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1.
Hematite, a type of inorganic-sorptive medium, was used for the removal of U (VI) from aqueous solutions. Variables of the batch experiments including solution pH, contact time, initial concentration, temperature, calcium and magnesium ions were studied. The results indicated that the adsorption capacities are strongly affected by the solution pH, contact time and initial concentration. A higher pH favors higher U (VI) removal. The adsorption was also affected by temperature and calcium and magnesium ions, but the effect is very weak. The maximum adsorption capacity (qm) only increased from 3.36 mg g−1 to 3.54 mg g−1 when the temperature was increased from 293 K to 318 K. A two-stage kinetic behavior was observed in the adsorption of uranium (VI): very rapid initial adsorption in a few minutes, followed by a long period of slower uptake. It was found that an increase in temperature resulted in a higher uranium (VI) loading per unit weight of the sorbent. The adsorption of uranium by hematite had good efficiency, and the equilibrium time of adsorbing uranium (VI) was about 6 h. The isothermal data were fitted with both Langmuir and Freundlich equations, but the data fitted the former better than the latter. The pseudo-first-order kinetic model, pseudo-second-order kinetic model and intraparticle diffusion model were used to describe the kinetic data, but the pseudo-second-order kinetic model was the best. The thermodynamic parameter ΔG0 were calculated, the negative ΔG0 values of uranium (VI) at different temperatures confirmed the adsorption processes were spontaneous.  相似文献   

2.
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.  相似文献   

3.
The effect of the matrix composition (main constituents) on the concentration and chemical behavior of uranium in phosphogypsum stack solutions and leachates has been investigated. Solid and aqueous samples were taken from three different sub-areas of a phosphogypsum stack at a coastal area in Vasilikos (Cyprus). The sub-areas are characterized whether by their acidity (e.g. "aged" and "non-aged" phosphogypsum) or by their salt content, originating from pulping water during wet stacking or (after deposition) from the adjacent sea. Measurements in stack solutions and leachates showed that phosphogypsum characteristics affect both, the concentration and the chemical behavior of uranium in solution. Uranium concentration in solutions of increased salinity is up to three orders of magnitude higher than in solutions of low salinity and this is attributed to the effect of ionic strength on the solubility of phosphogypsum. Modelling showed that uranium in stack solutions is predominantly present in the form of uranium(VI) phosphate complexes (e.g. UO(2)(H(2)PO(4))(2), UO(2)HPO(4)), whereas in leachates uranium(VI) fluoro complexes (e.g. UO(2)F(2), UO(2)F(3)(-)) are predominant in solution. The latter indicates that elution of uranium from phosphogypsum takes places most probably in the form of fluoro complexes. Both, effective elution by saline water and direct migration of uranium to the sea, where it forms very stable uranium(VI) carbonato complexes, indicate that the adjacent sea will be the final receptor of uranium released from Vasilikos phosphogypsum.  相似文献   

4.
Biosorption of uranium (VI) ions by immobilized Aspergillus fumigatus beads was investigated in a batch system. The influences of solution pH, biosorbent dose, U (VI) concentration, and contact time on U (VI) biosorption were studied. The results indicated that the adsorption capacity was strongly affected by the solution pH, the biosorbent dose and initial U (VI) concentration. Optimum biosorption was observed at pH 5.0, biosrobent dose (w/v) 2.5%, initial U (VI) concentration 60 mg L−1. Biosorption equilibrium was established in 120 min. The adsorption process conformed to the Freunlich and Temkin isothermal adsorption models. The dynamic adsorption model conformed to pseudo-second order model.  相似文献   

5.
The amine-modified polyhydroxyethylmethacrylate (poly(HEMA))-grafted biomaterial (tamarind fruit shell, TFS) carrying carboxyl functional groups at the chain end (PGTFS-COOH) was prepared and used as an adsorbent for the removal of uranium(VI) from water and nuclear industry wastewater. FTIR spectral analysis revealed that U(VI) ions and PGTFS-COOH formed a chelate complex. The adsorption process was relatively fast, requiring only 120 min to attain equilibrium. The adsorption kinetic data were best described by the pseudo-second-order equation. The equilibrium adsorption data were correlated with the Sips isotherm model. The maximum U(VI) ions uptake with PGTFS-COOH was estimated to be 100.79 mg/g. The complete removal of 10 mg/L U(VI) from simulated nuclear industry wastewater was achieved by 3.5 g/L PGTFS-COOH. The reusability of the adsorbent was demonstrated over 4 cycles using NaCl (1.0 M) + HCl (0.5 M) solution mixture to de-extract the U(VI). The results show that the PGTFS-COOH tested is very promising for the recovery of U(VI) from water and wastewater.  相似文献   

6.
The accumulations of both natural (U) and depleted (DU) uranium in the earthworms (Eisenia fetida) were studied to evaluate corresponding biological effects. Concentrations of metals in the experimental soil ranged from 1.86 to 600 mg kg−1. Five biological endpoints: mortality, animals’ weight increasing, lysosomal membrane stability by measuring the neutral red retention time (the NRRT), histological changes and genetic effects (Comet assay) were used to evaluate biological effects in the earthworms after 7 and 28 days of exposure. No effects have been observed in terms of mortality or weight reduction. Cytotoxic and genetic effects were identified at quite low U concentrations. For some of these endpoints, in particular for genetic effects, the dose (U concentration)-effect relationships have been found to be non-linear. The results have also shown a statistically significant higher level of impact on the earthworms exposed to natural U compared to depleted U.  相似文献   

7.
Phosphogypsum is a waste by-product of the phosphate fertilizer industry, which is usually disposed in the environment because of its restricted use in industrial applications. Physico-chemical conditions existing in stack fluids and leachates are of major importance and determine solubility and redox stability of phosphogypsum, as well as radionuclide release from stacks to terrestrial environments. The aim of this study is to assess the effect of key parameters (e.g. ionic strength, temperature, pH) on the solubility of phosphogypsum. Phosphogypsum sampling and in-situ measurements were carried out at a coastal stack in Cyprus, solubility experiments were performed in simulated laboratory systems and thermodynamic calculations by means of MINTEQA2, an equilibrium speciation model. Generally, increasing ionic strength and temperature leads to increased phosphogypsum solubility, with the former being much more effective. The increased solubility of phosphogypsum in saline solutions is attributed solely to ionic strength effects on the activity of ionic species in solution and no solid phase transformations could be observed. The effect of pH on phosphogypsum solubility seems to be insignificant at least in a pH range between 4 and 8. Regarding uranium levels, there is a strong correlation between salinity and uranium concentration and linear correlation between phosphogypsum solubility and uranium levels in stack solutions, indicating the incorporation of uranium into the gypsum lattice and the formation of a solid solution.  相似文献   

8.
Impact of water quality parameters on the sorption of U(VI) onto hematite   总被引:2,自引:0,他引:2  
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.  相似文献   

9.
Hydroponicaly cultivated plants were grown on medium containing uranium. The appropriate concentrations of uranium for the experiments were selected on the basis of a standard ecotoxicity test. The most sensitive plant species was determined to be Lactuca sativa with an EC50 value about 0.1 mM. Cucumis sativa represented the most resistant plant to uranium (EC50 = 0.71 mM). Therefore, we used the uranium in a concentration range from 0.1 to 1 mM.Twenty different plant species were tested in hydroponic solution supplemented by 0.1 mM or 0.5 mM uranium concentration. The uranium accumulation of these plants varied from 0.16 mg/g DW to 0.011 mg/g DW. The highest uranium uptake was determined for Zea mays and the lowest for Arabidopsis thaliana. The amount of accumulated uranium was strongly influenced by uranium concentration in the cultivation medium. Autoradiography showed that uranium is mainly localized in the root system of the plants tested. Additional experiments demonstrated the possibility of influencing the uranium uptake from the cultivation medium by amendments. Tartaric acid was able to increase uranium uptake by Brassica oleracea and Sinapis alba up to 2.8 times or 1.9 times, respectively. Phosphate deficiency increased uranium uptake up to 4.5 times or 3.9 times, respectively, by Brassica oleracea and S. alba. In the case of deficiency of iron or presence of cadmium ions we did not find any increase in uranium accumulation.  相似文献   

10.
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.  相似文献   

11.
Concentrations of the natural radionuclides 238U, 226Ra, 232Th and 40K have been measured by γ-ray spectrometry in 796 topsoil samples from the Pearl River Delta Zone (PRDZ) of Guangdong, China. The mean concentrations for 238U, 226Ra, 232Th and 40K were found to be 140 ± 37 Bq kg−1, 134 ± 41 Bq kg−1, 187 ± 80 Bq kg−1 and 680 ± 203 Bq kg−1 dry mass, respectively. These values were all higher than the mean values in soil for China and the world. Outdoor air-absorbed dose rates, calculated from activity concentrations of 226Ra, 232Th and 40K, ranged from 86 to 237 nGy h−1, with a mean value of 165 ± 46 nGy h−1. The corresponding annual outdoor effective dose rate per person was estimated to be between 0.11 and 0.29 mSv y−1, with a mean value of 0.20 ± 0.06 mSv y−1, which was also higher than the world mean value of 0.07 mSv y−1. The radium equivalent activity (Raeq) and the external hazard index (Ir) resulted from the natural radionuclides in soil, were also calculated and found to vary from 230 to 676 Bq kg−1 and from 0.6 to 1.8, respectively. The Raeq and the Ir in all the investigated regions were up to 75% higher than the set limits of 370 Bq kg−1 and 1.0, respectively.  相似文献   

12.
In order to evaluate the influence of faulting on the variability of geogenic radon at detailed scale (1:2000), data on gamma ray fluxes, U and Th concentrations in rocks, radon in soil-gas and radon in groundwater were collected in three target areas on the Oliveira do Hospital region (Central Portugal). This region stands on the Iberian Uranium Province, and is dominantly composed of Hercynian granites and metasedimentary rocks of pre-Ordovician age, crosscut by faults with dominant strike N35°E, N55°E and N75°E. Radiometric anomalies are frequent, associated with faults of the referred systems and metasedimentary enclaves; the analytical data confirms that these anomalies are produced by local high uranium contents in rocks and fault-filling materials (n = 34, range 13-724 ppm), while other radiogenic elements are relatively constant (e.g. Th 4-30 ppm). Radon concentration in soil can be extremely high, up to 12,850 kBq m−3 (n = 215), with a large proportion of results above 100 kBq m−3. Unsurprisingly, groundwater also shows high radon concentrations, with observed values in the range 150-4850 Bq.L−1 (n = 17). From the results it is concluded that metasedimentary enclaves, as well as faults, can accumulate uranium from circulating fluids, and as a consequence, strongly locally enhance geogenic radon potential. Due to this fact, for the purpose of land use planning in such uranium-enriched regions, very detailed geological mapping is needed to precisely recognize radon high risk areas. A correlation between radon concentration in soil or in groundwater and gamma ray fluxes was established pointing to the possible use of these fluxes as a first step in assessing geogenic radon potential, at least to geological setting similar to the study area.  相似文献   

13.
Adsorption of radionuclides on soils and sediments is commonly quantified by distribution coefficients (Kd values). This paper examines the relationship between Kd values for uranium(VI) adsorption and the specific surface area (SSA) of geologic materials. We then investigate the potential applicability of normalising uranium (U) Kd measurements using the SSA, to produce ‘Ka values’ as a generic expression of the affinity of U for the surface. The data for U provide a reasonably coherent set of Ka values on various solid phases, both with and without ligands. The Ka 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 Ka 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 Ka values should be interpreted cautiously.  相似文献   

14.
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.  相似文献   

15.
The uptake of plutonium(VI) and uranium(VI) by lichen biomass was studied in the foliose lichen Parmotrema tinctorum to elucidate the migration behavior of Pu and U in the terrestrial environment. Pu and U uptake by P. tinctorum averaged 0.040+/-0.010 and 0.055+/-0.015 g gdry (-1), respectively, after 96 h incubation with 4.0 x 10(14) mol 1(-1) Pu solutions of pH 3, 4 and 5. SEM observations showed that the accumulated Pu is evenly distributed on the upper and lower surfaces of P. tinctorum, in contrast to U(VI), which accumulated in both cortical and medullary layers. UV/VIS absorption spectroscopy demonstrates that a fraction of Pu(VI) in the solution is reduced to Pu(V) by the organic substances released from P. tinctorum, and the accumulated Pu on the surface is reduced to Pu(IV), while U(VI) keeps the oxidation state of VI. Since the solubility of Pu(IV) hydroxides is very low, reduced Pu(VI) does not penetrate to the medullary layers, but is probably precipitated as Pu(IV) hydroxides on the cortical lichen surface. It is concluded that the uptake and reduction of Pu(VI) by lichens is important to determine the mobilization and oxidation states of Pu in the terrestrial environment.  相似文献   

16.
New data are reported on the concentrations, isotopic composition and speciation of americium, plutonium and uranium in surface and ground waters in the Sarzhal region of the Semipalatinsk Test Site, and an adjacent area including the settlement of Sarzhal. The data relate to filtered water and suspended particulate from (a) streams originating in the Degelen Mountains, (b) the Tel′kem 1 and Tel′kem 2 atomic craters, and (c) wells on farms located within the study area and at Sarzhal. The measurements show that 241Am, 239,240Pu and 238U concentrations in well waters within the study area are in the range 0.04–87 mBq dm−3, 0.7–99 mBq dm−3, and 74–213 mBq dm−3, respectively, and for 241Am and 239,240Pu are elevated above the levels expected solely on the basis of global fallout. Concentrations in streams sourced in the Degelen Mountains are similar, while concentrations in the two water-filled atomic craters are somewhat higher. Suspended particulate concentrations in well waters vary considerably, though median values are very low, at 0.01 mBq dm−3, 0.08 mBq dm−3 and 0.32 mBq dm−3 for 241Am, 239,240Pu and 238U, respectively. The 235U/238U isotopic ratio in almost all well and stream waters is slightly elevated above the ‘best estimate’ value for natural uranium worldwide, suggesting that some of the uranium in these waters is of test-site provenance. Redox analysis shows that on average most of the plutonium present in the microfiltered fraction of these waters is in a chemically reduced form (mean 69%; 95% confidence interval 53–85%). In the case of the atomic craters, the proportion is even higher. As expected, all of the americium present appears to be in a reduced form. Calculations suggest that annual committed effective doses to individual adults arising from the daily ingestion of these well waters are in the range 11–42 μSv (mean 21 μSv). Presently, the ground water feeding these wells would not appear to be contaminated with radioactivity from past underground testing in the Degelen Mountains or from the Tel′kem explosions.  相似文献   

17.
Compared to agricultural lands, forests are complex ecosystems as they can involve diverse plant species associations, several vegetative strata (overstorey, shrubs, herbaceous and other annual plant layer) and multi-layered soil profiles (forest floor, hemi-organic and mineral layers). A high degree of variability is thus generally observed in radionuclide transfers and redistribution patterns in contaminated forests. In the long term, the soil compartment represents the major reservoir of radionuclides which can give rise to long-term plant and hence food contamination. For practical reasons, the contamination of various specific forest products has commonly been quantified using the aggregated transfer factor (Tag in m2 kg−1) which integrates various environmental parameters including soil and plant type, root distribution as well as nature and vertical distribution of the deposits. Long lasting availability of some radionuclides was shown to be the source of much higher transfer in forest ecosystems than in agricultural lands. This study aimed at reviewing the most relevant quantitative information on radionuclide transfers to forest biota including trees, understorey vegetation, mushrooms, berries and game animals. For both radiocaesium and radiostrontium in trees, the order of magnitude of mean Tag values was 10−3 m2 kg−1 (dry weight). Tree foliage was usually 2–12 times more contaminated than trunk wood. Maximum contamination of tree components with radiocaesium was associated with (semi-)hydromorphic areas with thick humus layers. The transfer of radionuclides to mushrooms and berries is high, in comparison with foodstuffs grown in agricultural systems. Concerning caesium uptake by mushrooms, the transfer is characterized by a very large variability of Tag, from 10−3 to 101 m2 kg−1 (dry weight). For berries, typical values are around 0.01–0.1 m2 kg−1 (dry weight). Transfer of radioactive caesium to game animals and reindeer and the rate of activity reduction, quantified as an ecological half-life, reflect the soil and pasture conditions at individual locations. Forests in temperate and boreal regions differ with respect to soil type and vegetation, and a faster decline of muscle activity concentrations in deer occurs in the temperate zone. However, in wild boar the caesium activity concentration shows no decline because of its special feeding habits. In the late phase, i.e. at least a few months since the external radionuclide contamination on feed plants has been removed, a Tag value of 0.01 m2 kg−1 (fresh weight) is common for 137Cs in the muscles of adult moose and terrestrial birds living in boreal forests, and 0.03 m2 kg−1 (fresh weight) for arctic hare. Radiocaesium concentrations in reindeer muscle in winter may exceed the summer content by a factor of more than two, the mean Tag values for winter ranging from 0.02 to 0.8 m2 kg−1 (fresh weight), and in summer from 0.04 to 0.4 m2 kg−1. The highest values are found in the year of initial contamination, followed by a gradual reduction. In waterfowl a relatively fast decline in uptake of 137Cs has been found, with Tag values changing from 0.01 to 0.002 m2 kg−1 (fresh weight) in the three years after the contaminating event, the rate being determined by the dynamics of 137Cs in aquatic ecosystems.  相似文献   

18.
Vegetables grown with phosphate fertilizer (conventional management), with bovine manure fertilization (organic management) and in a mineral nutrient solution (hydroponic) were analyzed and the concentrations of 238U, 226Ra and 228Ra in lettuce, carrots, and beans were compared. Lettuce from hydroponic farming system showed the lowest concentration of radionuclides 0.51 for 226Ra, 0.55 for 228Ra and 0.24 for 238U (Bq kg−1 dry). Vegetables from organically and conventionally grown farming systems showed no differences in the concentration of radium and uranium. Relationships between uranium content in plants and exchangeable Ca and Mg in soil were found, whereas Ra in vegetables was inversely correlated to the cation exchange capacity of soil, leading to the assumption that by supplying carbonate and cations to soil, liming may cause an increase of U and a decrease of radium uptake by plants. The soil to plant transfer varied from 10−4 to 10−2 for 238U and from 10−2 to 10−1 for 228Ra.  相似文献   

19.
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 (CDGT) 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.  相似文献   

20.
Accumulation and distribution of uranium in roots and shoots of four plants species differing in their cation exchange capacity of roots (CECR) was investigated. After exposure in hydroponics for seven days to 100 μmol U L−1, distribution of uranium in roots was investigated through chemical extraction of roots. Higher U concentrations were measured in roots of dicots which showed a higher CECR than monocot species. Chemical extractions indicated that uranium is mostly located in the apoplasm of roots of monocots but that it is predominantly located in the symplasm of roots of dicots. Translocation of U to shoot was not significantly affected by the CECR or distribution of U between symplasm and apoplasm. Distribution of uranium in roots was investigated through chemical extraction of roots for all species. Additionally, longitudinal and radial distribution of U in roots of maize and Indian mustard, respectively showing the lowest and the highest translocation, was studied following X-ray fluorescence (XRF) analysis of specific root sections. Chemical analysis and XRF analysis of roots of maize and Indian mustard clearly indicated a higher longitudinal and radial transport of uranium in roots of Indian mustard than in roots of maize, where uranium mostly accumulated in root tips. These results showed that even if CECR could partly explain U accumulation in roots, other mechanisms like radial and longitudinal transport are implied in the translocation of U to the shoot.  相似文献   

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