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1.
A study was conducted on the effects of carbon surface chemistry, solution pH, and ionic strength on the removal of diuron and amitrole from aqueous solutions by adsorption on an as-received and oxidized activated carbon fiber. Results obtained were explained by the surface characteristics of the adsorbents and the characteristics of the herbicide molecules. Under the experimental conditions used, diuron uptake was much higher than that of amitrole, despite its larger molecular dimensions, due to the lesser water solubility, greater hydrophobicity, and larger dipolar moment of diuron compared with amitrole. Uptake variations associated with differences in carbon surface oxidation, solution pH, and ionic strength were explained by corresponding changes in electrostatic, hydrophobic, and van der Waals interactions.  相似文献   

2.
Removal of amitrole from water was studied by adsorption on an activated carbon cloth and by oxidation with hydrogen peroxide using the same activated carbon cloth as catalyst. Study variables included the solution pH, ionic strength, and temperature in the adsorption process and the solution pH and the surface chemistry of the activated carbon cloth in the oxidation process. Results showed that amitrole adsorption on activated carbon cloth was not adequate to remove amitrole from water due to the high solubility and low aromaticity of the herbicide, which reduced its adsorption on the carbon. A higher amitrole removal rate was obtained with the activated carbon/H2O2 system. The best results were obtained on basic activated carbon surfaces at pH 7–10, when hydroxyl radical formation is favored, achieving the removal of 35–45% of the AMT, compared with 20–25% under the best adsorption conditions. Importantly, oxygen fixed on the carbon surface during AMT oxidation must be removed by heat treatment in order to regenerate the surface basicity of the carbon before its reutilization in another oxidation cycle.  相似文献   

3.
Adsorption of Cd(II) species at pH = 5 was studied on three carbon adsorbents: granular activated carbon, activated carbon fiber, and activated carbon cloth. As-received and oxidized adsorbents were used. Cd(II) adsorption greatly increased after oxidation due to the introduction of carboxyl groups. The use of a buffer solution to control the pH introduced some changes in the surface chemistry of carbons through the adsorption of one of the compounds used, biphthalate anions. The increase in ionic strength reduced Cd(II) uptake on both as-received and oxidized carbons due to a screening of the electrostatic attractions between the Cd(II) positive species and the negative surface charge, which in the case of as-received carbons derived from the biphthalate anions adsorbed and in the oxidized ones from the carboxyl groups. Tannic acid was used as a model compound for natural organic matter. Its adsorption was greatly reduced after oxidation, and most of the carbon adsorbents preadsorbed with tannic acid showed an increase in Cd(II) uptake. In the case of competitive adsorption between Cd(II) species and tannic acid molecules, there was a decrease in Cd(II) uptake on the as-received carbon whereas the contrary occurred with the oxidized carbons. These results illustrate the great importance of carbon surface chemistry in this competitive adsorption process. Finally, under all experimental conditions used, when the adsorption capacity of carbons was compared under the same conditions it increased in the following order: granular activated carbon < activated carbon fiber < activated carbon cloth.  相似文献   

4.
The effect of surface oxidation, solution pH, and ionic strength on the adsorption of Zn(II) ions from aqueous solution under static conditions was studied using commercial activated carbons in the form of grains and cloth. In addition, the effects of surface oxidation and the presence of dissolved natural organic matter (tannic acid) were studied under dynamic conditions using activated carbon cloth column beds. Under static conditions, surface oxidation largely increased Zn2+ uptake and two H+ ions were displaced from the oxidized carbon surface per Zn(II) ion adsorbed. It is proposed that adsorption of Zn(II) on the as-received basic carbons was due to C(pi)-cation interactions. An increase in solution pH in the range 3-6 increased Zn(II) uptake, whereas an increase in ionic strength decreased Zn(II) uptake because of the screening effect of the added salt. In the experiments carried out with carbon column beds, the oxidized activated carbon cloth was also more effective than the as-received carbon to remove Zn(II) ions. In this case, the presence of tannic acid decreased the efficiency of the oxidized activated carbon cloth bed to remove Zn(II) ions. An increase in the tannic acid initial concentration had a greater effect on the removal of tannic acid than on the removal of Zn(II) by the column bed. This may be a consequence of the greater size of tannic acid molecules and their low affinity for oxidized carbon surfaces.  相似文献   

5.
pH-dependence of pesticide adsorption by wheat-residue-derived black carbon   总被引:8,自引:0,他引:8  
The potential of black carbon as an adsorbent for pesticides in soils may be strongly influenced by the properties of the adsorbent and pesticides and by the environmental conditions. This study evaluated the effect of pH on the adsorption of diuron, bromoxynil, and ametryne by a wheat (Triticum aestivum L.) residue derived black carbon (WC) as compared to a commercial activated carbon (AC). The pH drift method indicated that WC had a point of zero charge of 4.2, much lower than that of 7.8 for AC. The density of oxygen-containing surface functional groups, measured by the Boehm titration, on WC was 5.4 times higher than that on AC, resulting in a pesticide adsorption by WC being 30-50% of that by AC, due to the blockage of WC surface by the waters associated with the functional groups. A small decrease (5.5%/unit pH) in diuron adsorption by WC with increase in pH resulted from increased deprotonation of surface functional groups at higher pH values. A much larger decrease (14-21%/unit pH) in bromoxynil adsorption by WC with increase in pH resulted from the deprotonation of both the adsorbate and surface functional groups of the adsorbent. The deprotonation reduced the adsorptive interaction between bromoxynil and the neutral carbon surface and increased the electrical repulsion between the negatively charged WC surface and bromoxynil anions. Deprotonation of ametryne with increase in pH over the low pH range increased its fraction of molecular form and thus adsorption on WC by 15%/unit pH. Further increase in pH resulted in a 20%/unit pH decrease in ametryne adsorption by WC due primarily to the development of a negative charge on the surface of WC. The pH-dependent adsorption of pesticides by black carbon may significantly influence their environmental fate in soils.  相似文献   

6.
Chun He  Xijun Hu 《Adsorption》2012,18(5-6):337-348
A?novel ordered mesoporous carbon containing basic nitrogen functional groups was synthesized by ammonia-tailoring at a temperature of 1173?K and was applied for reactive dye adsorption. The basic nitrogen-containing functional groups incorporated into the carbon surface could enhance the dispersive interactions between the carbon and dye molecules due to the electron-donating effect as well as the electrostatic interactions between the carbon surface and the anions of the dyes. It was found that this novel functionalized ordered mesoporous carbon could increase the adsorption capacity of reactive red 2 at 298?K by around 40?% and 100?% as compared with the unmodified carbon and a commercial activated carbon, respectively. The Freundlich isotherm showed better correlation with the experimental adsorption data of ammonia-tailored samples than the Langmuir isotherm due to the increased surface heterogeneity induced by the nitrogen-containing functional groups. Adsorption of reactive red 2 was an endothermic process as the adsorption capacity increased with increasing temperature. Low desorption efficiency revealed that the adsorption of reactive red 2 on the modified CMK-3 was extremely favorable, tending to be weakly reversible.  相似文献   

7.
A study was conducted on batch and column competitive adsorption of fluroxypyr (FLX) and tannic acid (TA) from distilled (DW) and tap water (TW) on activated carbon cloth (ACC) and granular activated carbon (GAC). Thermal desorption of the adsorbates from the spent ACC was also studied. FLX adsorption was higher from TW than from DW at low FLX equilibrium concentrations, and the inverse was observed at high FLX concentrations. The presence of TA diminished the amount of FLX adsorbed from both solvents due to partial blocking of the microporosity, but the same trends as before were observed at low and high FLX concentrations. Carbon consumption, obtained from the breakthrough curves, was lower as a function of superficial contact time with ACC than with GAC. The presence of TA increased carbon consumption, which was related to the microporosity of the adsorbents. Thermal desorption profiles of the spent ACC showed two peaks and one peak after adsorption from DW and TW, respectively. Desorption peaks shifted to higher temperatures with an increase in the heating rate, allowing the apparent activation energies and pre-exponential factors of the desorption processes to be determined.  相似文献   

8.
In this paper we report on the synthesis, characterization and use of monocarboxy-phthalocyanine-single walled carbon nanotube conjugates in the electrocatalysis of amitrole and diuron. UV-Vis, FTIR and XRD spectroscopies were used in the characterization of cobalt(II)-tris(benzyl-mercapto)-mono(carboxyphenoxy)-phthalocyanine conjugates (CoMCPc-PA-SWCNT(linked)), while AFM was used to show changes in surface morphologies of the modified electrodes. Cyclic voltammetry and chronoamperometry were used for the electrocatalytic oxidation of amitrole and diuron on the modified glassy carbon electrode. The catalytic rate constants for amitrole and diuron were found to be 1.83 × 106 and 1.99 × 106 M−1 s−1, respectively. The linear range for both was 1.0 × 10−5-2.0 × 10−4 M, with sensitivities of 5.10 and 3.70 A mol−1 L cm−2 for amitrole and diuron, respectively. The limits of detection were estimated to be 0.14 and 0.20 μM for amitrole and diuron, respectively, using the 3δ notation.  相似文献   

9.
The production and consumption of cassava (Manihot esculenta) occur in several places worldwide, producing large volumes of waste, mostly in the form of bark. This study sought to bring a new purpose to this biomass through producing activated carbon to use as an adsorbent to remove the herbicide Diuron from water. It was observed that the carbon contains the functional groups of methyl, carbonyl, and hydroxyl in a strongly amorphous structure. The activated carbon had a surface area of 613.7 m2 g−1, a pore volume of 0.337 cm3 g−1, and a pore diameter of 1.18 nm. The Freundlich model was found to best describe the experimental data. It was observed that an increase in temperature favored adsorption, reaching a maximum experimental capacity of 222 mg g−1 at 328 K. The thermodynamic parameters showed that the adsorption was spontaneous, favorable, and endothermic. The enthalpy of adsorption magnitude was consistent with physical adsorption. Equilibrium was attained within 120 min. The linear driving force (LDF) model provided a strong statistical match to the kinetic curves. Diffusivity (Ds) and the model coefficient (KLDF) both increased with a rise in herbicide concentration. The adsorbent removed up to 68% of pollutants in a simulated effluent containing different herbicides. Activated carbon with zinc chloride (ZnCl2), produced from leftover cassava husks, was shown to be a viable alternative as an adsorbent for the treatment of effluents containing not only the herbicide Diuron but also a mixture of other herbicides.  相似文献   

10.
This work has as objective the study about the adsorption behavior of fatty acids (acetic, propionic, and butyric) on activated carbon and on modified and unmodified montmorillonite clays as a function of temperature and initial concentration of the adsorbate, through adsorption isotherms and their thermodynamic parameters (ΔG, ΔH, and ΔS). The activated carbon presented a higher adsorption capacity due to its relatively large surface area, compared to others adsorbents. The polar characteristic of fatty acids decreased with the increase in the length of non-polar hydrocarbon chain, improving the affinity between the activated carbon (non-polar adsorbent) and the acids. The adsorption capacity of modified montmorillonite (polar adsorbent) was favored due to the presence of the organic cation among its layers, which make the surface more hydrophobic and organophilic when compared to the unmodified montmorillonite surface. The amount of fatty acids adsorbed in the adsorbents surface increased with the concentration, at constant temperature, and decreased with the increase of temperature, at constant concentration. The amount of fatty acids adsorbed in the three adsorbents was related to the surface area and polarity of the adsorbent, concentration and solubility of the adsorbate and temperature of the solution. The negative values of ΔG and ΔH showed that the adsorption on activated carbon and on modified and unmodified montmorillonite clays was a spontaneous and an exothermic process. The decrease in the values of ΔG, with the increase of temperature, demonstrated that the adsorption was benefited by the high temperature and the positive values of ΔS showed that the fatty acids molecules were in a more randomic condition in the adsorbed state than in solution. The experimental results obtained at the temperatures of (298, 303, 313, and 323) K showed that experimental data were well represented by the Langmuir and Freundlich isotherms models.  相似文献   

11.
Ionic liquids (ILs) are considered as emergent pollutants as their synthesis and further use at a large scale might generate environmental problems. The adsorption on activated carbons represents one of the most effective methods to remove ionic liquids and other micropollutants from wastewater. In this work, the adsorption properties on an activated carbon cloth of two pyridinium ionic liquids (4-tert-butyl-1-propylpyridinium bromide (IL1) and 4-tert-butyl-1-(2-carboxyethyl)pyridinium bromide (IL2)) newly synthesized, were compared with the ones of ibuprofen. The adsorption kinetics and isotherms were studied at pH 3 and 7.5. The adsorption thermodynamic parameters calculated from the isotherms indicate an exothermic process, typical of physisorption. The adsorption kinetics of a mixture of the molecules show a competition between ibuprofen and IL2. The location of each adsorbed ionic liquid and ibuprofen into the porosity of the activated carbon cloth was determined from N2 (at 77 K) and CO2 adsorption isotherms (at 273 K). The purification process of an effluent containing the ionic liquids and the ibuprofen in mixture or in single solute could be workable by adsorption on an activated cloth.  相似文献   

12.
Adsorption isotherms of NaCl on activated carbon cloth (ACC) and titania-incorporated activated carbon cloth (Ti-ACC) under an electric field were investigated to deduce the role of titania in capacitive deionization (CDI) of NaCl. Electrosorption of NaCl on the ACC was significantly increased by titania incorporation, whereas its physical adsorption was considerably decreased, resulting in an improved performance of the Ti-ACC as a CDI electrode. Langmuir isotherms based on a localized and fixed amount of adsorption were suitable for the simulation of electrosorption and physical adsorption of ions on the ACC electrodes. The variances of q(m) and b of Langmuir isotherms with electric potential indicate increases in the number of ions per adsorption site and in electrosorption strength of ions by titania incorporation. A cyclic voltammetric study for ion adsorption on ACC electrodes confirms the reversibility between electrosorption and desorption of ions, regardless of titania incorporation.  相似文献   

13.
The effects of carbon chain length and temperature were investigated on adsorption kinetics and surface tension of a group of slightly volatile, short carbon chain molecules: 1-octanol, 1-hexanol, and 1-butanol. Experiments were performed in a closed chamber where simultaneous adsorption from both sides of the vapor/liquid interface was considered. The dynamic (time dependent) and steady-state surface tensions were found to decrease with temperature ranging from 10 °C to 35 °C. It was shown that, at the final steady-state, the effect of adsorption from the vapor phase was much more important than that from the liquid phase especially for short carbon chain molecules (e.g., 1-butanol). The modified Langmuir equation of state and modified kinetic transfer equation, which account for adsorption from both sides of a vapor/liquid interface, were used to model the experimental data of the steady-state and dynamic surface tension, respectively. Modeling results showed that the equilibrium constants and adsorption rate constants were increased with temperature and carbon chain length. The maximum surface concentration showed a decrease with temperature and an increase with carbon chain length. Some variations in the fitting parameters were observed in the dynamic modeling. These variations may be due to the experimental errors or the limitations of the proposed model.  相似文献   

14.
为研究影响碳基吸附剂吸附超临界温度气体的主要因素,选择石墨化热解碳黑BP280和Ajax活性炭,分析超临界温度高压甲烷在其上的吸附平衡。应用容积法,在压力0~20.5 MPa、温度253 K~313 K测定甲烷的吸附平衡数据,并由等量吸附线标绘和亨利定律常数确定等量吸附热。引入通用吸附等温方程,再由方程的Langmuir标绘确定最大吸附容量,进而通过方程的线性化计算吸附平衡态中甲烷分子的作用能。结果表明,甲烷在两种吸附剂上的最大吸附容量均随温度而变化,并都小于液态甲烷的密度;甲烷在碳黑和活性炭上的等量吸附热分别为11.9 kJ/mol~12.5 kJ/mol和17.5 kJ/mol~22.5 kJ/mol,体现了两种吸附剂不同的表面能量分布;甲烷分子间作用能随吸附量的变化特点反映了超临界温度甲烷以类似于压缩气体状态聚集的特点和吸附剂结构上的差异。碳基吸附剂的比表面积和微孔容积是影响其储存甲烷容量的重要因素。  相似文献   

15.
This objective of this work was to summarize the main results obtained in previous papers related to the adsorbent-adsorbate interactions involved in the adsorption of naphthalenesulphonic acids and heavy metals (Cd(II) or Hg(II)) by modified activated carbons. The adsorption of organic compounds (1-naphthalenesulphonic acid, 1,5-naphthalenedisulphonic acid and 1,3,6-naphthalenetrisulphonic acid) and inorganic species (Cd(II) and Hg(II)) was studied on a series of ozonized activated carbon in aqueous phase. Commercial activated carbon (Filtrasorb 400) was treated with different ozone doses to study the effect of ozone treatment on its surface properties and investigate the behavior of the treated carbon samples in the above adsorption processes. After ozonation, carbonyl- and carboxyl-type groups were generated on the carbon surface. The action of ozone also affected the textural characteristics of the carbon; thus, the surface area diminished due both to the ozone attack and to the increase in oxygenated groups, which prevented the diffusion of nitrogen by obstructing micropore entrances. The capacity of activated carbon to adsorb naphthalenesulphonic acids sharply decreased with a greater number of sulphonic groups in the aromatic rings of these acids. As the concentration of oxygenated electron-withdrawing groups on the carbon surface increased, a significant reduction in adsorption capacity was observed. In all cases, the adsorption uptake decreased with higher solution pH. The adsorption of metallic ions, Cd(II) and Hg(II), by this series of ozonized activated carbons was also studied. In the case of Cd(II), the adsorption capacity and affinity of the adsorbents increased with a higher concentration of acid oxygenated groups on the activated carbon surface. In the case of Hg(II), the adsorption diminished with an increase in the degree of oxidation of the activated carbon. The adsorption of 1,3,6-naphthalenetrisulphonic acid on the ozonized carbons was also studied in the presence of Cd(II) and Hg(II). The presence of Cd(II)) in the medium enhanced the sulphonic acid uptake, mainly for the most ozonized activated carbon sample, whereas the presence of Hg(II) had no significant effect on the adsorption.  相似文献   

16.
A sensitive LC–electrospray MS–MS method using off-line solid-phase extraction for the determination of diuron and Irgarol 1051 has been developed, enabling determination of both compounds at sub-ppt levels. Diuron and Irgarol 1051 are used as alternatives for tributyltin in antifouling paints that prevent growth on boats, and an increase in their application is anticipated because of the upcoming ban on tributyltin in 2003. In 2000, a survey was carried out to assess contamination with diuron and Irgarol 1051 of a number of Dutch marinas and coastal waters. Depending on the time of year, both compounds were encountered at levels higher than the maximum permissible concentrations of 430 and 24 ng/l for diuron and Irgarol 1051, respectively. Outside marinas at reference locations, concentrations were much lower, depending on the geographical situation and the nature of the water exchange with the environment related to tidal cycles. A seasonal influence was observed with highest levels in summer, corresponding to the yachting season for both compounds. For diuron, use in agriculture could have contributed to the high concentration encountered in surface waters.  相似文献   

17.
A study has been made on the effect of pH upon the equilibrium adsorption capacity of triethyl phosphate, dimethyl phosphate and orthophosphate on to activated carbon cloth. It is shown that for molecular phosphates no dependence upon pH exists, whilst the adsorption of ionic phosphates exhibit a strong pH dependence. These adsorption trends may be explained in terms of pKa values, ionic strength and the surface charge of the activated carbon cloth is aqueous solution.  相似文献   

18.
We found that activated carbon effectively removed urea from solution and that urea adsorption onto activated carbon followed a pseudo-second-order kinetic model. We classified the urea adsorption on activated carbon as physical adsorption and found that it was best described by the Halsey adsorption isotherm, suggesting that the multilayer adsorption of urea molecules on the adsorption sites of activated carbon best characterized the adsorption system. The mechanism of adsorption of urea by activated carbon involved two steps. First, an amino (–NH2) group of urea interacted with a carbonyl (–C?O) group and a hydroxyl (?OH) group on the surface of activated carbon via dipole–dipole interactions. Next, the –C?O group of the urea molecule adsorbed to the activated carbon interacted with another –NH2 group from a second urea molecule, leading to multilayer adsorption.  相似文献   

19.
The present study aimed to explore the possibility of increasing the purification efficacy of ozone in the removal of high-toxicity contaminants by using carbons of basic character and to analyze the mechanism involved in this process. These carbons were prepared by treating a commercial activated carbon (Witco, W) with ammonia (W-A), ammonium carbonate (W-C), or urea (W-U), under high pressure and temperature. The ammonia and carbonate treatments slightly increased the mesoporosity and, to a greater degree, the macroporosity of carbon W, whereas the urea treatment produced an increase in the porosity across the whole range of pore sizes. In addition, treatment of the activated carbon with these nitrogenating agents produced a marked change in the chemical nature of its surface. Thus, according to the pH of the point of zero charge (pHPZC) values obtained for each sample, carbon W was neutral (pHPZC = 7.12), but the treated carbons were basic, especially carbon W-U (pHPZC = 8.85). This basicity results from an increased concentration of basic oxygenated and nitrogenated surface functional groups, as confirmed by the results of elemental and XPS analyses. An increase in the degradation of 1,3,6-naphthalenetrisulfonic acid was observed when the activated carbon samples were added to the system. This degradation was especially enhanced in the presence of carbon W-U. The increased NTS degradation rate in the presence of the activated carbon is due to an increased concentration of highly reactive radicals in the system. When the catalytic activity of the activated carbon samples was related to their chemical and textural characteristics, it was found that: (i) The catalytic activity increased with an increase in the surface basicity. Interestingly, in the sample with greatest catalytic activity in NTS ozonation, carbon W-U, most of the nitrogenated surface groups introduced were pyrrol groups. These groups increase the electronic density of the basal plane of the activated carbon, thereby enhancing the reduction of ozone on the surface and the generation of highly reactive radicals in the system. (ii) The greater catalytic activity of carbon W-U may also be partly related to its greater surface area and higher volume of mesopores and macropores; these large pores facilitate access of the ozone to the surface active centers of the carbon, increasing its catalytic activity. The presence of the activated carbon samples during NTS ozonation also favored the removal of total organic carbon present in the solution, due to (a) transformation of organic matter into CO2 through the generation of highly reactive species catalyzed by the presence of the activated carbons (catalytic contribution) and (b) adsorption of NTS oxidation byproducts on the activated carbon (adsorptive contribution). The results obtained show that activated carbons treated with nitrogenating agents are very promising catalysts for application in the ozonation of aromatic compounds.  相似文献   

20.
The adsorption by a coal-based mesoporous activated carbon of humic acids (HAs) isolated from two Polish lignites was studied. For comparison, a commercial Aldrich humic acid was also included into this study. The differences in chemical structure and functional groups of HAs were determined by elemental analysis and infrared spectroscopy DRIFT. Two activated carbons used differed in terms of mesopore volume, mesopore size distribution, and chemical properties of the surface. The kinetics of adsorption of HAs have been discussed using three kinetic models, i.e., the first-order Lagergren model, the pseudo-second-order model, and the intraparticle diffusion model. It was found that the adsorption of HAs from alkaline solution on mesoporous activated carbon proceeds according to the pseudo-second-order model. The correlation coefficients were close to 1. The intraparticle diffusion of HA molecules within the carbon particle was identified to be the rate-limiting step. Comparing the two activated carbons, the carbon with a higher volume of pores with widths of 10-50 nm showed a greater removal efficiency of HA. An increase in the Freundlich adsorption capacity with decreasing carbon content of HA was observed. Among the HAs studied, S-HA shows characteristics indicating the highest contribution of small-size fraction. The S-HA was removed by both activated carbons to the highest extent. The effect of pH solution on the adsorption of HA was examined over the range pH 5.4-12.2. It was found that the extent of adsorption decreased with decreasing pH of the solution.  相似文献   

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