Lin Gu

Adsorption and Fenton-like degradation of naphthalene dye intermediate on sewage sludge derived porous carbon

A sewage sludge derived porous carbon (SC), which was prepared by physicochemical activation and carbonization (600°C), was applied for the adsorption and degradation of 1-diazo-2-naphthol-4-sulfonic acid (1,2,4-Acid) in the presence of H(2)O(2) and the performance was compared to that of pure Fe(3)O(4) magnetic nanoparticles (MNPs). The prepared SC showed mesoporous structure with magnetic property, which made it favorable for solid-liquid separation application. Further experiments revealed that SC had a higher adsorption capacity and degradation efficiency of 1,2,4-Acid than bare Fe(3)O(4). The Langmuir and Freundlich model fitted the isotherm data and illustrated that the equilibrium adsorption amount of 1,2,4-Acid onto SC (95.1 mg g(-1)) was quadruple as large as that on Fe(3)O(4) (26.4 mg g(-1)). The subsequent degradation experiments were conducted at conditions (pH 5.0 in the presence of 15 mM H(2)O(2)) with regard to 1,2,4-Acid degradation efficiency and metal ions leach. The 120 mins treatment in SC/H(2)O(2) system achieved 94% of 1,2,4-Acid (from 150 mg L(-1) after adsorption equilibrium to 9 mg L(-1)) and 48.1% TOC reduction, far higher than the efficiency of 46% and 24.3% by using Fe(3)O(4) MNPs. Further analysis evidenced the co-catalytic effect of iron, carbon, silicon and aluminum, which existed in large quantities in sludge derived SC. The carbonaceous phase along with silica contributes to an increase in the dispersion of catalytic centers and an adsorbent to concentrate organic pollutant whereas the iron oxide as well as alumina provides the catalytic centers for a Haber-Weiss initiated reactions.

Near-infrared photocatalyst of Er3+/Yb3+ codoped (CaF2@TiO2) nanoparticles with active-core/active-shell structure

A novel near-infrared (NIR) photocatalyst of Er3+/Yb3+-(CaF2@TiO2) was synthesized with optically active centers (Er3+/Yb3+) presented both in the CaF2 cores and TiO2 shells, and the corresponding upconversion luminescence properties increased greatly, which was helpful for the organic dye solution removal efficiency under NIR irradiation.

Leaching behavior of heavy metals from sewage sludge solidified by cement-based binders.

Sewage sludge was stabilized and solidified (S/S) with cement-based binders prior to landfill in order to reduce the potential hazard of heavy metals. The leaching behavior and chemical speciation of heavy metals in the solidified sludge were studied by semi-dynamic leaching test, toxicity characteristic leaching procedure (TCLP) and sequential extraction procedures. The effectiveness of S/S treatment was evaluated by determining diffusion coefficients (De) calculated from the data achieved in semi-dynamic leaching test. High De values under low pH (4.0 compared to 7.0 and 10.0) and high temperature (35°C compared to 10°C and 25°C) conditions were always recorded. Acid-assisted S/S product showed lower De values and leaching tendency from TCLP test results for all the selected heavy metals (Ni, Cu, Zn and Pb) compared to traditional S/S product using the same binders. More heavy metals were converted into stable fractions by acid-assisted S/S than usual S/S according to sequential extraction test.

Degradation pathway of the naphthalene azo dye intermediate 1-diazo-2- naphthol-4-sulfonic acid using Fenton's reagent.

Degradation of naphthalene dye intermediate 1-diazo-2- naphthol-4-sulfonic acid (1,2,4-Acid) by Fenton process has been studied in depth for the purpose of learning more about the reactions involved in the oxidation of 1,2,4-Acid. During 1,2,4-Acid oxidation, the solution color initially takes on a dark red, then to dark black associated with the formation of quinodial-type structures, and then goes to dark brown and gradually disappears, indicating a fast degradation of azo group. The observed color changes of the solution are a result of main reaction intermediates, which can be an indicator of the level of oxidization reached. Nevertheless, complete TOC removal is not accomplished, in accordance with the presence of resistant carboxylic acids at the end of the reaction. The intermediates generated along the reaction time have been identified and quantified. UPLC-(ESI)-TOF-HRMS analysis allows the detection of 19 aromatic compounds of different size and complexity. Some of them share the same accurate mass but appear at different retention time, evidencing their different molecular structures. Heteroatom oxidation products like SO(4)(2-) have also been quantified and explanations of their release are proposed. Short-chain carboxylic acids are detected at long reaction time, as a previous step to complete the process of dye mineralization. Finally, considering all the findings of the present study and previous related works, the evolution from the original 1,2,4-Acid to the final products is proposed in a general reaction scheme.

Heavy metal recovery from electroplating wastewater by synthesis of mixed-Fe3O4@SiO2/metal oxide magnetite photocatalysts

Heavy metal recovery is a promising way to reduce the pollution from electroplating wastewater (EPW), and magnetite photocatalysts of mixed-ferrite (M-Fe3O4)@SiO2/metal oxides have been prepared to reuse heavy metals from simulated-EPW (S-EPW) and real-EPW (R-EPW). In this work, four pure magnetite photocatalysts M-Fe3O4@SiO2/ZnO, M-Fe3O4@SiO2/CuO, M-Fe3O4@SiO2/Fe2O3, and M-Fe3O4@SiO2/NiO were synthesized via a simple precipitation reaction, where the M-Fe3O4@SiO2 core–shell nanoparticles served as the magnetic cores and supports for the metal oxides. The structures, morphologies, and magnetic properties of these magnetite photocatalysts were characterized, and then the photocatalytic performances of the pure and complex magnetite photocatalysts (M-Fe3O4@SiO2 supported single and mixed-metal oxides) were tested and compared using methyl orange (MO) degradation experiments. It was found that M-Fe3O4@SiO2/ZnO had the best photocatalytic performance of the pure magnetite photocatalysts, with a MO removal rate of 91.5%, followed by 37.4% for M-Fe3O4@SiO2/NiO, 19.0% for M-Fe3O4@SiO2/Fe2O3, and 17.6% for M-Fe3O4@SiO2/CuO. The removal rates were 17.4% and 13.2% for the complex magnetite photocatalysts prepared from S-EPW and R-EPW, respectively. More than 98% of the heavy metals can be recovered from EPW through the simultaneous synthesis of the magnetite photocatalysts.

Combined humic acid adsorption and enhanced Fenton processes for the treatment of naphthalene dye intermediate wastewater.

In this work, an humic acid adsorption with an enhanced Fenton oxidation was employed to treat the real effluent originating from the 1-diazo-2-naphthol-4-sulfonic acid (1,2,4-Acid) production plant. In a first step, humic acid with MgSO(4) was selected as adsorbent and precipitant for physicochemical pretreatment, the synergetic effect had led to 39% of COD removal and 89% of colour removal. A multi-staged Fenton oxidation process with inner circulation was introduced subsequently. The TOC, COD, 1,2,4-Acid, NH(4)(+)-N, SS and colour were reduced from 3024 mg/L, 12,780 mg/L, 9103 mg/L, 110 mg/L, 240 mg/L and 25,600 (multiple) to 46 mg/L, 210 mg/L, 21 mg/L, 16 mg/L, 3 mg/L and 25 through the combined process, respectively. Hydrogen peroxide consumed per kg COD had saved up to 36% when two-staged Fenton process with inner circulation (flow-back to influent ratio: 3) was applied. Influence of H(2)O(2) concentration, flow-back to influent ratio and staged Fenton mode were investigated in detail in order to find out the optimal operating parameters. The kinetics of 1,2,4-Acid degradation by two-staged Fenton process was investigated. The evolution of the main intermediates during the degradation process was conducted using the LC-(ESI)-TOF-MS technique, and the results showed a staged degradation pathway from the ring opening of naphthalene compounds to the formation of benzene compounds and carboxyl acids. The combined process had been proved effective in both technical and economic aspects.

Preparation of sewage sludge based activated carbon by using Fenton's reagent and their use in 2-naphthol adsorption.

In this study, Fentons reagents (H2O2/Fe(2+)) are used to activate raw sewage sludge for the preparation of the sludge based activated carbon. The effect of the amount of hydrogen peroxide addition on carbons chemical composition, texture properties, surface chemistry and morphology are investigated. Choosing an appropriate H2O2 dosage (5 v%) (equivalent to 70.7 mM/(g VS)), it is possible to obtain a comparatively highly porous materials with SBET and the total pore volume being 321 m(2)/g and 0.414 cm(3)/g, respectively. Continuously increasing the oxidant ratio resulted in a decreased SBET value. Further adsorption experiments by using 2-naphthol as model pollutant revealed that the adoption followed a pseudo-second-order kinetics better than pseudo-first-order. The calculated adsorption capacity is 111.9 mg/g on the carbon with 5% H2O2 pretreatment while this value is just 51.5mg/g on carbons without any pretreatment.

A comparative study of aerobically digested and undigested sludge in preparation of magnetic chars and their application in 1-diazo-2-naphthol-4-sulfonic acid adsorption.

In this work, two types of sewage-sludges, aerobically digested and undigested sewage sludge, were used as precursors in the preparation of chars with magnetic property. The two solids were characterized to establish their textural and chemical properties. Due to different elemental composition, chars from the digested sludge were found to contain zeolite-like minerals such as NaP1 zeolite, which enables its abilities of anion exchange, while chars from undigested sewage sludge exhibited a well-degreed graphite structure. 1-Diazo-2-naphthol-4-sulfonic acid (1,2,4-Acid) was used as a model pollutant to investigate its adsorption on prepared chars. The adsorption kinetics of 1,2,4-Acid onto both chars followed pseudo-second-order kinetics. The simulated Langmuir-Freundlich model illustrated that the equilibrium adsorption amount of 1,2,4-Acid was 102.8 and 105.3mg/g, respectively, at 303 K. The adsorption amount declined on digested chars, whereas kept stable on the other in the presence of sodium chloride, suggesting the diversity in adsorption behavior.

Facile synthesis of magnetic sludge-based carbons by using Electro-Fenton activation and its performance in dye degradation

Highly stable iron based magnetic carbon were prepared by sequential Electro-Fenton (EF) activation and pyrolysis of sewage sludge. The applied voltage exerts great influence on EF treated sludge flocs and thus poses significant effect on physiochemical properties of the as-prepared carbons. High insertion rate of iron into sludge from EF activation resulted in carbons with highly dispersed iron oxides, which had average size of iron nanoparticles being 4.77nm. The carbon also presented well developed porosity which had Brunauer-Emmett-Teller (BET) surface area attaining 341m2/g. Carbons prepared by traditional Iron Impregnation (IM) were used as comparison to gain further insight into their catalytic role as Fenton-like catalyst. Results showed that EF-activated sludge carbon could yield 96.1% of Methyl Orange (MO) removal in 60min together with only 1.4% of iron leaching. After three cycles, the MO removal can still reach 80% with EF-activated carbons.

Nitrate removal from landfill leachate by zerovalent iron (ZVI)

AbstractBatch experiments were conducted on landfill leachate which was treated by membrane bioreactor process to test the nitrate removal by zerovalent iron (ZVI). The effects of iron-to-nitrate ratio, dissolved oxygen, and initial pH were investigated. The results showed that high iron-to-nitrate ratio, oxygen free condition, and low pH could improve the nitrate reduction. In order to investigate the theory of total nitrogen (TN) reduction, iron (coated with iron oxide) was analyzed by Fourier transform infrared spectroscopy after reactions and the results showed that some amount of ammonium was adsorbed onto iron oxides. In order to obtain higher nitrate removal efficiency, the effect of pH was studied through continuously stirred tank reactor. The results showed almost all the nitrate could be removed in 24 h when pH was controlled at 2.0. Actually, not only nitrate but organic pollutants, metals, and chloride were contaminants in landfill leachate. The removal efficiencies were thus discussed under o...