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High catalytic activity of Pt–Pd containing USY zeolite catalyst for low temperature CO oxidation from industrial off gases
2015
Lokhande, Suchita | Doggali, Pradeep | Rayalu, Sadhana | Devotta, Sukumar | Labhsetwar, Nitin
Small amounts (0.15wt%) of platinum and palladium were incorporated in porous, high surface area, ultra–stable H–USY–Zeolite by ion exchange method, and their catalytic activity was studied for carbon monoxide (CO) oxidation reaction, under various conditions of industrial importance. The catalyst was characterized by p–XRD, chemical analysis, SEM, TEM, evaluated for catalytic activity using a steady state, fixed bed catalytic reactor. The catalysts show high CO oxidation activity and it was possible to convert 0.044 mmols of CO per gram of catalyst at 120 °C, at a space velocity of 60 000 h−1 and with 100 ppm CO concentration in feed gas. The high catalytic activity of this noble metal catalyst also appears to be a factor of porous structure of zeolite facilitating mass transfer; high surface area as well as highly dispersed catalyst sites of palladium and platinum on zeolite structure. Introduction of acidic sites in zeolites probably makes them more resistant towards SO2, while their surface area and pore characteristics make this catalyst efficient even under high space velocity conditions, thus suggesting the potential of larger pore size zeolites over conventional porous materials for industrial applications.
Show more [+] Less [-]Characterization and activity of N doped TiO2 supported VPO catalysts for NO oxidation
2015
Jia, Yong | Du, Daqian | Bai, Jiachuan | Ding, Jie | Zhong, Qin | Ding, Xilou
Nitrogen (N) doped TiO2 supported vanadium phosphorus oxide (VPO) catalysts were prepared and tested for catalytic oxidation of NO. The experimental results showed that 0.1V(5)PO/TiN(1) was the optimal catalyst for NO oxidation and the NO conversion could reach 61% at temperature of 350°C. The physico–chemical properties of 0.1V(5)PO/TiN(1) catalyst were characterized by Brunauer–Emmett–Teller measurements (BET), Photoluminescence (PL), X–ray photoelectron spectroscopy (XPS), Infrared spectroscopy measurements of NH3 adsorbed on catalysts (NH3–IR), and Infrared Fourier transform spectroscopy (FTIR). The PL and XPS spectra revealed that the oxygen storage capacity and catalytic activity of VPO/Ti catalyst can be improved by nitrogen doping. The H2–TPR profile also indicated that V(5)PO/TiN(1) catalyst had a superior redox property. Activity test results and FTIR spectra showed that 0.1V(5)PO/TiN(1) catalysts had a superior resistivity to SO2 and the NO oxidation rate is above 50% at temperature of 350°C when SO2 concentration is 200ppm to 800ppm.
Show more [+] Less [-]Microwave assisted catalytic removal of elemental mercury from flue gas using Mn/zeolite catalyst
2015
Wei, Zaishan | Luo, Yuwei | Li, Baoren | Cheng, Zhouyang | Wang, Jianbin | Ye, Qihong
The integrated microwave with Mn/zeolite and ozone (MCO) and combined microwave with Mn/zeolite (MC) was employed to oxidize elemental mercury (Hg0) in simulated flue gas. The results show that mercury removal efficiency attained 35.3% in the MC, over 92% of Hg0 removal efficiency could be obtained in the MCO. The optimal microwave power and empty bed residence time (EBRT) in the microwave plasma catalytic oxidation were 264 W and 0.41 s, respectively. The effect of Hg0 oxidation in the MCO was much higher than that in the MC. Microwave accentuated catalytic oxidation of mercury, and increased mercury removal efficiency. The additional use of ozone to the microwave–catalysis over Mn/zeolite led to the enhancement of mercury oxidation. Mn/zeolite catalyst was characterized by X–ray diffraction (XRD), X–ray photoelectron spectroscopy (XPS), Fourier transform infrared spectra (FT–IR), scanning electron microscopy (SEM) and the Brunauer Emmett Teller (BET) method. Microwave catalytic mercury over Mn/zeolite was dominated by a free radical oxidation route. Ozone molecules in air could enhance free radical formation. The coupling role between ozone and radicals on mercury oxidation in the MCO was formed. The MCO appears to be a promising method for emission control of elemental mercury.
Show more [+] Less [-]Optimizing Phenanthrene and Anthracene Oxidation by Sodium Persulfate and Fe-Modified Diatomite Using the Response Surface Method
2015
da Silva, Celyna K. O. | Vianna, Marilda M. G. R. | Foletto, Edson L. | Chiavone-Filho, Osvaldo | do Nascimento, Claudio A. O.
This study proposes an improved activation for hydrogen peroxide and persulfate using Fe-modified diatomite (MD) to favorably lead the reaction to generate hydroxyl and sulfate radicals to degrade the contaminants phenanthrene and anthracene. Diatomite was modified by impregnating it with a mixture of ferrous (Fe²⁺) and ferric (Fe³⁺) ions in the form of precipitated iron oxides and hydroxides. The raw and synthesized materials were characterized by powder X-ray diffraction (XRD), X-ray fluorescence (XRF), particle size by laser diffraction, chemical microanalysis of the elements by energy-dispersive X-ray, and scanning electron microscopy (SEM). Batch experiments were performed to compare the new activator material (modified diatomite) with traditional methods of activation for these oxidants and to statistically study the optimum ratio between the amount of this material and the concentration of one oxidant to the degradation of the contaminants phenanthrene and anthracene. The characterization results showed that the materials are amorphous and that the Fe ion concentration was 4.78 and 17.65 % for the raw and modified diatomites, respectively. This result shows a significant increase in the amount of iron ions after synthesis. Comparing the traditional activation method with the modified diatomite, the results of batch experiments showed that the synthesized material presents significant catalytic activity for the oxidation of these contaminants, using sodium persulfate and hydrogen peroxide as oxidants. The analysis of the variables results showed that the concentration of the oxidant has higher significance than the amount of the catalyst.
Show more [+] Less [-]Remediation of Pentachlorophenol-Contaminated Soil by Non-specific Abiotic Reactions Using Heme and Hemoglobin
2015
Kang, Guyoung | Stevens, David K. | Chung, Namhyun
To treat PCP-contaminated soil, abiotic methods for PCP degradation have been developed, where heme or powder hemoglobin acts as a catalyst and hydrogen peroxide as an oxidant. Degradation of PCP had the first-order kinetics, and rate coefficients, k, were 0.073 and 0.104/day for heme and hemoglobin, respectively, indicating that the hemoglobin was a more efficient catalyst than heme. Approximately 96 % of the initial PCP was degraded at day 35. Thus, hemoglobin might be recommended as the catalyst of choice, since it is much less expensive than heme.
Show more [+] Less [-]Superporous Cryogel-M (Cu, Ni, and Co) Composites in Catalytic Reduction of Toxic Phenolic Compounds and Dyes from Wastewaters
2015
Sahiner, Nurettin | Seven, Fahriye | Al-lohedan, Hamad
P(Acrylamide) (p(AAm)) cryogel with superporous structure was synthesized by employing a cryopolymerization technique under freezing conditions. The prepared cryogels were modified by amidoximation to generate new functional groups as amid-p(AAm) cryogel, that binds metal ions, and the metal nanoparticles of those ions were prepared via in situ reduction method. The prepared amid-p(AAm)-M cryogel composites (M: Cu, Ni, and Co) were used as superporous reactor for the catalytic reduction of toxic phenol compounds 2- and 4-nitrophenol (2- and 4-NP) and some dyes methylene blue (MB) and Eosin Y (EY). P(AAm) cryogels and their metal composites were characterized by using FT-IR analysis, SEM images, and AAS measurements. The impact of porosity, the types and amount of metal catalyst, temperature of reaction medium, and so on were investigated for toxic 2-NP reduction by amid-p(AAm)-M cryogel composites. Very high total turnover frequencies (TOF) and low activation energy (Ea) values of 2.46 (mole 2-NP) (mole Cu. min)⁻¹and 20.2 kJmol⁻¹were obtained for catalytic reduction of 2-NP compound catalyzed by amid-p(AAm)-Cu cryogel composites. Consequently, superporous p(AAm) cryogel is the perfect support material for metal nanoparticle preparation and use in catalytic reduction reactions.
Show more [+] Less [-]The Use of Metal Nanoparticle-Embedded Poly(ethyleneimine) Composite Microgel in the Reduction of Nitrophenols
2015
Demirci, Sahin | Sahiner, Nurettin
Metal nanoparticles such as Ni, Cu, and Co were prepared within polyethyleneimine (PEI) microgels and were used in the reduction of 4-nitrophenol (4-NP) and 2-nitrophenol (2-NP) to 4-aminophenol (4-AP) and 2-aminophenol (2-AP). The metal nanoparticle content of the prepared PEI-M composite catalyst system (M = Co, Ni, and Cu) was increased by multiple loading and reduction cycles into PEI microgels to provide faster and better reduction of 4-NP and 2-NP. The TOF value increased to 1.48 from 0.353 (mol 4-NP (mol catalyst min)⁻¹) for 4-NP reduction catalyzed by PEI-Ni after three cycles of metal loading and reduction. The effect of temperature on 4-NP and 2-NP reductions catalyzed by PEI-M illustrated that higher temperature resulted in very fast reductions, e.g., at 70 °C 4-NP and 2-NP reduction by PEI-Ni resulted in very fast reduction times of 1.2 and 0.67 min to 4-AP and 2-AP, respectively. The activation parameters, such as energy, entropy, and enthalpy, were also calculated and mild activation energies of 38.8 and 46.0 kJ mol⁻¹for 4-NP and 2-NP catalyzed by PEI-Ni were found, respectively, in comparison to similar studies in the literature. Moreover, it was demonstrated that PEI-Ni microgels are reusable five times consecutively, with almost 100 % conversion and 100 % of their catalytic activity.
Show more [+] Less [-]Kinetic modeling of the photocatalytic degradation of clofibric acid in a slurry reactor
2015
A kinetic study of the photocatalytic degradation of the pharmaceutical clofibric acid is presented. Experiments were carried out under UV radiation employing titanium dioxide in water suspension. The main reaction intermediates were identified and quantified. Intrinsic expressions to represent the kinetics of clofibric acid and the main intermediates were derived. The modeling of the radiation field in the reactor was carried out by Monte Carlo simulation. Experimental runs were performed by varying the catalyst concentration and the incident radiation. Kinetic parameters were estimated from the experiments by applying a non-linear regression procedure. Good agreement was obtained between model predictions and experimental data, with an error of 5.9 % in the estimations of the primary pollutant concentration.
Show more [+] Less [-]Continuous Treatment of Phenol over an Fe2O 3/γ-Al 2O 3 Catalyst in a Fixed-Bed Reactor
2015
Lu, Minghui | Yao, Yue | Gao, Lulu | Mo, Dongmei | Lin, Fang | Lü, Shuxiang
Fe₂O₃/γ-Al₂O₃catalysts were prepared using the wet impregnation method and characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and nitrogen adsorption–desorption. The continuous catalytic wet hydrogen peroxide oxidation of an aqueous phenol solution over Fe₂O₃/γ-Al₂O₃was studied in a fixed-bed reactor. The effects of several factors, such as the weight hourly space velocity (WHSV), particle size, reaction temperature, H₂O₂concentration, and initial pH, were studied to optimize the operation conditions for phenol mineralization. For a 1 g L⁻¹phenolic aqueous solution, the phenol was nearly completely removed and chemical oxygen demand (COD) removal was approximately 92 % at steady-state conditions with a WHSV of 2.4 × 10⁻² gPₕOH h⁻¹ gcₐₜ⁻¹at 80 °C with 5.1 g L⁻¹H₂O₂. The long-term stability of the Fe₂O₃/γ-Al₂O₃catalyst was also investigated for the continuous treatment of phenolic water. The removal of phenol and COD exhibited a slowly decreasing trend, which was primarily due to the complexation of active sites with acid organic compounds and the adsorption of intermediate products. The deposition of organic carbon and Fe leached from the catalyst had a small role in the partial deactivation of the catalyst. The Fe leached from the catalyst partially contributed to the phenol removal during a short run. However, this contribution could be neglected after 36 h because the Fe leached from the catalyst decreased to approximately 5 mg L⁻¹.
Show more [+] Less [-]Intensify Removal of Nitrobenzene from Aqueous Solution Using Nano-Zero Valent Iron/Granular Activated Carbon Composite as Fenton-Like Catalyst
2015
Hu, Sihai | Yao, Hairui | Wang, Kaifeng | Lu, Cong | Wu, Yaoguo
To obtain a good catalytic effect of removing refractory organics from water by Fenton process, granular activated carbon (GAC) supported nano-zero valent iron (nZVI) composite (nZVI/GAC) was prepared by adsorption–reduction method, and characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and energy-dispersive X-ray spectroscopy (EDS). The catalytic degradation activity of the composite was evaluated to remove nitrobenzene (NB) pollutant via a heterogeneous Fenton-like system, and the initial pH value, nZVI/GAC dosage, and H₂O₂concentration influencing on NB removal were also investigated at room temperature. Experimental results showed that nZVI particle was uniformly dispersed over GAC matrix, and average particle size was 40–100 nm without agglomeration. The nZVI/GAC composite was very efficient in removing NB with average percentage of more than 85 %. However, the removal rate of Fenton-like reaction was highly affected by pH value, H₂O₂concentration, and nZVI/GAC dosage. The optimal reaction conditions were pH 4.0, 40 mg/L NB, 5.0 mmol/L H₂O₂, and 0.4 g/L nZVI/GAC in this study. Stability and repeatability tests as well as mechanism analysis illustrated that GAC improved catalytic action via enhancing nZVI dispersion and accelerating Fe(III)/Fe(II) cycle attributing to internal iron–carbon microelectrolysis in nZVI/GAC composite. Iron utilization efficiency, which played an important role in NB degradation by Fenton-like greatly increased resulting in dissolved iron <0.6 mg/L. This phenomenon strongly implied that the nZVI/GAC Fenton-like process was not only a practical combination of adsorption and Fenton oxidation but also some synergetic effects existing in such an nZVI/GAC composite.
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