadmium concentrations in Ellen Brook are estimated to be at 10–30% of their maximum for complete breakthrough from soils. Present concentrations of Cd in Ellen Brook average 0.1 μg L−1 and are estimated to approach the maximum for complete breakthrough in 100 yr. Maximum Cd concentrations in Ellen Brook could range from 0.6 to 2 μg L−1, depending on rates of input with fertiliser and future increases in agricultural land use in the catchment.Breakthrough curves, resulting from leaching Cd through small columns of sandy soil, indicate that adsorption significantly increases the effective hydrodynamic dispersion of Cd. Longitudinal dispersivities, measured at pore-water velocities of 0.7–14 m day−1, were 5 cm for Cd and 0.1–0.2 cm for chloride. The much greater dispersion of Cd in the sandy soils than of chloride is shown not to be caused by non-equilibrium adsorption.  相似文献   

16.
The influence of soil formation on copper sorption is documented based on chronosequences of soils from three river floodplains in Europe (Danube, Ebro and Elbe). Sequential extraction was used to fractionate copper in original and spiked soils in order to study the long-term and short-term behaviour of copper retention. Copper partitioning among defined geochemical fractions was mainly determined by soil pH and the contents of carbonates, organic matter and Fe-/Mn-oxides and hydroxides. Copper extracted with NH(2)OH.HCl correlated well with the contents of crystalline Fe-oxides and hydroxides, demonstrating increasing retention capacity with progressing soil development. Copper retained in original soils was found in more strongly bound fractions, whereas sorption of freshly added copper was primarily influenced by the presence of carbonates. Beyond the effect of progressing soil formation, variations in organic carbon contents due to different land use history affected the copper retention capacity of the investigated soils.  相似文献   

17.
The stability of TiO2 nanoparticles in soil suspensions and their transport behavior through saturated homogeneous soil columns were studied. The results showed that TiO2 could remain suspended in soil suspensions even after settling for 10 days. The suspended TiO2 contents in soil suspensions after 24 h were positively correlated with the dissolved organic carbon and clay content of the soils, but were negatively correlated with ionic strength, pH and zeta potential. In soils containing soil particles of relatively large diameters and lower solution ionic strengths, a significant portion of the TiO2 (18.8-83.0%) readily passed through the soils columns, while TiO2 was significantly retained by soils with higher clay contents and salinity. TiO2 aggregate sizes in the column outflow significantly increased after passing through the soil columns. The estimated transport distances of TiO2 in some soils ranged from 41.3 to 370 cm, indicating potential environmental risk of TiO2 nanoparticles to deep soil layers.  相似文献   

18.
One of the dominant tree species growing within and around the eastern portion of Los Alamos National Laboratory (LANL), Los Alamos, NM, lands is the pinon pine (Pinus edulis). Pinon pine is used for firewood, fence posts, and building materials and is a source of nuts for food--the seeds are consumed by a wide variety of animals and are also gathered by people in the area and eaten raw or roasted. This study investigated the (1) concentration of 3H, 137Cs, 90Sr, totU, 238Pu, 239,240Pu, and 241Am in soils (0- to 12-in. [31 cm] depth underneath the tree), pinon pine shoots (PPS), and pinon pine nuts (PPN) collected from LANL lands and regional background (BG) locations, (2) committed effective dose equivalent (CEDE) from the ingestion of nuts, and (3) soil to PPS to PPN concentration ratios (CRs). Most radionuclides, with the exception of 3H in soils, were not significantly higher (p < 0.10) in soils, PPS, and PPN collected from LANL as compared to BG locations, and concentrations of most radionuclides in PPN fromLANL have decreased over time. The maximum net CEDE (the CEDE plus two sigma minus BG) at the most conservative ingestion rate (10 lb [4.5 kg]) was 0.0018 mrem (0.018 microSv); this is far below the International Commission on Radiological Protection (all pathway) permissible dose limit of 100 mrem (1000 microSv). Soil-to-nut CRs for most radionuclides were within the range of default values in the literature for common fruits and vegetables.  相似文献   

19.
Rate limited processes including kinetic adsorption-desorption can greatly impact the fate and behavior of toxic arsenic compounds in heterogeneous soils. In this study, miscible displacement column experiments were carried out to investigate the extent of reactivity during transport of arsenite in soils. Arsenite breakthrough curves (BTCs) of Olivier and Windsor soils exhibited strong retardation with diffusive effluent fronts followed by slow release or tailing during leaching. Such behavior is indicative of the dominance of kinetic retention reactions for arsenite transport in the soil columns. Sharp decrease or increase in arsenite concentration in response to flow interruptions (stop-flow) further verified that non-equilibrium conditions are dominant. After some 40-60 pore volumes of continued leaching, 30-70% of the applied arsenite was retained by the soil in the columns. Furthermore, continued arsenite slow release for months was evident by the high levels of residual arsenite concentrations observed during leaching. In contrast, arsenite transport in a reference sand material exhibited no retention where complete mass recovery in the effluent solution was attained. A second-order model (SOM) which accounts for equilibrium, reversible, and irreversible retention mechanisms was utilized to describe arsenite transport results from the soil columns. Based on inverse and predictive modeling results, the SOM model successfully depicted arsenite BTCs from several soil columns. Based on inverse and predictive modeling results, a second-order model which accounts for kinetic reversible and irreversible reactions is recommended for describing arsenite transport in soils.  相似文献   

20.
Radionuclide levels in vegetation from a High Arctic location were studied and compared to in situ soil concentrations. Levels of the anthropogenic radionuclide 137Cs and the natural radionuclides 40K, 238U, 226Ra and 232Th are discussed and transfer factor (TF) values and aggregated transfer (Tag) values are calculated for vascular plants. Levels of 137Cs in vegetation generally followed the order mosses > lichen > vascular plants. The uptake of 137Cs in vascular plants showed an inverse relationship with the uptake of 40K, with 137Cs TF and Tag values generally higher than 40K TF and Tag values. 40K activity concentrations in all vegetation showed little correlation to associated soil concentrations, while the uptake of 238U, 226Ra and 232Th by vascular and non-vascular plants was generally low.  相似文献   

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