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1.
高岭石,蒙脱石和针铁矿对泥炭腐殖酸的吸附和分离   总被引:6,自引:0,他引:6  
Sorption of humic acid (HA) on mineral surfaces has a profound interest regarding the fate of hydrophobic organic contaminants (HOCs) and carbon sequestration in soils. The objective of our study is to determine the fractionation behavior of HA upon sorption on mineral surfaces with varying surface properties. HA was coated sequentially on kaolinite (1:1 clay), montmorillonite (2:1 clay), and goethite (iron oxide) for four times. The unadsorbed HA fractions were characterized by elemental analysis, diffuse reflectance infrared Fourier transform spectroscopy (DRIFT), and solid state 13C nuclear magnetic resonance spectroscopy (NMR). The mineral-HA complexes were characterized by DRIFT. Polarity index [(N+O)/C] revealed higher polarity of the unadsorbed HA fractions after coating on kaolinite, reflecting that relatively higher polarity fractions of HA remain unadsorbed. Sorption of aliphatic alcohol fraction along with carbohydrate was prominent on kaolinite surface. DRIFT results of the unadsorbed HA fractions indicated more sorption of aliphatic moieties on both kaolinite and montmorillonite. DRIFT results of the unadsorbed HA fractions after sorption on kaolinite and goethite showed the sorption of the proteinaceous fractions of HA. The HA fractions obtained after coating on goethite showed significant sorption of carboxylic moieties. The results mentioned above comply reasonably well with the DRIFT spectra of the mineral-HA complexes. 13C NMR results showed higher sorption of anomeric C on kaolinite surface. Higher sorption of paraffinic fraction was observed on montmorillonite. NMR data inferred the sorption of carboxylic moieties on goethite surface. Overall, this study showed that aliphatic moieties of HA preferentially sorbed on kaolinite and montmorillonite, while carboxylic functional groups play a significant role in sorption of HA on goethite. The sorbed fractions of HA may modify the mineral surface properties, and thus, the interaction with organic contaminants.  相似文献   

2.
Abstract

Laboratory experiments were carried out to evaluate lead (Pb), copper (Cu), zinc (Zn), and cadmium (Cd) sorption‐desorption by three soils of contrasting characteristics. Talamanca (silt loam, montmorillonite, Calcic Haploxeralfs), Mazowe (clay, kaolinite, Rhodic Kandiustalf), and Realejos (sandy silt loam, allophane, Typic Hapludands). A second objective was to study the effect of nitriloacetic acid (NTA) on the sorption process. The Talamanca soil, which had a native pH of 6.4 and presented the highest effective cation exchange capacity (ECEC), sorbed more of each of the metal tested than did the other two soils. When the other two soils were compared metal sorption was also related to pH and ECEC. The very low sorption capacity showed by Realejos may be attributed to the low net surface negative charge density of this soil, arising from its allophanic nature. A common feature of the three soils was the relative strong sorption of both Pb and Cu relative to Cd and Zn with Pb showing the highest sorption levels. The selectivity sequences of metals retention were Pb>Cu>Zn>Cd for Talamanca soil, Pb>Cu>Zn≈Cd for Mazowe, and Pb>Cu>Cd>Zn for Realejos. Metal desorption values were low. The order of metal desorption (Cd≈Zn>Cu>Pb) was the same for the three soils studied. Quantitative differences observed in the extractability of the sorbed metals between the soils (Realejos>Mazowe>Talamanca) indicated that soil properties which enhanced metal sorption contributed at the same time to slow down the backward reaction. The addition of NTA to the soil suspension significantly depressed metal sorption by the three soils investigated. Compared with the free ligand system Pb, Cu, Zn, and Cd sorption in the presence of NTA decreased roughly 50%.  相似文献   

3.

Potentiometric and ion-selective electrode titrations together with batch sorption/desorption experiments, were performed to explain the aqueous and surface complexation reactions between kaolinite, Pb, Cd and three organic acids. Variables included pH, ionic strength, metal concentration, kaolinite concentration and time. The organic acids used were p-hydroxybenzoic acid, o-toluic acid, and 2,4-dinitrophenol. Titrations were used to derive previously unavailable aqueous conditional stability constants for the organometallic complexes. Batch results showed that aqueous lead-organic complexation reduced sorption of Pb by kaolinite. Cadmium behavior was similar, except for 2,4-dinitrophenol, where Cd sorption was increased. Metal sorption increased with increasing pH and decreasing ionic strength. Distribution ratios (K d 's) decreased with increasing solid/solution ratio. The subsurface transport of lead and cadmium may be enhanced via complex interactions with organic wastes or their degradation products and sorbent mineral surfaces.

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4.

Purpose

Biochars are increasingly recognized as effective, inexpensive, and environmentally friendly sorbents for abating organic contaminants. In this study, the sorption and competitive sorption characteristics of simazine (SZ), metsulfuron-methyl (ME), and tetracycline (TC) to corn straw biochars and soil were examined to understand the interactions of herbicides and antibiotics with biochars and the potential role of biochars as engineered sorbents.

Materials and methods

Biochars were obtained by pyrolyzing corn straw at 400, 500, and 600 °C for 6 h under oxygen-limited conditions and were characterized via elemental analysis, N2-BET surface area determination, 13C nuclear magnetic resonance spectroscopy, and Fourier transform infrared spectroscopy. Soil was collected from North Tanggu Farm in Tianjin, and its organic carbon, cation exchange capacity, and particle size distribution were analyzed. The batch sorption experiments were performed to obtain the sorption isotherms of SZ, ME, and TC to biochars and soil.

Results and discussion

The biochars that were pyrolyzed at higher temperatures had higher sorption affinities for SZ, ME, and TC, which may be due to the enhancement of hydrophobic interactions, charge transfer (ππ*) interactions, and pore-filling mechanism. The sorption affinities for these compounds to all biochars decreased in the order SZ?>?TC?>?ME, indicating that the neutral molecule with a stronger hydrophobicity is more easily adsorbed by biochars. For soil, the decrease of the sorption affinities followed the order TC?>?SZ?>?ME due to the high sorption affinity of TC with clays in the soil. Moreover, the sorption affinities of TC by biochars were lower than by soil, indicating that corn straw biochars may be not an ideal sorbent for the immobilization of TC. Biochars were much more effective in sorbing SZ and ME than soil, indicating that corn straw biochars can potentially prevent transport of the herbicides to surface and ground water. Nevertheless, the presence of TC significantly hinders biochar adsorption of SZ and ME, implying that the coexisting contaminants should be considered when developing biochars as engineered sorbents.

Conclusions

The observations in this study demonstrated that the sorption of organic contaminants by biochars is dependent on the properties of the biochars and the molecular structures of the contaminants. Corn straw biochars effectively retain SZ and ME and hinder their transportation to surface and ground water; however, the coexisting contaminants should be considered. Our results will be helpful for designing biochars as engineered sorbents for environmental applications.  相似文献   

5.
Treated and untreated rice straw extensively exists in the soil. In order to elucidate its possible effect on the fate of organic pollutants, sorption of pyrene by rice straw and its main constituents (lignin, cellulose, and hemi-cellulose) were studied, as single solute and in the presence of other co-existing organic pollutants, phenanthrene (Phen), benzo[a]pyrene (BaP), phenol, and pentachlorophenol (PCP). Pyrene showed the greatest sorption on lignin with greater aromaticity and smaller polarity, and the sorption coefficient was almost two orders of magnitude greater than those on cellulose and hemi-cellulose. Bi-solute sorption results showed that Phen, BaP and PCP exhibited apparent competitive sorption with pyrene on the four sorbents; while the existence of phenol promoted the sorption of pyrene on rice straw and lignin but inhibited the sorption on cellulose and hemi-cellulose. For the two polycyclic aromatic hydrocarbon (PAH) co-solutes and PCP, hydrophobicity and molecular size played important roles in competition, suggesting the direct competition for hydrophobic sorption sites and pore blockage mechanisms. In contrast, the polar co-solute, phenol showed different effects on pyrene sorption onto the four sorbents, suggesting that multiple interactions between polar organic compounds and sorbents are involved in the sorption.  相似文献   

6.
This study evaluated cadmium (Cd), lead (Pb), zinc (Zn), and copper (Cu) sorption characteristics of three tropical soils. Data obtained conformed to Freundlich sorption model and the S-shaped isotherm curve. Sorption efficiency of Zn and Pb were highest in alkaline soil while slightly acid soil had the highest Cd and Cu sorption efficiency for monometal sorption. In competitive sorption, metals were more sorbed in slightly acid soil while the least efficiency was recorded in acid soil. Distribution coefficient; Kd (average across soil types) in monometal sorption followed the order: Pb > Zn > Cd > Cu. For competitive sorption, the order was Zn > Pb > Cu > Cd. When in competition, Cd was preferentially sorbed in slightly acid and alkaline soils and Zn for acid soil. Conclusively, lead is more in equilibrium solution when in competition with Cd, Zn and Cu making it potential agent of soil and groundwater pollution.  相似文献   

7.
In most phosphorus (P) sorption studies, P is added as an inorganic salt to a predefined background solution such as calcium chloride (CaCl2) or potassium chloride (KCl); however, in many regions, the application of P to agricultural fields is in the form of animal manure. The purpose of this study, therefore, was to compare the sorption behavior of dissolved reactive P (DRP) in monopotassium phosphate (KH2PO4)–amended CaCl2 and KCl solutions with sorption behavior of DRP in three different animal manure extracts. Phosphorus single‐point isotherms (PSI) were conducted on eight soils with the following solutions: KH2PO4‐amended 0.01 M CaCl2 solution, KH2PO4‐amended 0.03 M KCl solution, water‐extracted dairy manure, water‐extracted poultry litter, and swine lagoon effluent. The PSI values for the dairy manure extract were significantly lower than the CaCl2 solution for all eight soils and lower than the KCl solution for six soils. The PSI values were significantly higher, on the other hand, for poultry litter extract and swine effluent than the inorganic solutions in four and five of the soils, respectively. Our observations that the sorption of DRP in manure solutions differs significantly from that of KH2PO4‐amended CaCl2 and KCl solutions indicates that manure application rates based on sorption data collected from inorganic P salt experiments may be inaccurate.  相似文献   

8.
Sorption of antibiotics to clay minerals is a key process controlling their transport and fate in environment. In this study, the effects of pH, ionic strength, and Cu(II) on ofloxacin (OFL) sorption to kaolinite were investigated by batch sorption experiments. The results of sorption edge experiments suggested that OFL sorption to kaolinite was pH and ionic strength dependent. Cation exchange was a major contributor to the sorption of OFL+ to kaolinite. The decreased OFL sorption with increasing ionic strength indicated the formation of outer-sphere complexation. When solution pH was lower than 7.0, Cu-OFL complexes facilitated OFL sorption through electrostatic attraction or formation of kaolinite-Cu-OFL and kaolinite-OFL-Cu ternary surface complexes. However, existence of free Cu(II) cation in solution competed for sorption sites, and thus suppressed OFL sorption. When solution pH was higher than 7.0, Cu(II) existed as Cu(OH)2, and the Cu-OFL complexes in aqueous phase and solid phase (precipitation) enhanced OFL removal efficiency from solution. The results imply that Cu(II) effects should be taken into account in the evaluation of OFL mobility in environment.  相似文献   

9.

Purpose

Sorption of humic substances on other soil components plays an important role in controlling their function and fate in soil. Sorption of humic substances by individual soil components has been studied extensively. However, few studies reported the sorption characteristic of humic substances on composites of soil components. This study aimed to investigate the sorption characteristics of humic acid on Fe oxide-bacteria composites and improve the understanding on the interaction among humic substance Fe oxide bacteria in soil.

Materials and methods

Humic acid was purchased from Sigma-Aldrich and was purified. Hematite and ferrihydrite were synthesized in the lab. Bacillus subtilis and Pseudomonas putida were cultivated in Luria-Broth medium and harvested at stationary growth phase. Batch sorption experiments were carried out at pH 5.0. Various amounts of humic acid were mixed with 20 mg of Fe oxide, bacteria, or Fe oxide-bacteria composite (oxide to bacteria of 1:1) in 10 mL of KCl (0.02 mol L?1) to construct sorption isotherms. The effects of phosphate concentration and addition order among humic acid, Fe oxide, bacteria on the sorption of humic acid were also studied. The sorption of humic acid was calculated by the difference between the amount of humic acid added initially and that remained in the supernatant.

Results and discussion

The maximum sorption of humic acid on hematite, ferrihydrite, B. subtilis and P. putida was 73.2, 153.5, 69.1, and 56.7 mg C g?1, respectively. The maximum sorption of humic acid on examined Fe oxide-bacteria composite was 28.2–57.2 % less than the predicted values, implying that the sorption of humic acid was reduced by the interaction between Fe oxides and bacteria. The presence of phosphate exerted negligible influence on the sorption of humic acid on bacteria while it inhibited the sorption of humic acid on Fe oxides. On Fe oxide-bacteria composites, inhibiting influences followed by promoting or weak inhibiting effects of phosphate with increasing concentration on the sorption of humic acid were found.

Conclusions

The interaction between Fe oxides and bacteria reduced the sorption of humic acid; moreover, the reduction was greater by the interaction of bacteria with ferrihydrite than that with hematite. Phosphate exerted negligible and inhibiting influence on the sorption of humic acid by bacteria and Fe oxides, respectively. On Fe oxide-bacteria composites, humic acid sorption was initially inhibited and then promoted or weakly inhibited by phosphate with increasing concentration.  相似文献   

10.
Sorption of Cd at low concentrations onto two Danish soils (loamy sand, sandy loam) was examined in terms of kinetics and governing factors. From an environmental point of view soil sorption of Cd is a fast process: More than 95% of the sorption takes place within 10 min, equilibrium is reached in 1 hr, and exposures up to 67 wk did not reveal any long term changes in Cd sorption capacities. The soils have very high affinity for Cd at pH = 6.00 (10?3 M CaCl2) exhibiting distribution coefficients in the order of 200 to 250 (soil Cd concentration/solute Cd concentration). However, the sorption isotherms describing the distribution of Cd between soil and solute are slightly curvelinear. In the pH-interval 4 to 7.7, the sorption capacity of the soil approximately increases 3 times for a pH increase of one unit. Increasing the Ca concentration from 10?3 to 10?2 M reduces the sorption capacity of the sandy loam to one third.  相似文献   

11.
Phosphorus sorption and desorption processes in selected soils were investigated to evaluate the usefulness of phosphorus sorption isotherms in the estimation of the phosphorus supplying capacity of soils. There was a distinct hysteresis in the phosphorus sorption and desorption isotherms, resulting in an overestimation of the replenishing ability of soils to supply phosphorus to the soil solution, when phosphorus sorption isotherms were used for the estimations.

To attain a value of 0.2 ppm P in the soil solution, 115 µmol P/g soil are required in the Kuromatsunai Ando soil (Ochric Andosols) based on the estimation by the P desorption isotherms; this value is 29% higher than that indicated by the P sorption isotherm. Also 42 µmol P/g soil are required in the Mikatagahara Yellow soil (Helvic Acrisols)—which corresponds to a value 23% higher than that indicated by the P sorption isotherm.

Two types of hysteresis subloops were observed: A reversible type and an irreversible type. The former was found typically in the highly weathered Mikatahagara Yellow soil while the latter was observed in the Kuromatsunai Ando soil.  相似文献   

12.
The adsorption and ion-exchange behavior of Co, Cu, Zn, and Cd were studied in two soils of different genesis. The sorption parameters and selectivity coefficients of the Me-Ca ion exchange were determined using the Langmuir and Freundlich adsorption isotherms and two models of ion-exchange sorption based on the mass action law (a polyfunctional ion exchanger and a mixture of two ideal exchangers) for describing the relationships between the dissolved and sorbed metal forms. It was shown that simple models provided information for better understanding of the behavior of metals in sorption and ion-exchange processes, but the conclusions about the sorption of different metals in a specific soil or a specific metal in different soils based on these models can be different.  相似文献   

13.
The direct effects of dissolved organic matter (DOM) on the sorption of orthophosphate onto gibbsite, goethite, and kaolin were examined using a one-point phosphorus sorption index and the linear Tempkin isotherm model. DOM extracted from fresh and decomposed agricultural residues, as well as model organic and humic acids, were used. Changes in the chemical and sorptive characteristics of the DOM in the absence and presence of added orthophosphate (50 mg l−1) were also determined. For residue-derived materials, DOM sorption to all minerals correlated well with percent hydrophobicity, apparent molecular weight, and phenolic acidity in the absence of added orthophosphate. Sorption of DOM to goethite and gibbsite was significantly decreased in the presence of added P. The correlation coefficient values of percent hydrophobicity, apparent molecular weight, and phenolic acidity to sorption also declined in the presence of added P. Thus, the addition of P substantially lowered fractionation of DOM after sorption to goethite and gibbsite. In contrast, few significant P sorption-induced differences were observed in the kaolin system. According to one-point P sorption results, DOM in the form of Aldrich humic acid, oxalate, and decomposed clover and corn residue, significantly inhibited P sorption to goethite at concentrations of 50 and 200 mg total soluble carbon (CTS l−1). Phosphorus sorption to gibbsite was significantly inhibited by 50 mg CTS l−1 derived from decomposed corn residue, fresh dairy manure residue, and oxalate solution. At 200 mg CTS l−1, all DOM solutions were found to inhibit P sorption to gibbsite. This study suggests that DOM inhibition of P sorption depends on the chemical properties of both the sorbent and the DOM itself. In general, DOM from decomposed organic materials inhibited P sorption to a greater extent than did DOM derived from fresh materials. This stronger inhibition highlights the importance of microbial processes in the release of soluble soil P, a key determinant of P availability to plants.  相似文献   

14.
《Geoderma》2001,99(3-4):317-328
Experiments on the sorption of dissolved organic carbon (DOC) in soils were mainly conducted in batch approaches. Because varying setups were used in these studies, comparison of the results requires knowledge on the effects that different experimental conditions may have on the sorption of DOC. This investigation evaluated the DOC sorption of soils using differently pretreated soil samples (field-fresh (two sampling dates), air-dried, stored at 3°C and −18°C), at different soil-to-solution ratios (1:40, 1:20, 1:10 and 1:5 w/v) and different temperatures (5°C, 15°C, 25°C and 35°C). The sorption of DOC was analyzed using the initial mass (IM) approach, which regressed the initial amount of sorbate (normalized to soil mass) against the sorbed amount (normalized to soil mass). The DOC release — when a solution without DOC was added — strongly increased with temperature and soil-to-solution ratio. Among the different types of sample storage and preparation, air-drying resulted in the largest DOC release. The smallest release was from the field-fresh samples. Freezing and storage at 3°C resulted in intermediate DOC release with freezing having the greater effect. The release from air-dried samples exceeded that of field-fresh samples by a factor of four at maximum. In contrast, none of the experimental setups influenced the slope of the IM isotherms. Thus, it seems possible to compare directly the binding affinity of DOC to different soils as determined at varying experimental conditions.  相似文献   

15.
Previously presented evidence of Zn competition for Cd soil sorption sites has been confirmed by detailed studies of two Danish soils. Cadmium distribution between soil and solute decreases for increasing Zn solute concentrations. A Langmuir model accounting for both Cd and Zn sorption onto the same sorption sites was supported by independent experimental data on Cd and Zn distribution. The competition of Zn is governed by the product of the Zn soil sorption stability constant and the actual Zn solute concentration. Cadmium distribution coefficients may be significantly influenced by Zn at Zn solute concentrations above 100 μg Zn dm?3. This may have implications for interpreting Cd plant uptake and leaching.  相似文献   

16.
Abstracts

Three anion (selenite, phosphate, and fluoride) sorption, and the concomitant release of silicate, sulphate, and organic matters from soils, and proton consumption with sorption were investigated using two andosols in Japan. The following sequence of sorption by the andosols was, fluoride (F) >> phosphate (P) > selenite (Se); concomitant proton consumption with sorption, F >> P > Se; organic matter released, P > Se > F; and sulfate released, P > Se >> F. There was quite a difference between an allophanic and a non‐allophanic andosols in silicate released with anion sorption. Our results suggest that the fluoride sorption mechanism is different from the others and that surface sites with OH groups for inner‐sphere complexes with selenite on soil particles which are restricted as compared to phosphate and fluoride.  相似文献   

17.
Abstract

The sorption of several organic phosphates were measured on soil, peat and other organic and inorganic materials. The behavior of the phosphates on these materials differed from that reported for similar studies on acidic soil materials. In contrast to the sorption on acidic soils, where sorption maxima occur, the sorption on basic soils may reach a maximum but does not decline thereafter. Both clay and organic matter content govern the amount of sorption but calcium seems to account for the differences observed from those on acidic soil materials  相似文献   

18.
Abstract

Environmental changes and management practices which alter soil properties may affect the capacity of soils to sorb trace metals, such as copper (Cu), zinc (Zn), and cadmium (Cd), and thus influence the bioavailability and leach ability of the metals. Two agricultural soils were treated to partially oxidize organic matter and to decrease soil pH for evaluating the effects of acidification and organic matter oxidation on trace metal sorption onto soils. For the one soil with a pH value of 6.74 and organic carbon (C) content of 46.9 g‐kg‐1, loss of 11% of its organic matter reduced by 97, 72, and 62% the original sorption capacity for Cu, Zn, and Cd, respectively, while the corresponding values caused by acidifying the soil one pH‐unit were 32, 16, and 29%. For the another soil with a pH of 4.69 and organic C content of 16.3 g‐kg‐1, a decrease in pH by one unit resulted in a loss of 43, 21, and 52% of the sorption capacity for Cu, Zn, and Cd, respectively.  相似文献   

19.
Abstract

Phosphate sorption isotherms were determined for 16 representative major soils developed from different parent materials on Okinawa. Phosphate sorption characteristics were satisfactorily described by the Langmuir equation, which was used to determine phosphorus (P) sorption maxima of the soils. Phosphate sorption maxima ranged from 630 to 2208 mg P kg‐1 soil (mean 1,362 mg P kg‐1). The standard P requirement (i.e., the amount of P required to attain 0.2 mg P L‐1 equilibrium solution) followed the same trend as sorption maximum (r =0.94***), with values ranging from 132 to 1,020 mg P kg‐1 soil (mean 615 mg P kg‐1). This mean value corresponds to fertilizer addition of 923 kg P ha‐1 indicating that the soils have high P fertilizer requirements. Results of simple linear regression analysis indicated that sorption maximum was significantly correlated with clay content, organic matter, oxalate iron (Fe), pyrophosphate Fe, DCB aluminum (Al), oxalate Al, and pyrophosphate Al, but not with DCB Fe, pH, or available P content. The best regression model for predicting sorption maximum was the combination of clay, organic matter, pyrophosphate Fe, and DCB Al which altogether explained 79% of the variance in sorption maximum. The equation obtained could offer a rapid estimation of P sorption in Okinawan soils.  相似文献   

20.
Abstract. The phosphorus (P) sorption and desorption dynamics of eleven major agricultural grassland soil types in Ireland were examined using laboratory techniques, so that soils vulnerable to P loss might be identified. Desorption of P from soil using the iron-oxide paper strip test (Pfeo), water extractable P (Pw) and calcium chloride extractable P (Pcacl2) depended on soil P status in all soils. However, soil types with high organic matter levels (OM), namely peat soils (%OM >30), had lower Pfeo and Pw but higher Pcacl2 values compared to mineral soils at similar soil test P levels. Phosphorus sorption capacity remaining (PSCr) was measured using a single addition of P to soils and used to calculate total P sorption capacities (PSCt) and degree of P saturation (DPS). Phosphorus sorption capacities correlated negatively with % OM in soils indicating that OM may inhibit P sorption from solution to soil. High organic matter soils exhibited low P sorption capacities and poor P reserves (total P, oxalate extractable P) compared to mineral soils. Low P sorption capacities (PSCt) in peat soils were attributed to OM, which blocked or eliminated sorption sites with organic acids, therefore, P remained in the soil solution phase (Pcacl2). In this work, peat and high organic matter soils exhibited P sorption and desorption characteristics which suggest that these soils may not be suitable for heavy applications of manure or fertilizer P owing to their low capacities for P sorption and storage.  相似文献   

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