Adsorptive selenite removal from water using iron-coated GAC adsorbents

Removal of selenite from aqueous phase using iron-coated granular activated carbons (GAC) was investigated in this study. Five different types of GAC were used for iron coating by oxidizing ferrous chloride with sodium hypochlorite and the iron-coated GAC (Fe-GAC) were tested for selenite removal. Nitrogen adsorption-desorption analyses indicated that Brunauer-Emmett-Teller (BET) specific surface area, pore size, and pore volume decreased with the iron coating. The Darco 12x20 GAC was shown to be the most effective adsorbent among the five tested GACs after iron coating. Among the different concentrations used for iron coating, the Darco 12x20 GAC coated with 0.1M ferrous chloride achieved the highest selenite removal (97.3%). High removal efficiency of selenite occurred in a wide range of pH (i.e., 2-8), but the efficiency decreased when pH was higher than 8. Adsorption kinetics showed that selenite removal efficiency reached more than 90% after 6-h adsorption for initial selenium concentration of 2mg/L and equilibrium was obtained after 48h. A pseudo-second-order kinetic model was found to characterize the adsorption kinetics well for all the initial selenium concentrations and temperatures tested (R(2)>/=0.9969). Three temperatures (25, 35, 45 degrees C) were used to examine temperature effect on the adsorption behavior of the Fe-GAC with initial selenium concentration of 1mg/L. Activation energy was calculated to be 30.42kJ/mol. Adsorption isotherms for initial selenium concentration of 2mg/L at various temperatures and ionic strengths were developed and the data generally fit the Langmuir model well (R(2)>/=0.994). The adsorption capacity reached as high as 2.50mg-Se/g-adsorbent at equilibrium for initial concentration of 2mg/L at 25 degrees C. The Gibbs free energy was determined to be negative, indicating the spontaneous nature of the adsorption reaction. Oxyanion competitive adsorption showed that sulfate (0.1-5mM) barely affected selenite adsorption. Other anions (phosphate, silicate and carbonate) impact selenite adsorption to various degrees with phosphate completely excluded selenite adsorption at 5mM. The possible adsorption mechanisms were discussed.     

Comparison between thermal and ozone regenerations of spent activated carbon exhausted with phenol

Thermal and ozone regenerations of granular activated carbons (GAC) used in the removal of phenol from aqueous solution have been studied. The phenol isotherms for virgin GAC could be well represented by the Langmuir equation. Direct ozonation of GAC introduced large amounts of acidic surface oxygen groups, which caused a decrease in the phenol uptake. Thermogravimetric methods were used to investigate the mechanism of phenol adsorption onto virgin and ozonated carbons. Thermal regeneration was carried out at 1123K using nitrogen (pyrolysis alone) or nitrogen and carbon dioxide (pyrolysis plus oxidation). Results showed that spent carbons do not recover their adsorption characteristics when heated under inert conditions whereas carbon dioxide regeneration was effective at about 15% wt burn-off. Regeneration of GAC was also carried out with ozone as oxidizing gas at room temperature. Ozone dose and the nature of GAC have much influence on the regeneration performance. For an individual GAC there exits an optimum ozone dose for which phenol is eliminated together with most of its oxidation by-products without incurring in carbon surface chemical alterations. However, if excessive ozone is applied some acidic surface groups are formed on the GAC, thereby decreasing the adsorption capacity for phenol. Results showed that spent carbons can recover most of their adsorption characteristics and specific surface areas when regenerated through a number of adsorption-ozone regeneration cycles.     

Fenton-driven chemical regeneration of MTBE-spent GAC

Methyl tert-butyl ether (MTBE)-spent granular activated carbon (GAC) was chemically regenerated utilizing the Fenton mechanism. Two successive GAC regeneration cycles were performed involving iterative adsorption and oxidation processes: MTBE was adsorbed to the GAC, oxidized, re-adsorbed, oxidized, and finally re-adsorbed. Oxidant solutions comprised of hydrogen peroxide (H2O2) (1.7-2.0%) and FeSO4 x 7H2O (3 g/L) (pH 2.5), were recirculated through the GAC column (30% bed expansion). The regeneration efficiency after two full cycles of treatment was calculated to be 91%. The cost of H2O2 was 0.59 dollars/kg GAC (0.27 dollars/lb) per regeneration cycle. There was no loss of sorptive capacity. Small reductions in carbon surface area and pore volume were measured. The lack of carbon deterioration under aggressive oxidative conditions was attributed to the oxidation of the target contaminants relative to the oxidation of carbon surfaces. The reaction byproducts from MTBE oxidation, tertiary butanol and acetone, were also degraded and did not accumulate significantly on the GAC. Excessive accumulation of Fe on the GAC and consequent interference with MTBE sorption and carbon regeneration was controlled by monitoring and adjusting Fe in the oxidative solution.     

IMPROVING THE PERFORMANCE OF GRANULAR ACTIVATED CARBON (GAC) VIA PRE-REGENERATION ACID TREATMENT

A lab-scale acid treatment system was developed to Investigate the effects of hydrochloric acid on the removal of calcium from field spent GAC (FSGAC). The effects of acid treatment on the subsequent regeneration process and regenerated GAC properties were also investigated using a lab-scale furnace. A linear relationship between calcium remaining on the GAC following acid treatment and GAC mass losses during regeneration was exhibited. FSGAC treated with 0.1 N hydrochloric acid resulted in 7.5% lower mass losses than non-acid treated GAC. An increase in total surface area of 7.2% and micropore volume of 3.1% was also noted following acid treatment and regeneration. This was due to a reduction in calcium-catalysed gasification of the GAC structure, which may have occurred in samples, which had not received acid treatment. Improvements in porosity, adsorption capacity and surface chemistry indicate that acid treatment is an effective process, which may be used to provide superior regenerated GAC product.     

Regeneration of acid orange 7-exhausted granular activated carbons with microwave irradiation

An investigation was performed for the regeneration of three granular activated carbons (GACs) exhausted with acid orange 7 (AO7). The three GACs were made from different materials, i.e. coconut shells, almond nucleus and coal. The AO7 adsorption process was carried out in a continuous-flow adsorption column. After adsorption, the AO7-saturated GAC was dried at 120 °C, then regenerated in a quartz reactor by 2450 MHz microwave (MW) irradiation at 850 W for 5 min. The efficacy of this procedure was analyzed by determining the rates and amounts of AO7 adsorbed in successive adsorption–MW regeneration cycles. Effects of this regeneration on the structural properties, surface chemistry and the AO7 adsorption capacities of GAC samples were examined. It was found that after several adsorption–MW regeneration cycles, the adsorption rates and capacities of GACs could maintain relatively high levels, even higher than those of virgin GACs, as indicated by AO7 breakthrough curves and adsorption isotherms. The improvement of GAC adsorption properties resulted from the modification of pore size distribution and surface chemistry by MW irradiation.     

Removal of trivalent and hexavalent chromium with aminated polyacrylonitrile fibers: performance and mechanisms

Aminated polyacrylonitrile fibers (APANFs) were prepared and used as an adsorbent in a series of batch adsorption experiments for the removal of Cr(III) and Cr(VI) species from aqueous solutions of different pH values. The results show that significant amounts of Cr(III) or Cr(VI) species can be adsorbed by the APANFs, although the adsorption performances was greatly dependent upon the solution pH values. In general, the amounts of adsorption for Cr(III) species increased whereas that for Cr(VI) decreased with the increase of the solution pH values, which suggests that different adsorption mechanisms dominated the removal of Cr(III) or Cr(VI) species on the APANFs. X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy revealed that the adsorption of Cr(III) species on the APANFs was largely attributed to the formation of surface complexes between the nitrogen atoms on the APANFs and the Cr(III) species adsorbed, but the adsorption of Cr(VI) species on the APANFs was more likely effected through the formation of hydrogen bonds at high solution pH values or through both electrostatic attraction and surface complexation at low solution pH values. It was found that the Cr(VI)-adsorbed APANFs can be effectively regenerated in a basic solution and be reused almost without any loss of the adsorption capacity, while the Cr(III)-adsorbed APANFs needed to be regenerated in an acidic solution and the regeneration appeared to be less effective.     

Wet peroxide oxidation of chlorophenols

This study evaluates the application of Wet Peroxide Oxidation (WPO) for the treatment of solutions containing 4-chlorophenol (4-CP) and 2,4-dichlorophenol (2,4-DCP). These compounds are of special interest due to their high toxicity and low biodegradability. WPO is included in the Advanced Oxidation Processes, which are technologies based on an initial formation of hydroxyl radicals that further oxidize the organic matter. The influence of some operating conditions such as temperature, dosage of hydrogen peroxide and initial concentration of the chlorophenols was studied in absence of a catalyst. The results of this study prove that 4-CP and 2,4-DCP can be completely removed from wastewaters by means of WPO. Total Organic Carbon (TOC) and 4-CP removals of 72.3% and 100%, respectively, were achieved working at 100 degrees C with 2.5 mL of H(2)O(2) and an initial concentration of 500 ppm of 4-CP after 90 min of reaction. Under the same conditions but with an initial concentration of 500 ppm of 2,4-DCP a TOC removal of 59% and a complete removal of the target compound were achieved.     

Competitive adsorption of benzoic acid and p-nitrophenol onto activated carbon: isotherm and breakthrough curves

Three series of batch tests at 25 degrees C were performed to determine the benzoic acid and p-nitrophenol (PNP) binary adsorption isotherms onto GAC in the aqueous solutions and the experimental data were fitted to the extended Langmuir isotherm model successfully. The experimental data and the isotherm model parameters showed that the GAC used in this study had a higher affinity to PNP than benzoic acid. Three column tests were performed to determine the breakthrough curves and effluent solution pH with varying feed compositions. According to the experimental results, the weakly adsorbed BA exhibited an intermediate zone of effluent concentration higher than its feed one; the effluent solution pH could serve as a good indicator for breakthrough. The breakthrough curves with varying feed compositions could be predicted by the non-linear wave propagation theory satisfactorily. Only the adsorption isotherm models were required to construct the composition path diagram with which the breakthrough curves could be predicted.     

The regeneration of field-spent granular-activated carbons.

The thermal regeneration of field-spent granular-activated carbons (GAC) is being increasingly adopted as a cost-effective alternative to disposal. The success of this practice requires the adjustment of process conditions to maximise the recovery of the original carbon characteristics while minimising carbon loss. This paper describes an investigation into the regeneration of several field-spent GAC representative of those typically generated by the drinking water treatment industry. The carbons were initially investigated for their ash contents and inorganic compositions in order to determine the accumulation of metallic species that affect the regeneration process. Regeneration was conducted in steam at 800 degrees C over reaction times between 0 and 60 min in order to achieve different degrees of carbon gasification. Weight losses were determined for each condition and the resulting carbons characterised for their apparent density, porosity, surface area and aqueous adsorption characteristics. Results showed that spent carbons recovered most of their adsorption characteristics when heated to 800 degrees C under inert conditions. Steam gasification in the range of 5-10 wt% burn-off had some positive effects on the characteristics of the spent carbons which were in most cases counteracted by a reduction in the carbon yield. Steam gasification in excess of 15 wt% burn-off caused a rapid increase in the carbon mesoporosity but a significant deterioration in the carbon microporosity, BET surface area and adsorption capacity for organic species of small molecular size.     

Electrochemical regeneration of field spent GAC from two water treatment plants

The effectiveness of on-site thermal regeneration of field-spent granular activated carbon (GAC) from two municipal drinking water facilities was compared with bench-scale electrochemical regeneration, a novel regeneration technology. The regeneration method was evaluated using aqueous natural organic material (NOM) adsorption, iodine number analysis, and surface area analysis. In contrast to the large electrochemical regeneration efficiencies reported in the literature for GAC loaded with phenolics and other individual organic compounds, the electrochemical reactor tested was only able to regenerate 8-15% of the NOM adsorption capacity of the field spent GAC. In contrast, thermal reactivation achieved up to 103% regeneration efficiency. To more accurately assess the efficiency of regeneration processes for water treatment applications, GAC should be loaded in continuous-flow columns and not batch rectors. The iodine number analysis yielded higher efficiency values, however it did not give an accurate estimate of the regeneration efficiency. The small changes in GAC pore size distribution were consistent with the low electrochemical regeneration efficiencies. These low efficiencies appear to be related to the low reversibility of NOM adsorption and to pH-induced adsorbate desorption being the primary mechanism for this type of electrochemical regeneration system.     

Magnetic powder MnO-Fe2O3 composite--a novel material for the removal of azo-dye from water

Fine powder adsorbents or catalysts often show better adsorptive or catalytic properties, but they encounter the difficulties of separation and recovery in application. In this study, four inexpensive magnetic powder MnO-Fe2O3 composites used as adsorbent-catalyst materials were prepared and characterized. These materials could be recovered efficiently by a magnetic separation method. Their adsorptive properties for the removal of an azo-dye, acid red B (ARB), from water and the regeneration of adsorbents containing ARB by catalytic combustion was studied. These powder adsorbents showed excellent adsorption towards ARB under acidic conditions. A very fast adsorption rate was observed and could be well described by a pseudo-second-order kinetics model. The adsorption capacity increased with increasing Fe content and surface area of the adsorbent, and the highest adsorption capacity of 105.3 mg/g was obtained at pH 3.5. The adsorption was not affected by the presence of Cl-, but was significantly affected by SO4(2-). The adsorbent containing ARB can be regenerated by catalytic combustion of adsorbed ARB at 400 degrees C in air. Laboratory experiments demonstrated that this material is reusable.     

Iron amendment and Fenton oxidation of MTBE-spent granular activated carbon

Fenton-driven regeneration of methyl tert-butyl ether (MTBE)-spent granular activated carbon (GAC) involves an Fe amendment step to increase the Fe content and to enhance the extent of MTBE oxidation and GAC regeneration. Four forms of iron (ferric sulfate, ferric chloride, ferric nitrate, ferrous sulfate) were amended separately to GAC. Following Fe amendment, MTBE was adsorbed to the GAC followed by multiple applications of H₂O₂. Fe retention in GAC was high (83.8-99.9%) and decreased in the following order, FeSO₄·7H₂O > Fe₂(SO₄)₃·9H₂O > Fe(NO₃)₃·9H₂O > FeCl₃. A correlation was established between the post-sorption aqueous MTBE concentrations and Fe on the GAC for all forms of Fe investigated indicating that Fe amendment interfered with MTBE adsorption. However, the mass of MTBE adsorbed to the GAC was minimally affected by Fe loading. Relative to ferric iron amendments to GAC, ferrous iron amendment resulted in lower residual iron in solution, greater Fe immobilization in the GAC, and less interference with MTBE adsorption. MTBE oxidation was Fe limited and no clear trend was established between the counter-ion (SO₄²⁻, Cl⁻, NO₃⁻) of the ferric Fe amended to GAC and H₂O₂ reaction, MTBE adsorption, or MTBE oxidation, suggesting these processes are anion independent.     

树脂基水合氧化铈复合材料深度去除污水中磷酸盐

通过"前驱体导入-原位沉积"的工艺路线,将水合氧化铈(HCO)纳米颗粒负载入强碱阴离子交换树脂(SAE)孔道内,制得复合纳米吸附剂HCO@SAE并用于污水中磷酸盐的深度去除。试验结果表明:与其母体材料SAE、粉末活性炭(PAC)和大孔吸附树脂XAD-4相比,HCO@SAE具有最佳的磷酸盐吸附性能。溶液pH值对HCO@SAE吸附磷酸盐的性能有较大影响,且在中性条件下可获得最大的磷酸盐吸附量(30.96 mgP/g)。得益于负载HCO纳米颗粒对磷酸盐的专属内配位络合作用,HCO@SAE能够在共存高浓度竞争离子的条件下实现对磷酸盐的选择性吸附。采用NaOH-NaCl混合溶液作为脱附剂可实现对吸附饱和HCO@SAE的高效再生,再生后吸附性能保持稳定,从而实现多批次循环吸附操作。     

Removal of MIB and geosmin using granular activated carbon with and without MIEX pre-treatment

This study assessed the impact of MIEX pre-treatment, followed by either coagulation or microfiltration (MF), on the effectiveness of pilot granular activated carbon (GAC) filters for the removal of the taste and odour compounds, 2-methylisoborneol (MIB) and geosmin, from a surface drinking water source over a 2-year period. Complete removal of MIB and geosmin was achieved by all GAC filters for the first 10 months, suggesting that the available adsorption capacity was sufficient to compensate for differences in dissolved organic carbon (DOC) entering the GAC filters.Reduction of empty bed contact time (EBCT), in all but one GAC filter, resulted in breakthrough of spiked MIB and geosmin, with initial results inconclusive regarding the impact of MIEX pre-treatment. MIB and geosmin removal increased over the ensuing 12 months until complete removal of both MIB and geosmin was again achieved in all but one GAC filter, which had been pre-chlorinated. Autoclaving and washing the GAC filters had minimal impact on geosmin removal but reduced MIB removal by 30% in all but the pre-chlorinated filter, confirming that biodegradation impacted MIB removal. The impact of biodegradation was greater than any impact on GAC adsorption arising from DOC differences due to MIEX pre-treatment. It is not clear whether, at a lower initial EBCT, MIEX pre-treatment may have impacted on the adsorption capacity of the virgin GAC.The GAC filter maintained at the longer EBCT, which was also pre-chlorinated, completely removed MIB and geosmin for the period of the study, suggesting that the greater adsorption capacity was compensating for any decrease in biological degradation.     

Electrochemical regeneration of Fe2+ in Fenton oxidation processes

This study is to establish optimal conditions for the minimization of iron sludge produced in Fenton oxidation processes by electro-regenerating Fe(2+) with constant potential (CPM) or constant current mode (CCM). Results indicate that the optimal cathodic potential for Fe(2+) regeneration is -0.1 V vs. the saturated calomel electrode (SCE) in terms of current efficiency. Keeping the initial Fe(3+) concentration ([Fe(3+)](0)) constant, the average current density produced at -0.1 V vs. SCE (CPM) is approximately equal to the optimal current density applied in the CCM. The suitable pH range is below the pH value determined by Fe(3+) hydrolysis. As expected, increasing cathode surface area and solution temperature notably increases Fe(2+) regeneration rate. At the optimal potential, the average current density increases linearly with [Fe(3+)](0), exhibiting a slope of 8.48 x 10(-3)(A/m(2))(mg/L)(-1). The average current efficiency varies with [Fe(3+)](0), e.g., 75% and 96-98% at 100 and > or = 500 mg/L [Fe(3+)](0), respectively. Once reaching 75% of Fe(2+) regeneration capacity, further regeneration becomes difficult due to Fe(3+) mass transfer limitation. Fe(2+) can also be effectively regenerated by dissolving iron sludge at low pH (usually 相似文献   

The simultaneous removal of calcium and chloride ions from calcium chloride solution using magnesium-aluminum oxide

We investigated the removal of Ca(2+) and Cl(-) from CaCl(2) solution at 20-60 degrees C, using magnesium-aluminum oxide, Mg(0.80)Al(0.20)O(1.10), prepared by the thermal decomposition of a hydrotalcite-like compound, Mg(0.80)Al(0.20)(OH)(2)(CO(3))(0.10).0.78 H(2)O. The degree of Ca(2+) and Cl(-) removal from the solution increased with increasing initial CaCl(2) concentration, temperature, and quantity of Mg(0.80)Al(0.20)O(1.10) added. When Mg(0.80)Al(0.20)O(1.10) was added to 0.25 M CaCl(2) solution in a Mg(0.80)Al(0.20)O(1.10)/CaCl(2) molar ratio of 20, the degree of Ca(2+) and Cl(-) removal from the solution at 60 degrees C after 0.5 h was 93.0% and 98.2%, respectively. These results reveal that Mg(0.80)Al(0.20)O(1.10) has the capacity to remove Ca(2+) and Cl(-) simultaneously from aqueous solution.     

Removal of chromium from aqueous solutions by diatomite treated with microemulsion

In order to evaluate the sorption of heavy metals, a crude diatomite was impregnated with a microemulsion which showed remarkable increase in chromium sorption capacity as compared to untreated diatomite. Samples with two different granulometries were investigated, both yielding practically complete adsorption. The adsorption process is pH dependent and the best results for the initial Cr (III) concentration of 1.5 g/L were obtained at pH 2.95. The effect of the concentration of the chromium synthetic solution was also investigated. The adsorption isotherms were obtained (30. 40 and 50 degrees C) and the Freundlich and Langmuir models were used to determine the adsorption capacity of the adsorbent. Following the adsorption step, a desorption process was carried out using several eluant solutions. The best results were obtained using hydrochloric acid (100%) as eluant.     

Removal of estrone and 17beta-estradiol from water by adsorption

Endocrine disrupting chemicals (EDCs) are the focus of current environment concern, as they can cause adverse health effects in an intact organism, or its progeny, subsequent to endocrine function. The paper reports on the removal of estrone (E1) and 17beta-estradiol (E2) from water through the use of various adsorbents including granular activated carbon (GAC), chitin, chitosan, ion exchange resin and a carbonaceous adsorbent prepared from industrial waste. The results show that the kinetics of adsorption were adsorbent and compound-dependent, with equilibration being reached within 2 h for a waste-derived carbonaceous adsorbent to 71 h for an ion-exchange resin for E1, and within 7 h for the waste-derived carbonaceous adsorbent to 125 h for GAC for E2. Of all the adsorbents tested, the carbonaceous adsorbent showed the highest adsorption capacity, with a maximum adsorption constant of 87500 ml/g for E1 and 116000 ml/g for E2. The GAC also had a very high adsorption capacity for the two compounds, with a maximum adsorption constant of 9290 ml/g for E1 and 12200 ml/g for E2. The effects of some fundamental environmental parameters including adsorbent concentration, pH, salinity and the presence of humic acid and surfactant on adsorption were studied. The results show that adsorption capacity of activated carbon was decreased with an increase in adsorbent concentration and by the presence of surfactant and humic acid. The results have demonstrated excellent performance of a waste derived adsorbent in removing E1 and E2 from water, and indicated the potential of converting certain solid waste into useful adsorbents for pollution-control purposes.     

Desorption of dye from activated carbon beds: effects of temperature, pH, and alcohol.

The adsorption isotherms of yellow and red dye solutions onto granular activated carbon at varying solution pHs (2-8). temperatures (15-50 degrees C), and alcohol concentrations (0-20%) were experimentally determined by batch tests and the Tóth model was found to best fit the adsorption isotherm data for varying solution pHs. temperatures, and alcohol concentrations. The maximum adsorption capacity was found to decrease with increasing solution pH and alcohol concentration and could be predicted by the correlation equations obtained in this study. A correlation equation was also obtained to account for the effects of solution temperature on the adsorption equilibrium constant. The 25 degrees C water was found to be a very poor regenerant for the carbon bed presaturated with the yellow dye compared with 20% alcohol solution. A simple equation was derived, based on non-linear wave propagation theory, to predict the desorption curves of activated carbon bed. Given presaturation concentration, bed density and void fraction, and adsorption isotherm, the wave propagation theory predicted the desorption curves quite satisfactorily.