Microwave assisted catalytic wet air oxidation of H-acid in aqueous solution under the atmospheric pressure using activated carbon as catalyst

Catalytic wet air oxidation (CWAO) is a promising method for the treatment of heavily contaminated wastewater. However, its application is restricted due to severe operation conditions (high pressure and high temperature). A microwave (MW) assisted oxidation method was investigated aiming to treat heavily contaminated wastewater under milder conditions. H-acid (1-amino-8-naphthol-3, 6-disulfonic acid) was selected as target compound to evaluate the performance of this novel process. The removal of H-acid and TOC (total organic carbon) for H-acid solution of 3000 mg/L reached as high as 92.6% in 20 min and 84.2% in 60 min, respectively under optimal conditions. The existence of activated carbon and oxygen proved to be critical for effective treatment. The activated carbon acted not only as a catalyst for H-acid decomposition, but also as a special material for the absorption of MW energy. Air was supplied to the reactor as an oxygen source at constant flows. The amino group in H-acid was converted ultimately into nitrate, and sulfonic group into sulfate. This observation gave an evidence of H-acid mineralization although other organic intermediates were unable to be determined. The value of BOD(5)/COD (ratio of 5d biochemical oxygen demand to chemical oxygen demand) increased from 0.008 to 0.467 indicating a significant improvement of biodegradability for the solution, which is beneficial for the further biological treatment of the wastewater.     

Comparisons of sorbent cost for the removal of Ni2+ from aqueous solution by carbon nanotubes and granular activated carbon

The reversibility of Ni2+ sorption by NaOCl oxidized single-walled carbon nanotubes (SWCNTs), multiwalled carbon nanotubes (MWCNTs) and granular activated carbon (GAC) was investigated to evaluate their repeated availability performance in water treatment. Under the same conditions, the SWCNTs and MWCNTs possess more Ni2+ sorption capacities and show better reversibility of Ni2+ sorption and less weight loss after being repeated sorption/desorption processes than the GAC, suggesting that they are effective Ni2+ sorbents and can be reused through many cycles of water treatment and regeneration. A statistical analysis on the replacement cost of these sorbents revealed that SWCNTs and MWCNTs can be possibly cost-effective Ni2+ sorbents in water treatment regardless of their high unit cost at the present time.     

Abatement of phenolic mixtures by catalytic wet oxidation enhanced by Fenton's pretreatment: effect of H2O2 dosage and temperature

Catalytic wet oxidation (CWO) of a phenolic mixture containing phenol, o-cresol and p-cresol (500mg/L on each pollutant) has been carried out using a commercial activated carbon (AC) as catalyst, placed in a continuous three-phase reactor. Total pressure was 16 bar and temperature was 127 degrees C. Pollutant conversion, mineralization, intermediate distribution, and toxicity were measured at the reactor outlet. Under these conditions no detoxification of the inlet effluent was found even at the highest catalyst weight (W) to liquid flow rate (Q(L)) ratio used. On the other hand, some Fenton Runs (FR) have been carried out in a batch way using the same phenolic aqueous mixture previously cited. The concentration of Fe(2+) was set to 10mg/L. The influence of the H(2)O(2) amount (between 10 and 100% of the stoichiometric dose) and temperature (30, 50, and 70 degrees C) on phenols conversion, mineralization, and detoxification have been analyzed. Phenols conversion was near unity at low hydrogen peroxide dosage but mineralization and detoxification achieved an asymptotic value at each temperature conditions. The integration of Fenton reagent as pretreatment of the CWO process remarkably improves the efficiency of the CWO reactor and allows to obtain detoxified effluents at mild temperature conditions and relatively low W/Q(L) values. For a given phenolic mixture a temperature range of 30-50 degrees C in the Fenton pretreatment with a H(2)O(2) dosage between 20 and 40% of the stoichiometric amount required can be proposed.     

负载型Pd催化剂的制备及其对甲醇氧化的催化活性

采用等体积浸渍法制备了一系列负载型Pd+M(M=MgO、CaO、SrO、BaO)催化剂,运用BET、CO-化学吸附、XRD、H2-TPR和XPS等表征手段对催化剂进行了表征,并考察其对甲醇的催化氧化性能。结果表明,添加碱土金属可使Pd粒子高度分散,催化剂表面易还原氧物种量增多,还原速率加快;XPS分析可知,碱土金属可增强Pd-Ce间相互作用,促使Pd向氧化态过渡,同时增加催化剂表面Ce3+浓度,改善催化剂的氧化还原性能,进而提高催化剂的催化活性。助催化效果递变规律为BaOCaOMgOSrO。     

炭气凝胶负载Pt基催化剂的制备及其甲醇氧化催化性能

以间苯二酚(R)和甲醛(F)为原料,制备R-F炭气凝胶(RF-CAs).继以后者为载体采用浸渍还原法制备铂基催化剂Pt/CA,并比较其与由相同负载工艺制得的以Vulcan XC-72为载体的铂基催化剂Pt/XC72的催化甲醇氧化反应的性能.结果表明,前者具明显高的甲醇氧化催化活性,显示CAs是一种极具潜在竞争力的燃料电池催化剂载体材料.     

Preparation of activated carbon@ZnO composite and its application as a novel catalyst in catalytic ozonation process for metronidazole degradation

The present study aimed to investigate the efficiency of granular activated carbon modified with ZnO nanoparticles (GAC@ZnO composite) as a catalyst for metronidazole degradation using catalytic ozonation process. The catalytical properties of GAC@ZnO composite were measured by using FESEM, FT-IR, XRD, EDX, and BET advanced techniques. Also, the effects of pH factor (3, 5, 7, 9, and 11), initial concentration of contaminant (10–30 mg/L), reaction time (5–90 min), catalyst dosage (0.2–2.5 g/L), on the catalytic ozonation process, were studied. In addition, the effects of the interfering factors on the work of ozone degradation agent and hydroxyl radicals are tested. The results of characterisation study showed a successful formation of GAC@ZnO composite with favorable catalytic properties. In addition, the GAC surface properties were enhanced by the modification with ZnO nanoparticles, where more efficient reaction sites for metronidazole degradation were created onto GAC. The degradation performance of the GAC@ZnO composite was high in which 83% of metronidazole removal was achieved in optimum conditions (pH = 11, catalyst dosage = 2 g/L, and reaction time = 30 min). In addition, the degradation rate was noticeably found to be higher in case of using catalytic ozonation process than using ozonation process alone. The kinetic degradation reactions of metronidazole followed the pseudo-first-order equation. According to the results of this model’s parameters, the degradation process is occurred on or near GAC@ZnO composite surface depending on the concentration of the pollutant. From the results obtained, it can be concluded that the GAC@ZnO composite in the catalytic ozonation treatment process was efficacious catalyst as it has excellent performance toward eradication of metronidazole wastewater.     

Development of parthenium based activated carbon and its utilization for adsorptive removal of p-cresol from aqueous solution

The activated carbon was prepared from carbonaceous agriculture waste Parthenium hysterophorous by chemical activation using concentrated H2SO4 at 130+/-5 degrees C. The prepared activated carbon was characterized and was found as an effective adsorbent material. In order to test the efficacy of parthenium based activated carbon (PAC), batch experiments were performed to carryout the adsorption studies on PAC for the removal of highly toxic pollutant p-cresol from aqueous solution. The p-cresol adsorption studies were also carried out on commercial grade activated carbon (AC) to facilitate comparison between the adsorption capabilities of PAC and AC. For PAC and AC, the predictive capabilities of two types of kinetic models and six types of adsorption equilibrium isotherm models were examined. The effect of pH of solution, adsorbent dose and initial p-cresol concentration on adsorption behaviour was investigated, as well. The adsorption on PAC and on AC was found to follow pseudo-first order kinetics with rate constant 0.0016 min(-1) and 0.0050 min(-1), respectively. The highest adsorptive capacity of PAC and AC for p-cresol solution was attained at pH 6.0. Further, as an adsorbent PAC was found to be as good as AC for removal of p-cresol upto a concentration of 500 mg/l in aqueous solution. Freundlich, Redlich-Peterson, and Fritz-Schlunder models were found to be appropriate isotherm models for PAC while Toth, Radke-Prausnitz and Fritz-Schlunder were suitable models for AC to remove p-cresol from aqueous solution.     

Color removal of distillery wastewater by ozonation in the absence and presence of immobilized iron oxide catalyst

Ozone is a strong oxidant, which can oxidize both biodegradable and non-biodegradable organics. The main objective of this study was to use iron oxide as a heterogeneous catalyst to enhance the ozone oxidation process. The wastewater used in this study was distillery wastewater, which was diluted 20 times before use. The diluted distillery wastewater was fed continuously in a downflow direction in an ozonation column. The iron oxide catalyst was coated on 10.3mm diameter alumina balls (5.5 m2/g specific surface area) by using Fe(NO3)3 as a precursor. The prepared catalyst was in the form of ferric oxide, and its loading was 0.07%. From the experimental results of both with and without the iron oxide catalyst, an increase in hydraulic retention time resulted in an increase in the treatment efficiencies of both chemical oxygen demand (COD) and color reduction, since the residence time of ozone increased. When the ozone mass flow rate increased, both COD and color reduction increased, resulting from an increase in the hydroxyl radical available in the system. The ozonation system with the iron oxide catalyst gave the highest efficiency in both COD and color removals because the hydroxyl free radical generated from the catalyst is more reactive than the ozone molecule itself.     

Characterization of chemically modified corncobs and its application in the removal of metal ions from aqueous solution

The objective of this work was to convert corncobs to activated carbon by low temperature chemical treatment for removing copper from wastewater. The parameters for developing a new adsorbent i.e. sorption capacity, selectivity, regenerability, suspension test, and kinetics were investigated. All studies were performed in batch experiments. Removal of copper from aqueous solutions varied with the amount of adsorbent, metal ion concentration, agitation time, solution pH and the species of copper present. It was found that the effect of temperature was very small. The Langmuir model was found to best fit the equilibrium isotherm data. Kinetics of copper removal at two different temperatures obeyed Lagergren pseudo-first-order equation. Effect of water hardness, other cations (Pb(2+) and Zn(2+)) on copper removal was also studied. Experiments with anionic and cationic complexes of copper showed that anionic copper species are not removed at all by the prepared material. To observe the nature of surface and pore structure scanning electron microscope (SEM) images of modified corncobs were used. To study the interaction forces between the adsorbent and the metal ion functional group analysis with infrared spectroscopy and proximate analysis were carried out. In addition, recovery of the metals ion and regeneration of spent adsorbent was possible by acidified hydrogen peroxide. Since the uptake capacity of the prepared adsorbent is 26mg Cu/g for copper, it can be a potential adsorbent for removing and recovering other heavy metal ions from contaminated wastewaters. The sorption capacity of the treated corncobs for copper was better than the reported capacity of other activated carbons prepared from agricultural sources.     

The effect of temperature on toluene sorption by granular activated carbon and its use in permeable reactive barriers in cold regions

Granular activated carbon (GAC) has been used as an adsorbent for hydrocarbons in a range of permeable reactive barriers. This work investigates the influence of temperature on adsorption performance. In particular, the influence of temperature in the range of 20 °C to 4 °C on the sorption equilibrium and kinetics of toluene on GAC surface were investigated. The results show that low temperature leads to decreased toluene sorption by GAC and slower reaction kinetics. Sorption kinetics studies show that diffusion coefficients are also lower at 4 °C (3.65 × 10⁻¹³ m² s⁻¹) than 20 °C (5.112 × 10⁻¹³ m² s⁻¹).     

Synthesis of interstratified graphene/montmorillonite composite material through organics-pillared,delamination and co-stacking and its application in hexavalent chromium removal from aqueous solution

Layers from two different delaminated dispersions of 3-aminopropyltriethoxysilane (APTES)-intercalated montmorillonite (Mts) and octylamine (OA)-intercalated graphene oxide (GO) could be co-stacked to obtain APTES-intercalated Mts (Mts-APTES)/OA-intercalated GO (GO-OA) interstratified composites (MAGO). The synthesized composites were characterized by XRD, FTIR, BET, TGA, TEM and XPS, which showed that MAGO had been prepared successfully. The optimal concentration of APTES was 8% in anhydrous toluene which avoided self-polymerization of APTES while facilitating the nucleophilic attack of APTES amine groups and the protic character of ethanol to compete with silane for the intimal hydroxyl groups by H-bonding. The MAGO demonstrated an extremely fast Cr(VI) removal from aqueous solution with a high removal efficiency at low pH. Data from batch studies of the adsorption process followed pseudo-second-order kinetics. The results fit a Langmuir model of adsorption, with maximum adsorption capacities of MAGO composites at pH 3.0 being 44.25 mg g^?1, 47.46 mg g^?1, 49.58 mg g^?1 under 30 °C, 40 °C, 50 °C, respectively, which were much higher than capacities of some conventional adsorbents. The reusability of the MAGO composite was also determined through adsorption-desorption studies, providing evidence for the potential use of MAGO composite in the removal of Cr(VI) from acidic wastewater.     

蒲绒活性炭负载Fe2O3的制备及其在软质聚氯乙烯中的阻燃应用

以蒲绒为原料、H₃PO₄为活化剂制备了蒲绒活性炭（AC）,利用浸渍焙烧法,制备了AC负载Fe₂O₃（AC-Fe₂O₃）复合物,将AC及AC-Fe₂O₃应用于软质聚氯乙烯（PVC）的阻燃处理,制备了AC阻燃软质PVC（AC/PVC）复合材料和AC负载Fe₂O₃阻燃软质PVC（AC-Fe₂O₃/PVC）复合材料。采用热重分析法研究了AC/PVC和AC-Fe₂O₃/PVC阻燃复合材料的热分解行为,采用极限氧指数（LOI）、垂直燃烧（UL-94）、锥形量热（CONE）等方法测试了AC/PVC和AC-Fe₂O₃/PVC阻燃复合材料的阻燃性能。结果表明：添加阻燃剂所制备的PVC基复合材料均达到UL-94 V-0级,LOI值均有提高。相比纯PVC,AC/PVC和AC-Fe₂O₃/PVC复合材料的热释放速率峰值和烟释放总量均有明显降低。这主要是由于AC和Fe₂O₃在凝聚相发挥协同阻燃作用。一方面AC的加入起到了物理阻隔的作用;另一方面Fe₂O₃的加入促进了PVC的早期交联碳化反应,催化PVC在燃烧前期形成更加稳定的炭层,使残炭率提高,可以有效抑制PVC的燃烧。     

Synthesis of one-dimensional ZnO nanoneedles using thermal oxidation process in the air and its application as filed emitters

In the present work, a novel route for synthesizing one-dimensional ZnO nanoneedles were introduced; that is, a pure Zinc nanocrystalline layer was firstly plated by using a periodic reverse pulse plating process, and then the ZnO nanoneedles grew upon the layer through thermal oxidation process in the air. The results showed that the oxidation temperature played a key role for growth, morphology and density of ZnO nanoneedles, which leads to the difference of their filed emission properties due to the various field enhancement factors β. A novel self-catalyzed diffusion model was proposed for interpreting the nanoneedles growth mechanism.     

Effects of adsorbent dose, its particle size and initial arsenic concentration on the removal of arsenic, iron and manganese from simulated ground water by Fe3+ impregnated activated carbon

This paper presents the observations of the study on arsenic removal from a contaminated ground water (simulated) by adsorption onto Fe³⁺ impregnated granular activated carbon (GAC-Fe). Fe²⁺, Fe³⁺ and Mn²⁺ have also been considered along with arsenic species in the water sample. Similar study has also been done with untreated granular activated carbon (GAC) for comparison. The effects of adsorbent dose, particle size of adsorbent and initial arsenic concentration on the removal of As(T), As(III), As(V), Fe²⁺, Fe³⁺ and Mn²⁺ have been discussed. Under the experimental conditions, the optimum adsorbent doses for GAC-Fe and GAC have been found to be 8 g/l and 24 g/l, respectively with an agitation time of 15 h. Particle size of the adsorbents (both GAC and GAC-Fe) has shown negligible effect on the removal of arsenic and Fe species. However, for Mn removal the effect of adsorbent particle size is comparatively more. Percentage removal of As(T), As(V) and As(III) increase with the decrease in initial arsenic concentration (As₀). However, the increase in percentage removal of all the arsenic species with decrease in As₀ are less for higher value of As₀ (3000–500 ppb) than those of the lower value of As₀ (500–10 ppb). The % removal of As(T), As(III), As(V), Fe, and Mn were 95%, 92.4%, 97.6%, 99% and 41.2%, respectively when 8 g/l GAC-Fe was used at the As₀ value of 200 ppb. However, for GAC these values were 55.5%, 44%, 71%, 98% and 97%. The pH and temperature of the study were 7 ± 0.1 and 30 ± 1 °C, respectively.     

离子液体[bmim]PF6中制备纳米金属Ni及其催化苯乙烯加氢的研究

以化学还原手段分别在水溶液和离子液体1-丁基-3-甲基咪唑六氟磷酸盐([bmim]PF6)中制备了纳米金属Ni粉末,采用X射线衍射(XRD)、透射电镜(TEM)、傅立叶红外光谱(FT-IR)、紫外可见光谱(UV-vis)及热重(TG-DTA)对所制备样品的形貌和结构进行了表征.XRD表征结果显示:与水溶液制备纳米Ni相比,在[bmim]PF6中制备的纳米Ni具有立方相结构,无氧化峰出现;TEM结果显示:在[bmim]PF6中制备的纳米Ni具有更小的粒径和更好的颗粒分布,团聚现象不明显;FT-IR显示:离子液体不仅仅作为反应的介质,而且和纳米颗粒表面间存在着一定的化学结合,吸附在纳米颗粒的表面,有效的阻止了Ni纳米颗粒的团聚和氧化;TG-DTA及UV-vis结果进一步验证了Ni表明离子液体层的存在.苯乙烯加氢产物的分析结果表明,在[bmim]PF6中制备的纳米Ni催化苯乙烯加氢的活性显著高于常规制备的Ni催化剂.     

Simultaneous preconcentration and removal of iron, chromium, nickel with N,N'-etylenebis-(ethane sulfonamide) ligand on activated carbon in aqueous solution and determination by ICP-OES

In this study, Fe, Cr and Ni have been preconcentrated and removed by using N,N'-ethylenebis (ethane sulfonamide), (ESEN) ligand on activated carbon (AC) in aqueous solution. For this purpose, complexes between these metals and ligands have been investigated and used in preconcentration and removal studies. Factors which have affected adsorption of metals on activated carbon have been optimized. Adsorbed metals have been preconcentrated 10-fold and determined by ICP-OES. Interferences of Ca, Mg and K to this process have been investigated. The proposed method has been applied to the tap water and Ankara Creek water in order to Fe, Cr, and Ni remediation and preconcentration. Determination of metals by ICP-OES has been checked with standard reference material (NIST 1643e). The proposed method provides the recoveries of 87%, 108% and 106% for Fe, Cr and Ni, respectively, in preconcentration. It also provides the removal of Fe, Cr and Ni by 93%, 100% and 100% removal from waters, respectively.