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1.
The objective of this research was to assess the degradation of fipronil [5-amino-1-(2,6-dichloro-alpha,alpha,alpha -trifluoro-p-tolyl)-4-trifluoromethylsulfinylpyrazole-3-carbonitrile] in soils from sugar cane fields in Northeastern Brazil. Degradation experiments were carried out under laboratory conditions (controlled temperature and in the dark), where sterile and non-sterile soils (Ustoxs) were incubated [under moisture content of 55% of the water holding capacity (WHC)] and analyzed for fipronil disappearance and metabolite formation. Microbial communities present in the soil degrade fipronil. However, biodegradation seems to be dependent on the bioavailability of the fipronil and the half-life according to the zero-order model. Fipronil degradation rate appeared to be biphasic. Degradation fipronil ranged from 83 days (initial concentration = 978 ng g(-1); short-term experiment) to 200 days (initial concentration = 689 ng g(-1); long-term experiment). This an initial slower rate followed by a faster rate after 90 days of incubation may lead to shorter half-life than that calculated with the zero-order model. The sulfone derivative (an oxidation product) was the predominant metabolite, but the sulfide (a reduction product) and amide (a hydrolysis product) derivatives were also formed under non-sterile conditions after 120 days of incubation. The metabolites underwent further biodegradation, particularly the sulfone derivative. Bioavailability appears to affect fipronil degradation in soils with an effective capacity to adsorb fipronil (such as Ustoxs), while redox potential was important for the formation of metabolites. Despite the fine texture, more aerobic sites were present, thus favoring the formation of the sulfone metabolite over that of the sulfide metabolite. Therefore, microaggregation of Ustoxs, with high clay content, played a very important role in determining the types of metabolites formed.  相似文献   

2.
The objective of this research was to assess the degradation of fipronil [5-amino-1-(2,6-dichloro-α,α,α -trifluoro-p-tolyl)-4-trifluoromethylsulfinylpyrazole-3-carbonitrile] in soils from sugar cane fields in Northeastern Brazil. Degradation experiments were carried out under laboratory conditions (controlled temperature and in the dark), where sterile and non-sterile soils (Ustoxs) were incubated [under moisture content of 55% of the water holding capacity (WHC)] and analyzed for fipronil disappearance and metabolite formation. Microbial communities present in the soil degrade fipronil. However, biodegradation seems to be dependent on the bioavailability of the fipronil and the half-life according to the zero-order model. Fipronil degradation rate appeared to be biphasic. Degradation fipronil ranged from 83 days (initial concentration = 978 ng g? 1; short-term experiment) to 200 days (initial concentration = 689 ng g? 1; long-term experiment). This an initial slower rate followed by a faster rate after 90 days of incubation may lead to shorter half-life than that calculated with the zero-order model. The sulfone derivative (an oxidation product) was the predominant metabolite, but the sulfide (a reduction product) and amide (a hydrolysis product) derivatives were also formed under non-sterile conditions after 120 days of incubation. The metabolites underwent further biodegradation, particularly the sulfone derivative. Bioavailability appears to affect fipronil degradation in soils with an effective capacity to adsorb fipronil (such as Ustoxs), while redox potential was important for the formation of metabolites. Despite the fine texture, more aerobic sites were present, thus favoring the formation of the sulfone metabolite over that of the sulfide metabolite. Therefore, microaggregation of Ustoxs, with high clay content, played a very important role in determining the types of metabolites formed.  相似文献   

3.
The fumigant 1,3-dichloropropene (1,3-D) is considered a major replacement to methyl bromide, which is to be phased out of use in the United States by 2005. The main purpose of this study was to evaluate soil-water partitioning of 1,3-D in two California agricultural soils (Salinas clay loam and Arlington sandy loam). The partition coefficients (Kd and Kf) were determined by directly measuring the concentration of 1,3-D in the solid phase (Cs) and aqueous phase (Cw) after batch equilibration. In the Salinas clay loam, the Kf of cis-1,3-D in adsorption and desorption isotherms was 0.47 and 0.54, respectively, with respective values of 0.39 and 0.49 for trans-1,3-D. This slight hysteric effect suggests that a different range of forces are involved in the adsorption and desorption process. Since n was near unity in the Freundlich equation, the Freundlich isotherms can also be approximated using the liner isotherm. At 25 degrees C, the Kd of the 1,3-D isomers in both soils ranged from 0.46 to 0.56, and the Koc (organic matter partition coefficient) ranged from 58 to 70. The relatively low Kd values and a Koc that falls within the range of 50-150, suggests that 1,3-D is weakly sorbed and highly mobile in these soils. Understanding the sorption behavior of 1,3-D in soil is important when developing fumigation practices to reduce the movement of 1,3-D to the air and groundwater.  相似文献   

4.
This article reports on methabenzthiazuron [1-(1,3-benzothiazol-2-yl)-1,3-dimethylurea] (MBT) adsorption process on six agricultural allophanic and nonallophanic soils. The effect of amendment with exogenous organic matter was also studied. Adsorption kinetic fits an hyperbolic model. MBT adsorption reached an apparent equilibrium within 2 h and followed a second-order reaction. The maximum adsorbed amounts for natural soils ranged from 32 to 145 microg g(-1). Rate constants were considered relatively low (0.27-1.5 x 10(-4) [microg g(-1)](1-n) s-1); the slow process was attributed to a combined effect of difussion and adsorption. MBT adsorption fits the Freundlich model with r values > or =0.998 at P < or = 0.001 significance levels. Kf and Freundlich exponents (l/n) ranged from 5.3 to 82.1 cm3 g(-1) and from 0.66 to 0.73, respectively. Kf values for soils with a low organic matter content were lower than that obtained from the only typical allophanic soil derived from volcanic ash under study. Lineal regression analysis between Kf and organic matter content of nonallophanic soils gave a correlation coefficient of 0.980 (P = 0.02). Dispersion of Kd values together with close values of K(OM) indicate that organic matter (OM) was the principal component responsible for MBT adsorption in unamended soils. Addition of peat decreased soil pH and increased adsorption capacity for allophanic and nonallophanic soils. Kinetic experiments showed enhancements of Xmax values and lower rate constants.  相似文献   

5.
The objectives of this study were to assess sorption and desorption of tylosin, a macrolide antimicrobial chemical used in swine, cattle, and poultry production, in three silty clay loam soils of South Dakota and compare soil sorption to sand and manure sorption. The silty clay loam soils, from a toposequence in eastern South Dakota, standardized sand samples, and swine manure were used in 24-h batch sorption studies with tylosin concentrations ranging from 25 to 232 micro mole/L. Desorption from soil was conducted over a four-day period. Partition coefficients, based on the Freundlich isotherm (K(f)) or K(d) values, were calculated. K(f) values for the silty clay loams were similar, not influenced by landscape position, and averaged 1,350 with isotherm slopes ranging from 0.85 to 0.93. K(f) values for sand were dependent on solution/sand ratios and pH, ranging from 1.4 to 25.1. K(d) values of manure were dependent on the solution type and ranged from 840 L/kg with urine to about 175 L/kg when sorbed from water. Desorption of tylosin from each soil over the four-day period was < 0.2% of the amount added. The soils' high K(f) values and low desorption amounts suggest that once tylosin is in these soils, leaching to lower depths may not occur. However, this does not preclude runoff with soil eroded particles. If tylosin reaches a sand aquifer, through bypass flow or other mechanism(s), movement in the aquifer most likely would occur.  相似文献   

6.
This study was undertaken to obtain information about the behavior of sulfentrazone in soil by evaluating the sorption and desorption of the herbicide in different Brazilian soils. Batch equilibrium method was used and the samples were analyzed by high performance liquid chromatography. Based on the results obtained from the values of Freundlich constants (Kf), we determined the order of sorption (Haplic Planosol < Red-Yellow Latosol < Red Argisol < Humic Cambisol < Regolitic Neosol) and desorption (Regolitic Neosol < Red Argisol < Humic Cambisol < Haplic Planosol < Red-Yellow Latosol) of sulfentrazone in the soils. The process of pesticide sorption in soils was dependent on the levels of organic matter and clay, while desorption was influenced by the organic matter content and soil pH. Thus, the use of sulfentrazone in soils with low clay content and organic matter (low sorption) increases the probability of contaminating future crops.  相似文献   

7.
Herbicide leaching through soil into groundwater greatly depends upon sorption-desorption and degradation phenomena. Batch adsorption, desorption and degradation experiments were performed with acidic herbicide MCPA and three soil types collected from their respective soil horizons. MCPA was found to be weakly sorbed by the soils with Freundlich coefficient values ranging from 0.37 to 1.03 mg1−1/n kg−1 L1/n. It was shown that MCPA sorption positively correlated with soil organic carbon content, humic and fulvic acid carbon contents, and negatively with soil pH. The importance of soil organic matter in MCPA sorption by soils was also confirmed by performing sorption experiments after soil organic matter removal. MCPA sorption in these treated soils decreased by 37-100% compared to the original soils. A relatively large part of the sorbed MCPA was released from soils into aqueous solution after four successive desorption steps, although some hysteresis occurred during desorption of MCPA from all soils. Both sorption and desorption were depth-dependent, the A soil horizons exhibited higher retention capacity of the herbicide than B or C soil horizons. Generally, MCPA sorption decreased in the presence of phosphate and low molecular weight organic acids. Degradation of MCPA was faster in the A soil horizons than the corresponding B or C soil horizons with half-life values ranging from 4.9 to 9.6 d in topsoils and from 11.6 to 23.4 d in subsoils.  相似文献   

8.
Cao J  Guo H  Zhu HM  Jiang L  Yang H 《Chemosphere》2008,70(11):2127-2134
Sorption and desorption of the herbicide prometryne in two types of soil subjected to the changes of pH and soil organic matter and surfactant were investigated. The sorption and desorption isotherms were expressed by the Freundlich equation. Freundlich Kf and n values indicate that soil organic matter was the major factor affecting prometryne behavior in the test soils. We also quantified the prometryne sorption and desorption behavior in soils, which arose from the application of Triton X-100 (TX100), a nonionic surfactant and change in pH. Application of TX100 led to a general decrease in prometryne sorption to the soils and an increase in desorption from the soils when applied in dosages of the critical micella concentration (CMC) 0.5, 1 and 2. At the concentration below the CMC, the non-ionic surfactant showed a tendency to decrease prometryne sorption and desorption. It appeared that TX100 dosages above CMC were required to effectively mobilize prometryne. Results indicate that the maximum prometryne sorption and minimum prometryne desorption in soils were achieved when the solution pH was near its pKa. Finally, the influence of TX100 on the mobility of prometryne in soils using soil thin-layer chromatography was examined.  相似文献   

9.
10.
Sorption and desorption of sulfadiazine in soil and soil-manure systems   总被引:10,自引:0,他引:10  
Sulfadiazine is a widely used veterinary medicine that has high potential to enter the environment, especially the soil compartment by the application of manure on agricultural land and grass land or by the deposition of dung pats on pasture. Once it reaches the soil environments, it may enter into surface and ground water. Therefore, sorption-desorption behavior of sulfadiazine was studied under laboratory conditions in five different soils varying in their physicochemical properties. A batch equilibration technique was used with initial aqueous solution concentration of sulfadiazine at 5, 0.5, 0.05, and 0.005 microg mL(-1). Sorption-desorption data in soils with and without manure were well fitted with Freundlich model in log form (r(2), 0.99). A sorption-desorption hysteresis effect was apparent in all soils. A significant amount of sulfadiazine was found tightly bound to the soil particles and did not desorb after the desorption process. Moreover, presence of manure enhanced hysteresis effect. Hysteresis coefficient (H) value from soils in absence of manure (0.9-1.0) increased to the soils in presence of manure (0.9-1.8). Soils in the absence of manure showed low level of K(D Sorp.) values ranging from 0.1 to 24.3, suggesting low level sorption of sulfadiazine with appreciable risk of run-off and leaching, and in turn, surface and ground water contamination. However, presence of manure increased the sorption tendency of sulfadiazine significantly (K(D Sorp.), 6.9-40.2). K(D) values pertaining to desorption cycle increased from 1.2-90.4 to 10.4-167.3 in absence and presence of manure, respectively.  相似文献   

11.

The objectives of this study were to assess sorption and desorption of tylosin, a macrolide antimicrobial chemical used in swine, cattle, and poultry production, in three silty clay loam soils of South Dakota and compare soil sorption to sand and manure sorption. The silty clay loam soils, from a toposequence in eastern South Dakota, standardized sand samples, and swine manure were used in 24-h batch sorption studies with tylosin concentrations ranging from 25 to 232 μ mole/L. Desorption from soil was conducted over a four-day period. Partition coefficients, based on the Freundlich isotherm (K f ) or K d values, were calculated. K f values for the silty clay loams were similar, not influenced by landscape position, and averaged 1350 with isotherm slopes ranging from 0.85 to 0.93. K f values for sand were dependent on solution/sand ratios and pH, ranging from 1.4 to 25.1. K d values of manure were dependent on the solution type and ranged from 840 L/kg with urine to about 175 L/kg when sorbed from water. Desorption of tylosin from each soil over the four-day period was < 0.2% of the amount added. The soils' high K f values and low desorption amounts suggest that once tylosin is in these soils, leaching to lower depths may not occur. However, this does not preclude runoff with soil eroded particles. If tylosin reaches a sand aquifer, through bypass flow or other mechanism(s), movement in the aquifer most likely would occur.  相似文献   

12.
Imidacloprid, the major component of many widely used insecticide formulations, is highly persistent in soils. In this study, the sorption of imidacloprid by six soils as well as its photodegradation and hydrolysis in water were studied. The soils differed significantly in organic matter content and other physical and chemical properties. Sorption increased with increasing soil organic matter content but was not significantly correlated with other soil properties. Removal of organic matter via H2O2 oxidation decreased the sorption. By normalizing the Freundlich coefficients (Kf) to organic matter contents, the variability in obtained sorption coefficient (Kom) was substantially reduced. These results indicate that soil organic matter was the primary sorptive medium for imidacloprid. The low heat of sorption calculated from Kom suggests that partition into soil organic matter was most likely the mechanism. The photodegradation and hydrolysis of imidacloprid in water followed pseudo-first-order kinetics; however, the latter process needed a six-time-higher activation energy. While both processes produced the same main intermediate, they occurred via different pathways. The hydrolysis of imidacloprid was not catalyzed by the high interlayer pH in the presence of metal-saturated clays, which appeared to result from the lack of the pesticide adsorption in the interlayers of clays.  相似文献   

13.
To assess the risk of a pesticide to leach to groundwater or to run off to surface water after application, it is necessary to characterize the sorption of the pesticide to soil. For pyrethroids, their hydrophobicity, strong sorption to various materials, and low solubility make it difficult to accurately characterize sorption processes. The objective of this research was to evaluate the variability in cyfluthrin ((RS)-alpha -cyano-4-fluoro-3-phenoxybenzyl (1RS,3RS;1RS,3SR)-3-(2,2-dichlorovinyl)-2,2-dimethylcyclopropanecarboxylate) sorption to soil as affected by experiment conditions. To minimize cyfluthrin sorption on the walls of glass, silanized-glass, stainless steel, and PTFE centrifuge tubes, cyfluthrin solution was added to aqueous soil slurries or directly to soil, after which it was equilibrated with aqueous solution. Depending on the soil, variation in sorption coefficients, Koc, obtained using different experimental methodologies with one soil can be comparable to the variation in Koc values obtained for soils with different physical and chemical properties using one method. Koc values for cyfluthrin ranged from 56,000 to 300,000 L kg-1. Sorption methodology needs to be evaluated before sorption coefficients are used in predictive transport models.  相似文献   

14.
Paraquat adsorption, degradation, and remobilization were investigated in representative tropical soils of Yom River Basin, Thailand. Adsorption of paraquat in eight soil samples using batch equilibration techniques indicated that adsorption depended on soil characteristics, including exchangeable basic cations and iron content. Multiple regression analysis indicated significant contribution of exchangeable calcium percentage (ECP), total iron content (TFe) and exchangeable sodium percentage (ESP) to paraquat sorption (Q). ESP and TFe were significant at all adsorption stages, whereas ESP was significant only at the initial stage of paraquat adsorption. Adsorption studies using two soils representing clay and sandy loam textures showed that paraquat adsorption followed the Freundlich model, exhibiting a nonlinear sorption curve. Paraquat adsorption was higher in the clay soil compared to the sandy loam soil with Kf values of 787 and 18, respectively. Desorption was low with 0.04 to 0.17% and 0.80 to 5.83% desorbed in clay and sandy loam soil, respectively, indicating some hysteresis effect. Time-dependent paraquat adsorption fitted to the Elovich kinetic model indicated that diffusion was a rate-limiting process. Paraquat mobility and degradation studies conducted using both field and laboratory soil column experiments with clay soil showed low mobility of paraquat with accumulation only in the surface 0-5 cm layer under field conditions and in the 0-1 cm layer in a laboratory soil column experiment. Degradation of paraquat in soil was faster under field conditions than at ambient laboratory conditions. The degradation rate followed a first-order kinetic model with the DT50 at 36-46 days and DT90 around 119-152 days.  相似文献   

15.
Adsorption of metolachlor and atrazine was studied in the fly ash (Inderprastha and Badarpur)- amended Inceptisol and Alfisol soils using batch method. Results indicated that sorption of both the herbicides in soil+fly ash mixtures was highly nonlinear and sorption decreased with a higher herbicide concentration in the solution. Also, nonlinearity increased with an increase in the level of fly ash amendment from 0-5%. Three two-parameter monolayer isotherms viz. Langmuir, Temkin, Jovanovic and one imperical Freundlich models were used to fit the experimental data. Data analysis and comparison revealed that the Temkin and the Freundlich isotherms were best-suited to explain the sorption results and the observed and the calculated adsorption coefficient values showed less variability. The study suggested that sorption mechanism of metolachlor and atrazine involved the physical association at the sorbate surface and the nonlinearity in the sorption at higher pesticide or fly ash concentration was due to a decrease in the heat of adsorption and higher binding energy.  相似文献   

16.
The sorption-desorption of metolachlor [2-chloro-N-(ethyl-6-methyl phenyl)-N-(2-methoxy-1-methyl ethyl) acetamide], isoproturon [3-(4-isopropyl phenyl)-1,1-dimethyl urea] and terbuthylazine [N6-tert butyl-6-chloro-N4-ethyl-1,3,5-triazine-2,4-diamine] herbicides was studied in two German soils at 1:10 soil to water ratio by batch method. Equilibrium of herbicides between soil and water (0.01 M CaCl2) was attained in 2 h. Sorption data fitted very well to Freundlich equation, represented by very high correlation coefficient (r2 > 0.934). Comparison of Freundlich K values indicated that sorption of all the three herbicides was most pronounced in soil having higher organic carbon content. Koc values were as expected nearly identical for each herbicide in the two soils. The Freundlich constant (1/n) was about 1 for metolachlor and less than 1 for terbuthylazine and isoproturon indicating a L-type of sorption isotherms. Desorption of all the three herbicides showed hysteresis. Nearly equal amounts of metolachlor, isoproturon and terbuthylazine were desorbed from both soils. There was a good correlation between Koc and solubility.  相似文献   

17.
Ptaquiloside (PTA) is a carcinogenic norsesquiterpene glucoside produced by Bracken in amounts up to at least 500 mg m(-2). The toxin is transferred from Bracken to the underlying soil from where it may leach to surface and groundwater's impairing the quality of drinking water. The objectives of the present study were to characterize the solubility, degradation and retention of PTA in soils in order to evaluate the risk for groundwater contamination. PTA was isolated from Bracken. The logarithmic octanol-water and ethyl acetate-water partitioning coefficients for PTA were -0.63 and -0.88, respectively, in agreement with the high water solubility of the compound. PTA hydrolysed rapidly in aqueous solution at pH 4 or lower, but was stable above pH 4. Incubation of PTA with 10 different soils at 25 degrees C showed three different first order degradation patterns: (i) rapid degradation observed for acid sandy soils with half life's ranging between 8 and 30 h decreasing with the soil content of organic matter, (ii) slow degradation in less acid sandy soils with half-lives of several days, and (iii) fast initial degradation with a concurrent solid phase-water partitioning reaction observed for non-acid, mostly clayey soils. The presence of clay silicates appears to retard the degradation of PTA, possibly through sorption. Degradation at 4 degrees C was generally of type (iii) and degradation rates were up to 800 times lower than at 25 degrees C. Sorption isotherms for the same set of soils were almost linear and generally showed very low sorption affinity with distribution coefficients in the range 0.01-0.22 l kg(-1) at a solution concentration of 1 mg l(-1) except for the most acid soil; Freundlich affinity coefficients increased linearly with clay and organic matter contents. Negligible sorption was also observed in column studies where PTA and a non-sorbing tracer showed almost coincident break-through. Leaching of PTA to the aqueous environment will be most extensive on sandy soils, having pH >4 and poor in organic matter which are exposed to high precipitation rates during cold seasons.  相似文献   

18.
Sorption-desorption behavior of imidacloprid in six soils collected from five coastal regions in Croatia at 20, 30 and 40°C was investigated using batch equilibrium technique. Isothermal data were applied to Freundlich, Langmuir and Temkin equations, and the thermodynamic parameters ΔH°, ΔG°, ΔS° were calculated. The sorption isotherm curves were non-linear and may be classified as L-type, suggesting a relatively high sorption capacity for imidacloprid. Our results showed that the K( sor ) ( F ) values decreased for all the tested soils as the temperature increased, indicating that the temperature strongly influences the sorption. Values of ΔG° were negative (-4.65 to -2.00 kJ/mol) indicating that at all experimental temperatures the interactions of imidacloprid with soils were spontaneous processes. The negative and small ΔH° values (-19.79 to -8.89 kJ/mol) were in the range of weak forces, such as H-bonds, consistent with interactions and partitioning of the imidacloprid molecules into soil organic matter. The ΔS° values followed the range of -57.12 to -14.51 J/molK, suggesting that imidacloprid molecules lose entropy during transition from the solution phase to soil surface. It was found that imidacloprid desorption from soil was concentration and temperature-dependent, i.e. at lower imidacloprid concentrations and temperature, lower desorption percentage occurred. Desorption studies revealed that hysteretic behavior under different temperature treatments existed, and it was more pronounced at 20°C in the soils with higher OC content. The study results emphasize the importance of thermodynamic parameters in controlling soil pesticide mobility in different geographical locations, seasons and greenhouse conditions.  相似文献   

19.
Atrazine and metolachlor were more strongly retained on earthworm (Lumbricus terrestris L.) castings than on soil, suggesting that earthworm castings at the surface or at depth can reduce herbicide movement in soil. Herbicide sorption by castings was related to the food source available to the earthworms. Both atrazine and metolachlor sorption increased with increasing organic carbon (C) content in castings, and Freundlich constants (Kf values) generally decreased in the order: soybean-fed > corn-fed > not-fed-earthworm-castings. The amount of atrazine or metolachlor sorbed per unit organic carbon (Koc values) was significantly greater for corn-castings compared with other castings, or soil, suggesting that the composition of organic matter in castings is also an important factor in determining the retention of herbicides in soils. Herbicide desorption was dependent on both the initial herbicide concentration, and the type of absorbent. At small equilibrium herbicide concentrations, atrazine desorption was significantly greater from soil than from any of the three casting treatments. At large equilibrium herbicide concentrations, however, the greater organic C content in castings had no significant effect on atrazine desorption, relative to soil. For metolachlor, regardless of the equilibrium herbicide concentration, desorption from soybean- and corn-castings treatments was always less than desorption from soil and not-fed earthworm castings treatments. The results of this study indicate that, under field conditions, the extent of herbicide retention on earthworm castings will tend to be related to crop and crop residue management practices.  相似文献   

20.
This investigation was undertaken to determine the effect of amendment of two fly ashes [Kota and Inderprastha (IP)] on sorption behavior of metsulfuron-methyl in three Indian soil types. Kota fly ash (5%) did not show any effect on herbicide sorption while IP fly ash significantly enhanced the sorption. Further studies on metsulfuron-methyl sorption-desorption behavior in 0.5, 1, 2, and 5% IP fly ash-amended soils suggested that effect of fly ash varied with soil type and better effect was observed in low organic carbon content soils. The sorption-desorption isotherms fitted very well to the Freundlich sorption equation and, in general, slope (1/n) values less than unity were observed. Metsulfuron-methyl sorption in the IP fly ash-amended soils showed strong correlation with the fly ash content and compared to the Freundlich sorption constant (K f), K FA values (sorption normalized to fly ash content) showed less variation. Metsulfuron-methyl leaching studies suggested greater retention of herbicide in the application zone in IP fly ash-amended soils, but effect varied with soil type and no herbicide leaching was observed in 5% fly ash-amended soils. The study suggested that all coal fly ashes are not effective in enhancing the sorption of metsulfuron-methyl in soils. However, one which enhanced herbicide sorption, could play an important role in reducing its leaching losses.  相似文献   

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