Search results for: bimetallic catalyst

Authors: Joy Marie Mora, Mark Daniel De Luna, Tsair-Wang Chung

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Transesterification reaction of soybean oil with methanol was carried out to produce fatty acid methyl esters (FAME) using calcined alkali metal (Na and Li) supported by pumice silica as the solid base catalyst. Pumice silica catalyst was activated by loading alkali metal ions to its surface via an ion-exchange method. Response surface methodology (RSM) in combination with Box-Behnken design (BBD) was used to optimize the operating parameters in biodiesel production, namely: reaction temperature, methanol to oil molar ratio, reaction time, and catalyst concentration. Using the optimized sets of parameters, FAME yields using sodium and lithium silicate catalysts were 98.80% and 98.77%, respectively. A pseudo-first order kinetic equation was applied to evaluate the kinetic parameters of the reaction. The prepared catalysts were characterized by several techniques such as X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), Brunauer-Emmett-Teller (BET) sorptometer, and scanning electron microscopy (SEM). In addition, the reusability of the catalysts was successfully tested in two subsequent cycles.

Keywords: alkali metal, biodiesel, Box-Behnken design, heterogeneous catalyst, kinetics, optimization, pumice, transesterification

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Authors: Nadeem Bashir, Ghulam Mustafa Peerzada

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The present study pertains to the nonlinear behavior of acetaminophen based uncatalyzed Belousov-Zhabotinsky (BZ) oscillator and its dynamics in the presence of Ferroin as the catalyst. The role of free metal ions as catalysts was examined and the results compared with corresponding complexed catalysts. Free metal ions were found to be sluggish with respect to the evolution of the oscillatory regime as compared to complexed ones. Effect of change of the ligand moiety of the catalyst complex on the oscillatory parameters was monitored. Since ethanol potentiates the hepatotoxicity caused by acetaminophen in-vivo, it is thought to understand this interaction by virtue of causing perturbation of the acetaminophen based oscillator with different concentrations of the ethanol with and without ferroin as the catalyst. Another dimension to the ethanol effect was added by perturbation of the system with ethanol at different stages of the reaction so as to get an idea whether it is acetaminophen or some reactive intermediate generated in the reaction system which reacts with ethanol. Further, the ferroin-catalyzed oscillator is taken as a prototype inorganic model of the acetaminophen-ethanol syndrome, as ferroin and HOBr were inorganic replacements to Cyt P450 and NADPH in the alcohol metabolism.

Keywords: Belousov-Zhabotinsky reaction, ferroin, Paracetamol-Ethanol syndrome, kinetics

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Authors: Swarnalata Sahoo, Smita Mohanty, S. K. Nayak

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Environmentally friendly Polyurethane(PU) synthesis from Castor oil(CO) has been studied extensively. Probably due to high proportion of fatty hydroxy acids and unsaturated bond, CO showed better performance than other oil, can be easily utilized as commercial applications. In this work, cured PU polymers having different –NCO/OH ratio with and without catalyst were synthesized by using partially biobased Isocyanate with castor oil (CO). Curing time has been studied by observing at the time of reaction, which can be confirmed by AT-FTIR. DSC has been studied to monitor the reaction between CO & Isocyanates using non Isothermal process. Curing kinetics have also been studied to investigate the catalytic effect of the NCO / OH ratio of Polyurethane. Adhesion properties were evaluated from Lapshear test. Tg of the PU polymer was evaluated by DSC which can be compared by DMA. Surface Properties were studied by contact angle measurement. Improvement of the interfacial adhesion between the nonpolar surface of Aluminum substrate and the polar adhesive has been studied by modifying surface.

Keywords: polyurethane, partially bio-based isocyanate, castor oil, catalyst

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Authors: S. Said, Asmaa A. Abdulrahman

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MoOₓ/Al₂O₃ based catalyst has long been widely used as an active catalyst in oxidative desulfurization reaction due to its high stability under severe reaction conditions and high resistance to sulfur poisoning. In this context, 4 & 9wt.% MoO₃ grafted on mesoporous γ-Al₂O₃ has been synthesized using the modified atomic layer deposition (ALD) method. Another MoO₃/Al₂O₃ sample was prepared by the conventional wetness impregnation (IM) method, for comparison. The effect of the preparation methods on the metal-support interaction was evaluated using different characterization techniques, including X-ray diffraction, X-ray photoelectron spectroscopy (XPS), N₂-physisorption, transmission electron microscopy (TEM), H₂- temperature-programmed reduction and FT-IR. Oxidative desulfurization (ODS) reaction of the model fuel oil was used as a probe reaction to examine the catalytic efficiency of the prepared catalysts. ALD method led to samples with much better physicochemical properties than those of the prepared one via the impregnation method. However, the 9 wt.%MoO₃/Al₂O₃ (ALD) catalyst in the ODS reaction of model fuel oil shows enhanced catalytic performance with ~90%, which has been attributed to the more Mo⁶⁺ surface concentrations relative to Al³⁺ with large pore diameter and surface area. The kinetic study shows that the ODS of DBT follows a pseudo first-order rate reaction.

Keywords: mesoporous Al₂O₃, xMoO₃/Al₂O₃, atomic layer deposition, wetness impregnation, ODS, DBT

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Authors: Pauline Bredy, Yves Schuurman, David Farrusseng

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To fulfill climate objectives, the production of synthetic e-fuels using CO₂ as a raw material appears as part of the solution. In particular, Power-to-Liquid (PtL) concept combines CO₂ with hydrogen supplied from water electrolysis, powered by renewable sources, which is currently gaining interest as it allows the production of sustainable fossil-free liquid fuels. The proposed process discussed here is an upgrading of the well-known Fischer-Tropsch synthesis. The concept deals with two cascade reactions in one pot, with first the conversion of CO₂ into CO via the reverse water gas shift (RWGS) reaction, which is then followed by the Fischer-Tropsch Synthesis (FTS). Instead of using a Fe-based catalyst, which can carry out both reactions, we have chosen the strategy to decouple the two functions (RWGS and FT) on two different catalysts within the same reactor. The FTS shall shift the equilibrium of the RWGS reaction (which alone would be limited to 15-20% of conversion at 250°C) by converting the CO into hydrocarbons. This strategy shall enable optimization of the catalyst pair and thus lower the temperature of the reaction thanks to the equilibrium shift to gain selectivity in the liquid fraction. The challenge lies in maximizing the activity of the RWGS catalyst but also in the ability of the FT catalyst to be highly selective. Methane production is the main concern as the energetic barrier of CH₄ formation is generally lower than that of the RWGS reaction, so the goal will be to minimize methane selectivity. Here we report the study of different combinations of copper-based RWGS catalysts with different cobalt-based FTS catalysts. We investigated their behaviors under mild process conditions by the use of high-throughput experimentation. Our results show that at 250°C and 20 bars, Cobalt catalysts mainly act as methanation catalysts. Indeed, CH₄ selectivity never drops under 80% despite the addition of various protomers (Nb, K, Pt, Cu) on the catalyst and its coupling with active RWGS catalysts. However, we show that the activity of the RWGS catalyst has an impact and can lead to longer hydrocarbons chains selectivities (C₂⁺) of about 10%. We studied the influence of the reduction temperature on the activity and selectivity of the tandem catalyst system. Similar selectivity and conversion were obtained at reduction temperatures between 250-400°C. This leads to the question of the active phase of the cobalt catalysts, which is currently investigated by magnetic measurements and DRIFTS. Thus, in coupling it with a more selective FT catalyst, better results are expected. This was achieved using a cobalt/iron FTS catalyst. The CH₄ selectivity dropped to 62% at 265°C, 20 bars, and a GHSV of 2500ml/h/gcat. We propose that the conditions used for the cobalt catalysts could have generated this methanation because these catalysts are known to have their best performance around 210°C in classical FTS, whereas the iron catalysts are more flexible but are also known to have an RWGS activity.

Keywords: cobalt-copper catalytic systems, CO₂-hydrogenation, Fischer-Tropsch synthesis, hydrocarbons, low-temperature process

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Authors: Allah Bakhsh Javid, Ali Mashayekh-Salehi, Fatemeh Davardoost

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This study presents the preparation, characterization and catalytic activity of a novel natural mineral-based catalyst for destructive adsorption of tetracycline (TTC) as water emerging compounds. Degradation potential of raw and calcined magnetite catalyst was evaluated at different experiments situations such as pH, catalyst dose, reaction time and pollutant concentration. Calcined magnetite attained greater catalytic potential than the raw ore in the degradation of tetracycline, around 69% versus 3% at reaction time of 30 min and TTC aqueous solution of 50 mg/L, respectively. Complete removal of TTC could be obtained using 2 g/L calcined nanoparticles at reaction time of 60 min. The removal of TTC increased with the increase in solution temperature. Accordingly, considering its abundance in nature together with its very high catalytic potential, calcined pyrite is a promising and reliable catalytic material for destructive decomposition for catalytic decomposition and mineralization of such pharmaceutical compounds as TTC in water and wastewater.

Keywords: catalytic degradation, tetracycline, pyrite, emerging pollutants

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Authors: Zohreh Derikvand

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Nanoreactors Zr-MCM-41were prepared via the reaction of ZrOCl2, Fumed silica, sodium hydroxide and cethyltrimethyl ammonium bromide under hydrothermal condition. The prepared nanoreactors were characterized by FT-IR spectroscopy, X-ray diffraction (XRD), Scanning electron micrographs (SEM) and nitrogen adsorption-desorption. The XRD pattern of Zr-MCM-41 exhibits a high-intensity (100) and two low-intensity reflections (110 and 200) which are characteristic of hexagonal structure, exhibiting the long-range order and good textural uniformity of mesoporous structure. Based on the green chemistry approach, we report an efficient and environmentally benign protocol to study the catalytic activity of Zr-MCM-41 in the Biginelli type reactions initially. Nanoreactors Zr-MCM-41 were used as highly recoverable and reusable catalyst for synthesis of 3,4-dihydropyrimidin-2(1H)-one, octahydroquinazolinone, benzimidazolo-quinazolineone and 4,6-diarylpyrimidin-2(1H)-one. The methodology offers several advantages such as short reaction time, high yields and simple operation. The catalyst was active up to three cycles.

Keywords: Zr-MCM-41 nanoreactors, Biginelli like reactions, 3, 4-dihydropyrimidin-2(1H)-ones, ctahydroquinazolinones

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Authors: Alexsandro Bayestorff da Cunha, Dpebora Caline de Mello, Camila Alves Corrêa

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In the production of fiberboards, an adhesive based on urea-formaldehyde resin is used, which has the advantages of low cost, homogeneity of distribution, solubility in water, high reactivity in an acid medium, and high adhesion to wood. On the other hand, as a disadvantage, there is low resistance to humidity and the release of formaldehyde. The objective of the study was to determine the viability of adding industrial boiler ash to the urea formaldehyde-based adhesive for the production of medium-density fiberboard. The raw material used was composed of Pinus spp fibers, urea-formaldehyde resin, paraffin emulsion, ammonium sulfate, and boiler ash. The experimental plan, consisting of 8 treatments, was completely randomized with a factorial arrangement, with 0%, 1%, 3%, and 5% ash added to the adhesive, with and without the application of a catalyst. In each treatment, 4 panels were produced with density of 750 kg.m⁻³, dimensions of 40 x 40 x 1,5 cm, 12% urea formaldehyde resin, 1% paraffin emulsion and hot pressing at a temperature of 180ºC, the pressure of 40 kgf/cm⁻² for a time of 10 minutes. The different compositions of the adhesive were characterized in terms of viscosity, pH, gel time and solids, and the panels by physical and mechanical properties, in addition to evaluation using the IMAL DPX300 X-ray densitometer and formaldehyde emission by the perforator method. The results showed a significant reduction of all adhesive properties with the use of the catalyst, regardless of the treatment; while the percentage increase of ashes provided an increase in the average values of viscosity, gel time, and solids and a reduction in pH for the panels with a catalyst; for panels without catalyst, the behavior was the opposite, with the exception of solids. For the physical properties, the results of the variables of density, compaction ratio, and thickness were equivalent and in accordance with the standard, while the moisture content was significantly reduced with the use of the catalyst but without the influence of the percentage of ash. The density profile for all treatments was characteristic of medium-density fiberboard, with more compacted and dense surfaces when compared to the central layer. For thickness, the swelling was not influenced by the catalyst and the use of ash, presenting average values within the normalized parameters. For mechanical properties, the influence of ashes on the adhesive was negatively observed in the modulus of rupture from 1% and in the traction test from 3%; however, only this last property, in the percentages of 3% and 5%, were below the minimum limit of the norm. The use of catalyst and ashes with percentages of 3% and 5% reduced the formaldehyde emission of the panels; however, only the panels that used adhesive with catalyst presented emissions below 8mg of formaldehyde / 100g of the panel. In this way, it can be said that boiler ash can be added to the adhesive with a catalyst without impairing the technological properties by up to 1%.

Keywords: reconstituted wood panels, formaldehyde emission, technological properties of panels, perforator

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Authors: Krasimir I. Ivanov, Elitsa N. Kolentsova, Dimitar Y. Dimitrov, Georgi V. Avdeev, Tatyana T. Tabakova

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In recent research copper and manganese systems were found to be the most active in CO and organic compounds oxidation among the base catalysts. The mixed copper manganese oxide has been widely studied in oxidation reactions because of their higher activity at low temperatures in comparison with single oxide catalysts. The results showed that the formation of spinel CuxMn3−xO4 in the oxidized catalyst is responsible for the activity even at room temperature. That is why most of the investigations are focused on the hopcalite catalyst (CuMn2O4) as the best copper-manganese catalyst. Now it’s known that this is true only for CO oxidation, but not for mixture of CO and VOCs. The purpose of this study is to investigate the alumina supported copper-manganese catalysts with different Cu/Mn molar ratio in terms of oxidation of CO, methanol and dimethyl ether. The catalysts were prepared by impregnation of γ-Al2O3 with copper and manganese nitrates and the catalytic activity measurements were carried out in continuous flow equipment with a four-channel isothermal stainless steel reactor. Gas mixtures on the input and output of the reactor were analyzed with a gas chromatograph, equipped with FID and TCD detectors. The texture characteristics were determined by low-temperature (- 196 oС) nitrogen adsorption in a Quantachrome Instruments NOVA 1200e (USA) specific surface area&pore analyzer. Thermal, XRD and TPR analyses were performed. It was established that the active component of the mixed Cu-Mn/γ–alumina catalysts strongly depends on the Cu/Mn molar ratio. Highly active alumina supported Cu-Mn catalysts for CO, methanol and DME oxidation were synthesized. While the hopcalite is the best catalyst for CO oxidation, the best compromise for simultaneous oxidation of all components is the catalyst with Cu/Mn molar ratio 1:5.

Keywords: supported copper-manganese catalysts, CO, VOCs oxidation, combustion of exhaust gases

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Authors: Corazon Virtudazo-Ligaray, Mark Daniel G. de Luna, Meng-Wei Wan, Ming-Chun Lu

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A series of ternary compound catalyst with nanocomposites of ceria, tungsten trioxide and titania (CeO2-WOx-TiO2) with different WOx mole fraction (10, 20, 30, 40) have been synthesized by sol-gel method. These nanocomposite catalysts were used for oxidative extractive desulfurization of model fuel oil, which were composed of dibenzothiophene (DBT) dissolved in toluene. The 30% hydrogen peroxide, H2O2 was used as oxidant and acetonitrile as extractant. These catalysts were characterized by SEM-EDS to determine the morphology. Catalytic oxidation results show that the catalysts have high selectivity in refractory fuel oil with organo sulfur contents. The oxidative removal of DBT increases as the HPW content increases. The nanocomposites CeO2-WOx-TiO2 also shows high selectivity for DBT oxidation in the DBT–toluene acetonitrile system. The catalytic oxidative desulfurization ratio of model fuel reached to 100% with nanocomposites CeO2-WOx-TiO2 (35-30-35) mol percent catalyst nanocomposition under 333 K in 30 minutes.

Keywords: ceria, oxidative desulfurization, titania, phosphotungstic acid

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Authors: Y. J. Lin, Y. F. Lin

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CO2 is the primary greenhouse gas which causes global warming in recent years. As the carbon capture and storage (CCS) getting maturing, the reuse of carbon dioxide which made from CCS is the important issue. In this way, the most common method is the synthesis of cyclic carbonate chemicals from the cycloaddition reaction of carbon dioxide and epoxide. The catalyst plays an important role in the CO2/epoxide cycloaddition reactions. The Lewis acid and base sites are both needed on the catalyst surface for the help of epoxide ring opening, leading to the synthesis of cyclic carbonate. Furthermore, the larger specific surface area and more active site of the catalyst are also needed to enhance the efficiency of the CO2/epoxide cycloaddition reactions. Aerogel is a mesoporous nanomaterial (pore size between 2~50 nm) with high specific surface area and porosity (at least 90%) and low density. In this study, the ternary metal oxide aerogels, Mg-doped Al2O3 aerogels, with higher specific surface area and Lewis acid and base sites on the aerogel surface are successfully prepared by using a facile sol-gel reaction. The as-prepared Mg-doped Al2O3 aerogels are also served as heterogenous catalyst for the CO2/propylene- oxide cycloaddition reaction. Compared to the pristine Al2O3 aerogels, the Mg-doped Al2O3 aerogels possessed both Lewis acid and base sites on the surface are able to enhance the efficiency of the CO2/propylene oxide cycloaddition reactions. As a result, the as-prepared Mg-doped Al2O3 aerogels are a promising and novel catalyst for the CO2/epoxide cycloaddition reactions.

Keywords: ternary, metal oxide aerogel, CO2 reuse, cycloaddition, propylene oxide

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Authors: Zhanzhao Fu, Chongyi Ling, Jinlan Wang

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Water splitting and rechargeable air-based batteries are emerging as new renewable energy storage and conversion technologies. However, the discovery of suitable catalysts with high activity and low cost remains a great challenge. In this work, we report a single-atom trifunctional catalyst, namely Ti₃C₂O₂ supported single Pd atom (Pd1@Ti₃C₂O₂), for the hydrogen evolution reaction (HER), oxygen evolution reaction (OER) and oxygen reduction reaction (ORR). This catalyst is selected from 12 candidates and possesses low overpotentials of 0.22 V, 0.31 V and 0.34 V for the HER, OER and ORR, respectively, making it an excellent electrocatalyst for both overall water splitting and rechargeable air-based batteries. The superior OER and ORR performance originates from the optimal d band center of the supported Pd atom. Moreover, the excellent activity can be maintained even if the single Pd atoms aggregate into small clusters. This work offers new opportunities for advancing the renewable energy storage and conversion technologies and paves a new way for the development of multifunctional electrocatalysts.

Keywords: DFT, SACs, OER, ORR, HER

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Authors: Victor R. Thulari, John Akach, Haleden Chiririwa, Aoyi Ochieng

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Solar-light activated titanium dioxide photocatalysts were prepared by hydrolysis of titanium (IV) isopropoxide with thiourea, followed by calcinations at 450 °C. The experiments demonstrated that methyl orange in aqueous solutions were successfully degraded under solar light using doped TiO₂. The photocatalytic oxidation of a mono azo methyl-orange dye has been investigated in multi ion doped TiO₂ and solar light. Solutions were irradiated by solar-light until high removal was achieved. It was found that there was no degradation of methyl orange in the dark and in the absence of TiO₂. Varieties of laboratory prepared TiO₂ catalysts both un-doped and doped using titanium (IV) isopropoxide and thiourea as a dopant were tested in order to compare their photoreactivity. As a result, it was found that the efficiency of the process strongly depends on the working conditions. The highest degradation rate of methyl orange was obtained at optimum dosage using commercially produced TiO₂. Our work focused on laboratory synthesized catalyst and the maximum methyl orange removal was achieved at 81% with catalyst loading of 0.04 g/L, initial pH of 3 and methyl orange concentration of 0.005 g/L using multi-ion doped catalyst. The kinetics of photocatalytic methyl orange dye stuff degradation was found to follow a pseudo-first-order rate law. The presence of the multi-ion dopant (thiourea) enhanced the photoefficiency of the titanium dioxide catalyst.

Keywords: degradation, kinetics, methyl orange, photocatalysis

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Authors: Farrukh Jamil, Ala'a H. Al-Muhtaseb, Lamya Al-Haj, Mohab A. Al-Hinai

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Date pits are major agricultural waste produced in Oman. Current work was conducted to produce jet fuel and green diesel from hydrodeoxygenation of Date pits oil in the presence of Pd/C catalyst. The hydrodeoxygenation of Date pits oil occurred to be highly efficient at following mild operating conditions such as conditions temperature 300°C pressure 10bar with continuous stirring at 500rpm. Detailed product characterization revealed that large fraction of paraffinic hydrocarbons was found which accounts up to 91.1 % which attributed due to efficient hydrodeoxygenation. Based on the type of components in product oil, it was calculated that the maximum fraction of hydrocarbons formed lies within the range of green diesel 72.0 % then jet fuel 30.4% by using Pd/C catalysts. The densities of product oil were 0.88 kg/m³, the viscosity of products calculated was 3.49 mm²/s. Calorific values for products obtained were 44.11 MJ/kg when Pd/C catalyst was used for hydrodeoxygenation. Based on products analysis it can conclude that Date pits oil could successfully utilize for synthesizing green diesel and jet fuel fraction.

Keywords: biomass, jet fuel, green diesel, catalyst

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Authors: Xin Zhao. Xuerong Zheng. Andrey L. Rogach

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Using single metal atoms has been considered an efficient way to develop new HER and OER catalysts. MXenes, a class of two-dimensional materials, have attracted tremendous interest as promising substrates for single-atom metal catalysts. However, there is still a lack of systematic investigations on the interaction mechanisms between various MXenes substrates and single atoms. Besides, due to the poor interaction between metal atoms and substrates resulting in low loading and stability, dual-atom MXenes-based catalysts have not been successfully synthesized. We summarized the electrocatalytic enhancement mechanism of three MXenes-based single-atom catalysts through experimental and theoretical results demonstrating the stronger hybridization between Co 3d and surface-terminated O 2p orbitals, optimizing the electronic structure of Co single atoms in the composite. This, in turn, lowers the OER and HER energy barriers and accelerates the catalytic kinetics in the case of the Co@V2CTx composite. The poor interaction between single atoms and substrates can be improved by a surface modification to synthesize dual-atom catalysts. The synergistic electronic structure enhances the stability and electrocatalytic activity of the catalyst. Our study provides guidelines for designing single-atom and dual-atom MXene-based electrocatalysts and sheds light on the origins of the catalytic activity of single-atoms on MXene substrates.

Keywords: dual-atom catalyst, single-atom catalyst, MXene substrates, water splitting

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Authors: Majid Farsadrouh Rashti, Amir Shafiee Kisomi, Parisa Jahani

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The direct ethanol fuel cells (DEFCs) are contemplated as a promising energy source because, In addition to being used in portable electronic devices, it is also used for electric vehicles. The synthesis of bimetallic nanostructures due to their novel optical, catalytic and electronic characteristic which is precisely in contrast to their monometallic counterparts is attracting extensive attention. Galvanic replacement (sometimes is named to as cementation or immersion plating) is an uncomplicated and effective technique for making nanostructures (such as core-shell) of different metals, semiconductors, and their application in DEFCs. The replacement of galvanic does not need any external power supply compared to electrodeposition. In addition, it is different from electroless deposition because there is no need for a reducing agent to replace galvanizing. In this paper, a fast method for the palladium (Pd) wire nanostructures synthesis with the great surface area through galvanic replacement reaction utilizing copper nanowires (CuNWS) as a template by the assistance of ultrasound under room temperature condition is proposed. To evaluate the morphology and composition of Pd@ Copper nanowires/MultiWalled Carbon nanotubes-Chitosan, emission scanning electron microscopy, energy dispersive X-ray spectroscopy were applied. In order to measure the phase structure of the electrocatalysts were performed via room temperature X-ray powder diffraction (XRD) applying an X-ray diffractometer. Various electrochemical techniques including chronoamperometry and cyclic voltammetry were utilized for the electrocatalytic activity of ethanol electrooxidation and durability in basic solution. Pd@ Copper nanowires/MultiWalled Carbon nanotubes-Chitosan catalyst demonstrated substantially enhanced performance and long-term stability for ethanol electrooxidation in the basic solution in comparison to commercial Pd/C that demonstrated the potential in utilizing Pd@ Copper nanowires/MultiWalled Carbon nanotubes-Chitosan as efficient catalysts towards ethanol oxidation. Noticeably, the Pd@ Copper nanowires/MultiWalled Carbon nanotubes-Chitosan presented excellent catalytic activities with a peak current density of 320.73 mAcm² which was 9.5 times more than in comparison to Pd/C (34.2133 mAcm²). Additionally, activation energy thermodynamic and kinetic evaluations revealed that the Pd@ Copper nanowires/MultiWalled Carbon nanotubes-Chitosan catalyst has lower compared to Pd/C which leads to a lower energy barrier and an excellent charge transfer rate towards ethanol oxidation.

Keywords: core-shell structure, electrocatalyst, ethanol oxidation, galvanic replacement reaction

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Authors: Yeidy Sorani Montenegro Camacho, Samir Bensaid, Nunzio Russo, Debora Fino

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LiFeO2 nano-powders were prepared via solution combustion synthesis (SCS) method and were used as carbon gasification catalyst in a reduced atmosphere. The gasification of soot with CO2 and H2O in the presence of CO and H2 (syngas atmosphere) were also investigated under atmospheric conditions using a fixed-bed micro-reactor placed in an electric, PID-regulated oven. The catalytic bed was composed of 150 mg of inert silica, 45 mg of carbon (Printex-U) and 5 mg of catalyst. The bed was prepared by ball milling the mixture at 240 rpm for 15 min to get an intimate contact between the catalyst and soot. A Gas Hourly Space Velocity (GHSV) of 38.000 h-1 was used for the tests campaign. The furnace was heated up to the desired temperature, a flow of 120 mL/min was sent into the system and at the same time the concentrations of CO, CO2 and H2 were recorded at the reactor outlet using an EMERSON X-STREAM XEGP analyzer. Catalytic and non-catalytic soot gasification reactions were studied in a temperature range of 120°C – 850°C with a heating rate of 5 °C/min (non-isothermal case) and at 650°C for 40 minutes (isothermal case). Experimental results show that the gasification of soot with H2O and CO2 are inhibited by the H2 and CO, respectively. The soot conversion at 650°C decreases from 70.2% to 31.6% when the CO is present in the feed. Besides, the soot conversion was 73.1% and 48.6% for H2O-soot and H2O-H2-soot gasification reactions, respectively. Also, it was observed that the carbon gasification in mixed atmosphere, i.e., when simultaneous carbon gasification with CO2 and steam take place, with H2 and CO as co-reagents; the gasification reaction is strongly inhibited by CO and H2, as well has been observed in single atmospheres for the isothermal and non-isothermal reactions. Further, it has been observed that when CO2 and H2O react with carbon at the same time, there is a passive cooperation of steam and carbon dioxide in the gasification reaction, this means that the two gases operate on separate active sites without influencing each other. Finally, despite the extreme reduced operating conditions, it has been demonstrated that the 32.9% of the initial carbon was gasified using LiFeO2-catalyst, while in the non-catalytic case only 8% of the soot was gasified at 650°C.

Keywords: soot gasification, nanostructured catalyst, reducing environment, syngas

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Authors: Ana M. Antolín, Sandra Contreras, Francesc Medina, Didier Tichit

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Introduction: High levels of nitrates (> 50 ppm NO3-) in drinking water are potentially risky to human health. In the recent years, the trend of nitrate concentration in groundwater is rising in the EU and other countries. Conventional catalytic nitrate reduction processes into N2 and H2O lead to some toxic intermediates and by-products, such as NO2-, NH4+, and NOx gases. Alternatively, photocatalytic nitrate removal using solar irradiation and heterogeneous catalysts is a very promising and ecofriendly technique. It has been scarcely performed and more research on highly efficient catalysts is still needed. In this work, different nanocatalysts supported on Aeroxide Titania P25 (P25) have been prepared varying: 0.5-4 % wt. Ag); Pt (2, 4 % wt.); Pt precursor (H2PtCl6/K2PtCl6); and impregnation order of both metals. Pt was chosen in order to increase the selectivity to N2 and decrease that to NO2-. Catalysts were characterized by nitrogen physisorption, X-Ray diffraction, UV-visible spectroscopy, TEM and X Ray-Photoelectron Spectroscopy. The aim was to determine the influence of the composition and the preparation method of the catalysts on the conversion and selectivity in the nitrate reduction, as well as going through an overall and better understanding of the process. Nanocatalysts synthesis: For the mono and bimetallic catalysts preparation, wise-drop wetness impregnation of the precursors (AgNO3, H2PtCl6, K2PtCl6) followed by a reduction step (NaBH4) was used to obtain the metal colloids. Results and conclusions: Denitration experiments were performed in a 350 mL PTFE batch reactor under inert standard operational conditions, ultraviolet irradiations (λ=254 nm (UV-C); λ=365 nm (UV-A)), and presence/absence of hydrogen gas as a reducing agent, contrary to most studies using oxalic or formic acid. Samples were analyzed by Ionic Chromatography. Blank experiments using respectively P25 (dark conditions), hydrogen only and UV irradiations without hydrogen demonstrated a clear influence of the presence of hydrogen on nitrate reduction. Also, they demonstrated that UV irradiation increased the selectivity to N2. Interestingly, the best activity was obtained under ultraviolet lamps, especially at a closer wavelength to visible light irradiation (λ = 365 nm) and H2. 2% Ag/P25 leaded to the highest NO3- conversion among the monometallic catalysts. However, nitrite quantities have to be diminished. On the other hand, practically no nitrate conversion was observed with the monometallics based on Pt/P25. Therefore, the amount of 2% Ag was chosen for the bimetallic catalysts. Regarding the bimetallic catalysts, it is observed that the metal impregnation order, amount and Pt precursor highly affects the results. Higher selectivity to the desirable N2 gas is obtained when Pt was firstly added, especially with K2PtCl6 as Pt precursor. This suggests that when Pt is secondly added, it covers the Ag particles, which are the most active in this reaction. It could be concluded that Ag allows the nitrate reduction step to nitrite, and Pt the nitrite reduction step toward the desirable N2 gas.

Keywords: heterogeneous catalysis, hydrogenation, nanocatalyst, nitrate removal, photocatalysis

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Authors: Shashank Bahri, Divyanshu Arya, Rajni Jain, Sreedevi Upadhyayula

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Petroleum products can be obtained from syngas catalytic conversion using Fischer Tropsch Reaction. The liquid fuels obtained from FTS are sulphur and nitrogen free and thus may easily meet the increasing stringent environment regulations. In the present work we have synthesized Meso porous ZSM-5 supported catalyst. Meso structure were created in H-ZSM-5 crystallites by demetalation via subsequent base and acid treatment. Desilication through base treatment provides H-ZSM-5 with pore size and volumes similar to amorphous SiO2 (Conventional Carrier). Modifying the zeolite texture and surface chemistry by Desilication and acid washing alters its accessibility and interactions with metal phase and consequently the CO adsorption behavior and hydrocarbon product distribution. Increasing the mesoporosity via desilication provides the micro porous zeolite with essential surface area to support optimally sized metal crystallites. This improves the metal dispersion and hence improve the activity of the catalyst. Transition metal (Co) was loaded using wet impregnation method. Synthesized catalysts were characterized by Infrared Spectroscopy, Powdered X-Ray Diffraction, Scanning Electron Microscopy (SEM), BET Method analytical techniques. Acidity of the catalyst which plays an important role in FTS reaction was measured by DRIFT setup pyridine adsorption instead of NH3 Temperature Programmed Desorption. The major difference is that, Pyridine Adsorption can distinguish between Lewis acidity and Bronsted Acidity, thus giving their relative strengths in the catalyst sample, whereas TPD gives total acidity including Lewis and Bronsted ones.

Keywords: mesopourus, fischer tropsch reaction, pyridine adsorrption, drift study

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Authors: Wei-Jing Li, Ren-Xuan Yang, Kui-Hao Chuang, Ming-Yen Wey

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Nowadays, plastic product and utilization are extensive and have greatly improved our life. Yet, plastic wastes are stable and non-biodegradable challenging issues to the environment. Waste-to-energy strategies emerge a promising way for waste management. This work investigated the co-production of hydrogen and carbon nanotubes from the syngas which was from the gasification of polypropylene. A nickel-silica core-shell catalyst was applied for syngas reaction from plastic waste gasification in a fixed-bed reactor. SiO2 were prepared through various synthesis solvents by Stöber process. Ni plays a role as modified SiO2 support, which were synthesized by deposition-precipitation method. Core-shell catalysts have strong interaction between active phase and support, in order to avoid catalyst sintering. Moreover, Fe or Co metal acts as promoter to enhance catalytic activity. The effects of calcined atmosphere, second metal addition, and reaction temperature on hydrogen production and carbon yield were examined. In this study, the catalytic activity and carbon yield results revealed that the Ni/SiO2 catalyst calcined under H2 atmosphere exhibited the best performance. Furthermore, Co promoted Ni/SiO2 catalyst produced 3 times more than Ni/SiO2 on carbon yield at long-term operation. The structure and morphological nature of the calcined and spent catalysts were examined using different characterization techniques including scanning electron microscopy, transmission electron microscopy, X-ray diffraction. In addition, the quality and thermal stability of the nano-carbon materials were also evaluated by Raman spectroscopy and thermogravimetric analysis.

Keywords: plastic wastes, hydrogen, carbon nanotube, core-shell catalysts

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Authors: M. Belhadj Lachachi, Tayeb Benabdallah, M. Hadj Youcef, Jason M. Lynama

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The application of inorganic chemistry to catalysis and environmental chemistry is a rapidly developing field, and novel catalytic metal complexes are now having an impact on the industrial development practice. Advances in organometallic chemistry are crucial for improving the design of compounds to reduce toxic side effects and understand their mechanisms of action. The reaction of platinum(II) organometallic complexes with bidentate Schiff bases derived from 2-Hydroxynaphtalydeneaniline have been carried out. It concerns N,N’-naphtalidene para-nitroaniline (1-a), the, the N,N’-naphtalidene para-ethoxyaniline (1-b), the N,N’-naphtalideneaniline (1-c), the N,N’-naphtalidene para-chloroaniline (1-d) and the N,N’-naphtalidene para-methoxyaniline (1-e). The ligands were fully characterized by I.R., elemental analysis, 1H-NMR, 13C-NMR, ESI Mass Spectrometry and X-Ray Diffraction. The resulting metal complexes were obtained as a cationic species, through a simple substitution reaction, leading to two geometric isomers [1, 2], and characterized by IR, 1H-NMR, 13C-NMR, LIFDI Mass Spectrometry and supported by Elemental Analysis and X-Ray diffraction. Furthermore, a bimetallic platinum complex was prepared from the same ligands and dichloro(1,5-cyclooctadiene)platinum and characterized by X-Ray diffraction [3]The catalytic properties of the prepared platinum complexes in the hydrogenative and dehydrogenative silylation of styrene were investigated, and reaction kinetics conversion to products was determined by 1H-NMR and confirmed by GC-MS. This presentation will detail a comparison of the catalytic activity of five platinum organometallic complexes bearing different Schiff base ligands in the hydrosilylation of styrene, varying the experimental conditions of temperature, nature of the complex and the loading of the catalyst.

Keywords: catalysis, hydrosilylation, organometallic, schiff base

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Authors: Olga A. Krysiak, Grzegorz Cichowicz, Wojciech Hyk, Michal Cyranski, Jan Augustynski

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Metal oxides are known electrocatalyst in water oxidation reaction. Due to the fact that it is desirable for efficient oxygen evolution catalyst to contain numerous redox-active metal ions to guard four electron water oxidation reaction, mixed metal oxides exhibit enhanced catalytic activity towards oxygen evolution reaction compared to single metal oxide systems. On the surface of fluorine doped tin oxide coated glass slide (FTO) deposited (doctor blade technique) mixed metal oxide layer composed of nickel, iron, and chromium. Oxide coating was acquired by heat treatment of the aqueous precursors' solutions of the corresponding salts. As-prepared electrodes were photosensitive and acted as an efficient oxygen evolution catalyst. Our results showed that obtained by this method electrodes can be activated which leads to achieving of higher current densities. The recorded current and photocurrent associated with oxygen evolution process were at least two orders of magnitude higher in the presence of oxide layer compared to bare FTO electrode. The overpotential of the process is low (ca. 0,2 V). We have also checked the activity of the catalyst at different known photoanodes used in sun-driven water splitting. Herein, we demonstrate that we were able to achieve efficient oxygen evolution catalysts using relatively cheap precursor consisting of earth abundant metals and simple method of preparation.

Keywords: chromium, electrocatalysis, iron, metal oxides, nickel, oxygen evolution

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Authors: Lina F. Ballesteros, Hafsae Lamsaf, Miguel A. Cerqueira, Lorenzo M. Pastrana, Sandra Carvalho, Jose A. Teixeira, S. Calderon V.

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The use of bio-based packaging materials containing metallic and bimetallic nanostructures is relatively modern technology. In this sense, the food packaging industry has been investigating biological and renewable resources that can replace petroleum-based materials to reduce the environmental impact and, at the same time, including new functionalities using nanotechnology. Therefore, the main objective of the present work consisted of developing bio-based poly-lactic acid (PLA) films with Zinc (Zn) and Zinc-Iron (Zn-Fe) nanostructures deposited by magnetron sputtering. The structural, antimicrobial, and optical properties of the films were evaluated when exposed at 60% and 96% relative humidity (RH). The morphology and elemental analysis of the samples were determined by scanning (transmission) electron microscopy (SEM and STEM), and inductively coupled plasma optical emission spectroscopy (ICP-OES). The structure of the PLA was monitored before and after deposition by Fourier transform infrared spectroscopy (FTIR) analysis, and the antimicrobial and color assays were performed by using the zone of inhibition (ZOI) test and a Minolta colorimeter, respectively. Finally, the films were correlated in terms of the deposit conditions, Zn or Zn-Fe concentrations, and thickness. The results revealed PLA films with different morphologies, compositions, and thicknesses of Zn or Zn-Fe nanostructures. The samples showed a significant antibacterial and antifungal activity against E. coli, P. aeruginosa, P. fluorescens, S. aureus, and A. niger, and considerable changes of color and opacity at 96% RH, especially for the thinner nanostructures (150-250 nm). On the other hand, when the Fe fraction was increased, the lightness of samples increased, as well as their antimicrobial activity when compared to the films with pure Zn. Hence, these findings are relevant to the food packaging field since intelligent and active films with multiple properties can be developed.

Keywords: biopolymers, functional properties, magnetron sputtering, Zn and Zn-Fe nanostructures

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Authors: Yuri A. Kalvachev, Totka D. Todorova

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Zeolite mordenite has been investigated as a transition metal support for the preparation of efficient catalysts in the oxidation of volatile organic compounds (VOCs). The highly crystalline mordenite samples were treated with hydrofluoric acid and ammonium fluoride to get hierarchical material with secondary porosity. The obtained supports by this method have a high active surface area, good diffusion properties and prevent the extraction of metal components during catalytic reactions. The active metal phases platinum and copper were loaded by impregnation on both mordenite materials (parent and acid treated counterparts). Monometalic Pt and Cu, and bimetallic Pt/Cu catalysts were obtained. The metal phases were fine dispersed as nanoparticles on the functional porous materials. The catalysts synthesized in this way were investigated in the reaction of complete oxidation of propane and benzene. Platinum, copper and platinum/copper were loaded and there catalytic activity was investigated and compared. All samples are characterized by X-ray diffraction analysis, nitrogen adsorption, scanning electron microscopy (SEM), X-ray photoelectron measurements (XPS) and temperature programed reduction (TPR). The catalytic activity of the samples obtained is investigated in the reaction of complete oxidation of propane and benzene by using of Gas Chromatography (GC). The oxidation of three organic molecules was investigated—methane, propane and benzene. The activity of metal loaded mordenite catalysts for methane oxidation is almost the same for parent and treated mordenite as a support. For bigger molecules as propane and benzene, the activity of catalysts based on treated mordenite is higher than those based on parent zeolite.

Keywords: metal loaded catalysts, mordenite, VOCs oxidation, zeolites

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Authors: E. Kolvari, N. Koukabi, A. Sabet, A. Fakhraee, M. Ramezanpour

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A green and efficient method for oxidation of thiols to the corresponding disulfides is reported using free nano-iron oxide in the H2O2 and methanol as solvent at room tempereture. H2O2 is anoxidant for S-S coupling variety aromatic of thiols to corresponding disulfide in the presence of supported iron oxide as recoverable catalyst. This reaction is clean, fast, mild and easy work-up with no side reaction.

Keywords: thiol, disulfide, free nano-iron oxide, H2O2, oxidation, coupling

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Authors: Nagwa Mourad Abdelazeem, Marwa El-hussieny

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Multicomponent reactions (MCRs), one-pot reactions form products from more than two different starting compounds. (MCRs) are ideal reaction systems leading to high structural diversity and molecular complexity through a single transformation. (MCRs) have a lot of advantage such as higher yield, less waste generation, use of readily available starting materials and high atom. (MCRs) provide a rapid process for efficient synthesis of key structures in discovery of drug on the other hand silica sulfuric acid (SSA) has been used as an efficient heterogeneous catalyst for many organic transformations. (SSA) is low cost, ease of preparation, catalyst recycling, and ease of handling, so in this article we used 2-(thiophen-2-yl)-1H-indole, N-substituted anilines and aldehyde in the presence of silica sulfuric acid (SSA) as a catalyst in water as solvent at room temperature to prepare 3,3'-(phenylmethylene)bis(2-(thiophen-2-yl)-1H-indole) and N-methyl-4-(phenyl(2-(thiophen-2-yl)-1H-indol-3-yl)methyl)aniline derivatives Via one-pot reaction. Compound 2-(thiophen-2-yl)-1H-indole belongs to the ubiquitous class of indoles which enjoy broad synthetic, biological and industrial applications ]. Cancer is considered the first or second most common reason of death all through the world. So the synthesized compounds will be tested as anticancer. We expected the synthesized compounds will give good results comparison to the reference drug.

Keywords: aldehydes, aza-friedel-crafts reaction, indole, multicomponent reaction

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Authors: Ouahiba Bechiri, Mostefa Abbessi

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The color removal from industrial effluents is a major concern in wastewater treatment. The main objective of this work was to study the decolorization of a mixture of Orange G acid (OG) and naphthol blue black dye (NBB) in aqueous solution by hydrogen peroxide using [H1,5Fe1,5P2W12Mo6O61,23H2O] as catalyst. [H1,5Fe1,5P2 W12Mo6O61,23H2O] is a recyclable DAWSON type heteropolyanion. Effects of various experimental parameters of the oxidation reaction of the dye were investigated. The studied parameters were: the initial pH, H2O2 concentration, the catalyst mass and the temperature. The optimum conditions had been determined, and it was found that efficiency of degradation obtained after 15 minutes of reaction was about 100%. The optimal parameters were: initial pH = 3; [H2O2]0 = 0.08 mM; catalyst mass = 0.05g; for a concentration of dyes = 30mg/L.

Keywords: Dawson type heteropolyanion, naphthol blue-black, dye degradation, orange G acid, oxidation, hydrogen peroxide

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Authors: Jin Lin, Shouxiang Lu, Kim Meow Liew

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The requirement for the long-term mission of the submarine and spacecraft has made the removal of CO₂ and trace CO the critical technology to ensure the health and life of the crews. In this work, CuMnCe, a metal oxide catalyst, supporting K₂CO₃ sorbent was prepared by the wet-solid state impregnation method to realize the integrated CO and CO₂ removal, which might also reduce the volume/mass load of the purification units in the limited space. The as-prepared samples with different addition amount of K₂CO₃ were tested using the fixed bed reactor to reveal the CO oxidation and CO₂ absorption behavior. And the regeneration and stability experiments were also conducted. The results showed that the samples realized the catalyst and sorbent integration to capture CO and CO₂ at the same time. The addition amount of the sorbent had a weak influence on the CO oxidation performance. While the addition amount affected the CO₂ sorption efficiency and capacity significantly. Meanwhile, the presence of water vapor could reduce the CO oxidation activity of the samples similarly, whether with K2CO3 sorbent addition or not. Furtherly, regeneration and stability experiment results showed that the samples after 3-5 times regeneration exhibited almost the same performance of CO and CO₂ removal. Summarily, CuMnCe catalyst supporting K₂CO₃ sorbent could be a good attempt to control CO and CO₂ pollutants generated from the daily equipment running and staff breathing in the confined space such as submarine and spacecraft.

Keywords: CO oxidation, CO₂ absorptio, potassium carbonate, CuMnCe metal oxide, confined space

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Authors: Elitsa Kolentsova, Dimitar Dimitrov, Vasko Idakiev, Tatyana Tabakova, Krasimir Ivanov

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Formaldehyde production by selective oxidation of methanol is an important industrial process. The main by-products in the waste gas are CO and dimethyl ether (DME). The idea of this study is to combine the advantages of both Cu-Mn and Cu-Co catalytic systems by obtaining a new mixed Cu-Mn-Co catalyst with high activity and selectivity at the simultaneous oxidation of CO, methanol, and DME. Two basic Cu-Mn samples with high activity were selected for further investigation: (i) manganese-rich Cu-Mn/γ–Al2O3 catalyst with Cu/Mn molar ratio 1:5 and (ii) copper-rich Cu-Mn/γ-Al2O3 catalyst with Cu/Mn molar ratio 2:1. Manganese in these samples was replaced by cobalt in the whole concentration region, and catalytic properties were determined. The results show a general trend of decreasing the activity toward DME oxidation and increasing the activity toward CO and methanol oxidation with the increase of cobalt up to 60% for both groups of catalyst. This general trend, however, contains specific features, depending on the composition of the catalyst and the nature of the oxidized gas. The catalytic activity of the sample with Cu/(Mn+Co) molar ratio of 2:1 is gradually changed with increasing the cobalt content. The activity of the sample with Cu/(Mn+Co) molar ratio of 1: 5 passes through a maximum at 60% manganese replacement by cobalt, probably due to the formation of highly dispersed Co-based spinel structures (Co3O4 and/or MnCo2O4). In conclusion, the present study demonstrates that the Cu-Mn-Co/γ–alumina supported catalysts have enhanced activity toward CO, methanol and DME oxidation. Cu/(Mn+Co) molar ratio 1:5 and Co/Mn molar ratio 1.5 in the active component can ensure successful oxidation of CO, CH3OH and DME. The active component of the mixed Cu-Mn-Co/γ–alumina catalysts consists of at least six compounds - CuO, Co3O4, MnO2, Cu1.5Mn1.5O4, MnCo2O4 and CuCo2O4, depending on the Cu/Mn/Co molar ratio. Chemical composition strongly influences catalytic properties, this effect being quite variable with regards to the different processes.

Keywords: Cu-Mn-Co catalysts, oxidation, carbon oxide, VOCs

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Authors: Kumaresh Selvakumar, Man Young Kim

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Catalytic combustor substantially reduces emission entailing fuel-air premixing at very low equivalence ratios. The catalytic combustion of natural gas has the potential to become sufficiently active at light off temperature by the convection of heat from the catalyst surface. Only one channel is selected to investigate both the gas and surface reactions in the catalyst bed because of the honeycomb structure of the catalytic combustor. The objective of the present study is to find the methane catalytic combustion behavior inside the catalytic combustor, where the gas phase kinetics is employed by homogeneous methane combustion and surface chemistry is described with the heterogeneous catalysis of the oxidation of methane on a platinum catalyst. The reaction of the premixed mixture in the catalytic regime improves flame stability with complete combustion for lower operating flame temperature. An overview of the flow behavior is presented inside the single channel catalytic combustor including the operation of catalytic combustion with various F/A ratios and premixed inlet temperature.

Keywords: catalytic combustor, equivalence ratios, flame temperature, heterogeneous catalysis, homogeneous combustion

Procedia PDF Downloads 264