Search results for: gold catalysts

Authors: Dinda A. Utami, Muhammad N. Alfarizi

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The purpose of this study was to determine the ability of zeolite catalyst for the trans- esterification reaction in biodiesel production from animal fat. The ability of the zeolite as a catalyst is determined by the structure and composition of the zeolite. An important factor that determines the properties of zeolites in catalysis includes adsorption capability to the compound of the reactants. Zeolites with a pore size of specific properties selectively adsorbing molecules. A molecule can be adsorbed by either the zeolite cavities if the size and shape of the molecule in accordance with the size and shape of the cavity in the zeolite. At this time, it is common to use homogeneous catalysts for biodiesel. We know these catalysts have some disadvantages in its use. Such as the difficulty of separation of the product with the catalyst, the generation of waste that is harmful to the environment due to residual catalysts can’t be reused, and the difficulty of handling and storage. But nowadays, solid catalyst developed technically to improve the efficiency of biodiesel production. In this case of study, we used trans-esterification process wherein the triglyceride is reacted with an alcohol with zeolite as a solid catalyst and it will produce biodiesel and glycerol as a byproduct. Development of solid catalyst seems to be the perfect solution to address the problems associated with homogeneous catalysts.

Keywords: biodiesel, animal fat, trans esterification, zeolite catalyst

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Authors: Inalegwu Stephany Akipu

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Before the advent of Colonialists on the shores of Nigeria between the 16th and 17th Centuries, there existed the traditional systems of governance which was successful with Women as active participants. However, the current state of politics in Nigeria reveals an obvious absence of women in the Country’s governance. Being that the economy rests on the quality of leaders and their constructive contribution to the plight of the masses, it becomes pertinent to exhaust all the avenues that may be open to good governance-women inclusive. It is against this backdrop that this paper attempts to compare the machinery that were in place in pre-colonial Nigerian governance that aided the womenfolk to successfully reign or assist in leadership with the seeming lack of interest by women in present times. Factors that militate against the women will also be highlighted. Furthermore, suggestions are made on how to revive these successful traditional systems of governance. The paper concludes by emphasising the role of women as the needed catalysts for this aforementioned rehabilitation of traditional systems and the impact of media in achieving this feat.

Keywords: catalysts, governance, media, rehabilitation

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Authors: O. S. Adeyemi, C. G. Whiteley

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The present study determined the toxic potential of metal nanoparticles in cell culture system. Silver and gold nanoparticles were synthesized and characterized following established "green" protocols. The synthesized nanoparticles, in varying concentrations ranging from 0.1–100 µM were evaluated for toxicity in metastatic MDA-MB-231 cells. The nanoparticles promoted a generation of reactive oxygen species and reduced cell viability to less than 50% in the demonstration of cellular toxicity. The nanoparticles; gold and the silver-gold mixture had IC50 values of 56.65 and 18.44 µM respectively. The IC50 concentration for silver nanoparticles could not be determined. Furthermore, the probe of the cell death using flow cytometry and confocal microscopy revealed the partial involvement of apoptosis as well as necrosis. Our results revealed cellular toxicity caused by the nanoparticles but the mechanism remains yet undefined.

Keywords: cell death, nanomedicine, nanotoxicology, toxicity

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Authors: Iwona Misztalewska-Turkowicz, Agnieszka Z. Wilczewska, Karolina H. Markiewicz

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Carbenes - species which possess neutral carbon atom with two shared and two unshared valence electrons, are known for their high reactivity and instability. Nevertheless, it is also known, that some carbenes i.e. N-heterocyclic carbenes (NHCs), can form stable crystals. The usability of NHCs in organic synthesis was studied. Due to their exceptional properties (high nucleophilicity) NHCs are commonly used as organocatalysts and also as ligands in transition metal complexes. NHC ligands possess better electron-donating properties than phosphines. Moreover, they exhibit lower toxicity. Due to these features, phosphines are frequently replaced by NHC ligands. In this research is discussed the synthesis of five-membered NHCs which are mainly obtained by deprotonation of azolium salts, e.g., imidazolium or imidazolinium salts. Some of them are immobilized on a solid support what leads to formation of heterogeneous, recyclable catalysts. Magnetic nanoparticles (MNPs) are often used as a solid support for catalysts. MNPs can be easily separated from the reaction mixture using an external magnetic field. Due to their low size and high surface to volume ratio, they are a good choice for immobilization of catalysts. Herein is presented synthesis of N-heterocyclic carbene copper complexes directly on the surface of magnetic nanoparticles. Formation of four different catalysts is discussed. They vary in copper oxidation state (Cu(I) and Cu(II)) and structure of NHC ligand. Catalysts were tested in Huisgen reaction, a type of copper catalyzed azide-alkyne cycloaddition (CuAAC) reaction. Huisgen reaction represents one of the few universal and highly efficient reactions in which 1,2,3-triazoles can be obtained. The catalytic activity of all synthesized catalysts was compared with activity of commercially available ones. Different reaction conditions (solvent, temperature, the addition of reductant) and reusability of the obtained catalysts were investigated and are discussed. The project was financially supported by National Science Centre, Poland, grant no. 2016/21/N/ST5/01316. Analyses were performed in Centre of Synthesis and Analyses BioNanoTechno of University of Bialystok. The equipment in the Centre of Synthesis and Analysis BioNanoTechno of University of Bialystok was funded by EU, as a part of the Operational Program Development of Eastern Poland 2007-2013, project: POPW.01.03.00-20-034/09-00 and POPW.01.03.00-20-004/11.

Keywords: N-heterocyclic carbenes, click reaction, magnetic nanoparticles, copper catalysts

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Authors: A. S. Al-Fatesh, A. A. Ibrahim, A. M. AlSharekh, F. S. Alqahtani, S. O. Kasim, A. H. Fakeeha

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Hydrogen is the expected future fuel since it produces energy without any pollution. It can be used as a fuel directly or through the fuel cell. It is also used in chemical and petrochemical industry as reducing agent or in hydrogenation processes. It is produced by different methods such as reforming of hydrocarbon, electrolytic method and methane decomposition. The objective of the present paper is to study the decomposition of methane reaction at 700°C and 800°C. The catalysts were prepared via impregnation method using 20%Fe and different proportions of combined alumina and silica support using the following ratios [100%, 90%, 80%, and 0% Al₂O₃/SiO₂]. The prepared catalysts were calcined and activated at 600 OC and 500 OC respectively. The reaction was carried out in fixed bed reactor at atmospheric pressure using 0.3g of catalyst and feed gas ratio of 1.5/1 CH₄/N₂ with a total flow rate 25 mL/min. Catalyst characterizations (TPR, TGA, BET, XRD, etc.) have been employed to study the behavior of catalysts before and after the reaction. Moreover, a brief description of the weight loss and the CH₄ conversions versus time on stream relating the different support ratios over 20%Fe/Al₂O₃/SiO₂ catalysts has been added as well. The results of TGA analysis provided higher weights losses for catalysts operated at 700°C than 800°C. For the 90% Al₂O₃/SiO₂, the activity decreases with the time on stream using 800°C reaction temperature from 73.9% initial CH₄ conversion to 46.3% for a period of 300min, whereas the activity for the same catalyst increases from 47.1% to 64.8% when 700°C reaction temperature is employed. Likewise, for 80% Al₂O₃/SiO₂ the trend of activity is similar to that of 90% Al₂O₃/SiO₂ but with a different rate of activity variation. It can be inferred from the activity results that the ratio of Al₂O₃ to SiO₂ is crucial and it is directly proportional with the activity. Whenever the Al/Si ratio decreases the activity declines. Indeed, the CH₄ conversion of 100% SiO₂ support was less than 5%.

Keywords: Al₂O₃, SiO₂, CH₄ decomposition, hydrogen, iron

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Authors: Emmanuel Agunloye, Asterios Gavriilidis, Luca Mazzei

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Gold nanoparticles are commonly synthesized by reducing chloroauric acid with sodium citrate. This method, referred to as the citrate method, can produce spherical gold nanoparticles (NPs) in the size range 10-150 nm. Gold NPs of this size are useful in many applications. However, the NPs are usually polydisperse and irreproducible. A better understanding of the synthesis mechanisms is thus required. This work thoroughly investigated the only model that describes the synthesis. This model combines mass and population balance equations, describing the NPs synthesis through a sequence of chemical reactions. Chloroauric acid reacts with sodium citrate to form aurous chloride and dicarboxy acetone. The latter organizes aurous chloride in a nucleation step and concurrently degrades into acetone. The unconsumed precursor then grows the formed nuclei. However, depending on the pH, both the precursor and the reducing agent react differently thus affecting the synthesis. In this work, we investigated the model for different conditions of pH, temperature and initial reactant concentrations. To solve the model, we used Parsival, a commercial numerical code, whilst to test it, we considered various conditions studied experimentally by different researchers, for which results are available in the literature. The model poorly predicted the experimental data. We believe that this is because the model does not account for the acid-base properties of both chloroauric acid and sodium citrate.

Keywords: citrate method, gold nanoparticles, Parsival, population balance equations, Turkevich organizer theory

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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: Elaf Ahmed, Shahid Rasul, Ohoud Alharbi, Peng Wang

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Ultra-Small Nanoparticles of metals (USNPs) have attracted the attention from the perspective of both basic and developmental science in a wide range of fields. These NPs exhibit electrical, optical, magnetic, and catalytic phenomena. In addition, they are considered effective catalysts because of their enormously large surface area. Many chemical methods of synthesising USNPs are reported. However, the drawback of these methods is the use of different capping agents and ligands in the process of the production such as Polyvinylpyrrolidone, Thiol and Ethylene Glycol. In this research ultra-small nanoparticles of gold, palladium and platinum metal have been successfully produced using electrochemically active biofilm (EAB) after optimising the pH of the media. The production of ultra-small nanoparticles has been conducted in a reactor using a simple two steps method. Initially biofilm was grown on the surface of a carbon paper for 7 days using Shewanella Loihica bacteria. Then, biofilm was employed to synthesise platinum, palladium and gold nanoparticles in water using sodium lactate as electron donor without using any toxic chemicals at mild operating conditions. Electrochemically active biofilm oxidise the electron donor and produces electrons in the solution. Since these electrons are a strong reducing agent, they can reduce metal precursors quite effectively and quickly. The As-synthesized ultra-small nanoparticles have a size range between (2-7nm) and showed excellent catalytic activity on the degradation of methyl orange. The growth of metal USNPs is strongly related to the condition of the EAB. Where using low pH for the synthesis was not successful due to the fact that it might affect and destroy the bacterial cells. However, increasing the pH to 7 and 9, led to the successful formation of USNPs. By changing the pH value, we noticed a change in the size range of the produced NPs. The EAB seems to act as a Nano factory for the synthesis of metal nanoparticles by offering a green, sustainable and toxic free synthetic route without the use of any capping agents or ligands and depending only on their respiration pathway.

Keywords: electrochemically active biofilm, electron donor, shewanella loihica, ultra-small nanoparticles

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Authors: T. P. Oladele, C. A. Snyders, S. M. Bradshaw, G. Akdogan

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The effect of temperature, contact time and agitation during pre-treatment was investigated on the elution of gold from granular activated carbon at fixed caustic-cyanide concentration and elution conditions. It was shown that there are interactions between parameters during pre-treatment. At 80oC, recovery is independent of the contact time while the maximum recovery is obtained in the absence of agitation (0rpm). Increase in agitation speed from 0 rev/min to 1200 rev/min showed a decrease in recovery of approximately 20 percent at 80°C. Recovery with increased time from 15 minutes to 45 minutes is only pronounced at 25°C with approximately 4 percent increase at all agitation speeds. The results from elution recovery are aimed to give insight into the mechanisms of pre-treatment under the combinations of the chosen parameters.

Keywords: gold, temperature, contact time, agitation speed, recovery

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Authors: Sergey Svita, Valeriy Astapenko

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The study is devoted to theoretical analysis of ultrashort electromagnetic pulses (USP) absorption on gold nanospheres. Dependencies of USP energy absorption on nanospheres placed in various matrix are compared. The results of calculation of absorbed energy on gold nanospheres as a function of ultrashort electromagnetic pulse carrier frequency and number of pulse cycles of carrier frequency show strong non-linear dependence of absorbed energy on number of cycles of carrier frequency, but for relatively large number of cycles on USP carrier frequency it goes to linear dependence.

Keywords: ultrashort electromagnetic pulses, absorption, nanospheres, theoretical research

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Authors: Kholod Hajo

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In this study COMSOL Multiphysics was used to design lateral flow biosensors (LFBs) which provide advantages in low cost, simplicity, rapidity, stability and portability thus making LFBs popular in biomedical, agriculture, food and environmental sciences. This study was focused on simulation model of biosensor based on gold nanoparticles (GNPs) designed using software package (COMSOL Multiphysics), the magnitude of the laminar velocity field in the flow cell, concentration distribution in the analyte stream and surface coverage of adsorbed species and average fractional surface coverage of adsorbed analyte were discussed from the model and couples of suggestion was given in order to functionalize GNPs and to increase the accuracy of the biosensor design, all above were obtained acceptable results.

Keywords: model, gold nanoparticles, biosensor, COMSOL Multiphysics

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Authors: Marcin Kruszewski, Barbara Sochanowicz, Sylwia Męczyńska-Wielgosz, Maria Wojewódzka, Lucyna Kapka-Skrzypczak

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Metallic NPs are widely used in a number of applications in industry, science and medicine. Among metallic NPs foreseen to be widely used in medicine are gold nanoparticles (AuNPs) due to their low toxicity, and silver NPs (AgNPs) due to their strong antimicrobial activity. In this study, we compared an effect of AgNPs and gold NPs (AuNPs) on the formation of DNA damage and global DNA methylation and in A2780 and 4T1 cell lines, widely used models of human ovarian carcinoma and murine mammary carcinoma, respectively. The cells were treated with AgNPs coated with citrate (AgNPs(cit) or PEG (AgNPs(PEG), or AuNPs. A global DNA methylation was investigated with ELISA, whereas the formation of DNA damage was investigated by a comet +/- FPG. AgNPs decreased global DNA methylation and increased the formation of DNA lesions in both cell lines. The effect was dependent on the type of NPs used, it's coating, and cell line used. In conclusion, the epigenetic and genotoxic effects of NPs strongly depends on NP nature and cellular context. Epigenetic changes observed upon the action of AgNPs may play a crucial role in NPs-induced changes in protein expression.

Keywords: DNA damage, gold nanoparticles, methylation, silver nanoparticles

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Authors: Agnė Mikalauskaitė, Renata Karpicz, Vitalijus Karabanovas, Arūnas Jagminas

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The use of biocompatible precursors for the synthesis and stabilization of fluorescent gold nanoclusters (NCs) with strong red photoluminescence creates an important link between natural sciences and nanotechnology. Herein, we report the cost-effective synthesis of Au nanoclusters by templating and reduction of chloroauric acid with the cheap amino acid food supplements. This synthesis under the optimized conditions leads to the formation of biocompatible Au NCs having good stability and intense red photoluminescence, peaked at 680 to 705 nm, with a quantum yield (QY) of ≈7% and the average lifetime of up to several µs. The composition and luminescent properties of the obtained NCs were compared with ones formed via well-known bovine serum albumin reduction approach. Our findings implied that synthesized Au NCs tend to accumulate in more tumorigenic breast cancer cells (line MDA-MB-213) and after dialysis can be prospective for bio imagining.

Keywords: gold nanoclusters, proteins, materials chemistry, red-photoluminescence, bioimaging

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Authors: R. Karmouch

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A thin gold metal layer was deposited on the top of silicon oxide films containing embedded Si nanocrystals (Si-nc). The sample was annealed in gas containing nitrogen, and subsequently characterized by photoluminescence. We obtained 3-fold enhancement of photon emission from the Si-nc embedded in silicon dioxide covered with a Gold layer as compared with an uncovered sample. We attribute this enhancement to the increase of the spontaneous emission rate caused by the coupling of the Si-nc emitters with the surface plasmons (SP). The evolution of PL emission with laser irradiated time was also collected from covered samples, and compared to that from uncovered samples. In an uncovered sample, the PL intensity decreases with time, approximately with two decay constants. Although the decrease of the initial PL intensity associated with the increase of sample temperature under CW pumping is still observed in samples covered with a gold layer, this film significantly contributes to reduce the permanent deterioration of the PL intensity. The resistance to degradation of light-emitting silicon nanocrystals can be increased by SP coupling to suppress the permanent deterioration. Controlling the permanent photodeterioration can allow to perform a reliable optical gain measurement.

Keywords: photodeterioration, silicon nanocrystals, ion implantation, photoluminescence, surface plasmons

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Authors: G. Gevorgyan, S. Khudaverdyan, A. Vaseashta

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The Lake Sevan basin is situated in the eastern part of the Republic of Armenia (Gegharquniq marz/district). The heavy metal pollution of the some tributaries of Lake Sevan was investigated. Water sampling was performed in August and December, 2014 from the 4 observation sites: 1) Sotq river upstream (about 600 meters upstream from the Sotq gold mine); 2) Sotq river mouth; 3) Masrik river mouth; 4) Dzknaget river mouth. Heavy metal (V, Fe, Ni, Cu, As, Mo, Pb) concentrations in the water samples were determined by the standard methods using an atomic absorption spectrophotometer. The results of the study showed that heavy metal content mainly increased from the upstream of the Sotq river to the mouth of the Masrik river which may have been conditioned by the influence of gold mining activity as the Masrik and its tributary-Sotq rivers passing through the gold mining area were exposed to heavy metal pollution. The observation sites can be ranked by pollution degree as follows: №3> №2> №1> №4. The highest heavy metal pollution degree was observed in the Masrik river mouth which may have been conditioned by the direct impact of gold mining activity and the pressure of its tributary–the Sotq river which flows through the gold mining area. The lowest heavy metal pollution degree was registered in the Dzknaget river mouth which flowing through rural areas wasn’t subject to significant heavy metal pollution. According to the observation sites of the Sotq and Masrik rivers, high positive correlation was mainly observed between the concentrations of the investigated heavy metals (except nickel) which indicated that all the heavy metals except the nickel had the same anthropogenic pollution source which was the activity of the Sotq gold mine. In general, it is possible to state that the activity of the Sotq gold mine in the Lake Sevan basin caused the heavy metal pollution of the Sotq and Masrik rivers which may have posed environmental hazards. Heavy metals are nondegradable substances, and heavy metal pollution of freshwater systems may pose risks to the environment and human health through accumulation in the tissues of aquatic organisms, water-food chain as well as oral ingestion and dermal contact.

Keywords: Armenia, Lake Sevan basin, gold mining activity, river ecosystems, heavy metal pollution

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Authors: Lucian Mocan, Teodora Mocan, Matea Cristian, Cornel Iancu

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We present method of nanoparticle enhanced laser thermal ablation of Klebsiella pneumoniae infections, using gold nanoparticles combined with a specific growth factor and demonstrate its selective therapeutic efficacy. Ab (antibody solution) bound to GNPs (gold nanoparticles) was administered in vitro and determined the specific delivery of the nano-bioconjugate into the microorganism. The extent of necrosis was considerable following laser therapy, and at the same time, normal cells were not seriously affected. The selective photothermal ablation of the infected tissue was obtained after the selective accumulation of Ab bound to GNPs into bacteria following perfusion. These results may represent a major step in antibiotherapy treatment using nanolocalized thermal ablation by laser heating.

Keywords: gold nanoparticles, Klebsiella pneumoniae, nanoparticle functionalization, laser irradiation, antibody

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Authors: Weerachit Pulsawas, Thirasak Rirksomboon

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Due to its abundance from catalytic reforming and thermal cracking of naphtha, toluene could become more value-added compound if it is converted into xylenes, particularly p-xylene, via toluene methylation. Attractively, toluene methylation with methanol is an alternative route to produce xylenes in the absence of other hydrocarbon by-products for which appropriate catalyst would be utilized. In this study, HZSM-5 catalysts with Si/Al molar ratio of 100 were synthesized via hydrothermal treatment and modified by either chemical liquid deposition using tetraethyl-orthosilicate or dealumination with steam. The modified catalysts were characterized by several techniques and tested for their catalytic activity in a continuous down-flow fixed bed reactor. Various operating conditions including WHSV’s of 5 to 20 h-1, reaction temperatures of 400 to 500 °C, and toluene-to-methanol molar ratios (T/M) of 1 to 4 were investigated for attaining possible highest p-xylene selectivity. As a result, the catalytic activity of parent HZSM-5 with temperature of 400 °C, T/M of 4 and WHSV of 24 h-1 showed 65.36% in p-xylene selectivity and 11.90% in toluene conversion as demonstrated for 4 h on stream.

Keywords: toluene methylaion, HZSM-5, silylation, dealumination

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Authors: Emmanuel Jr. Ballad, Herman Mendoza

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The recovery of fine activated carbon with adsorbed gold in the cyanidation tailings of a small-scale gold plant was investigated due to the high amount of gold present. In the study, collectors that were used are kerosene and diesel. Emulsification of the oils was done to improve its collecting property, thus also the recovery. It was found out that the best hydrophile lypophile balance (HLB) of emulsified diesel and kerosene oil is 13 and 12 respectively. The amount of surfactants (SPAN 20 and TWEEN 20) for the best stability of the emulsified oils was found to be 10% in both kerosene and diesel. Optical microscopy showed that the oil dispersion in the water forms spherical droplets like features. The higher the stability, the smaller the droplets and their number were increasing. The smaller droplets indicate better dispersion of oil in the water. Consequently, it will have a greater chance of oil and activated carbon particle interaction during flotation. Due to the interaction of dispersed oil phase with carbon, the hydrophobicity of the carbon will be improved and will be attached to the bubble. Thus, flotation recovery will be increased. Results showed that the recovery of the fine activated carbon using emulsified diesel or kerosene is three times more effective than using pure diesel or kerosene.

Keywords: emulsified oils, flotation, hydrophile lyophile balance, non-ionic surfactants

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Authors: Ali Zazi, Ouiza Cherifi

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Natural gas currently represents a raw material of choice for the manufacture of a wide range of chemical products via synthesis gas, among the routes of transformation of methane into synthesis gas The reaction of the oxidation of methane by gas vapor 'water. This work focuses on the study of the effect of cerieum on the nickel-based catalyst supported by silica for the methane vapor reforming reaction, with a variation of certain parameters of the reaction. The reaction temperature, the H₂O / CH₄ ratio and the flow rate of the reaction mixture (CH₄-H₂O). Two catalysts were prepared by impregnation of Degussa silica with a solution of nickel nitrates and a solution of cerium nitrates [Ni (NO₃) 2 6H₂O and Ce (NO₃) 3 6H₂O] so as to obtain the 1.5% nickel concentrations. For both catalysts and plus 1% cerium for the second catalyst. These Catalysts have been characterized by physical and chemical analysis techniques: BET technique, Atomic Absorption, IR Spectroscopy, X-ray diffraction. These characterizations indicated that the nitrates had impregnated the silica. And that the NiO and Ce₂O3 phases are present and Ni°(after reaction). The BET surface of the silica decreases without being affected. The catalytic tests carried out on the two catalysts for the steam reforming reactions show that the addition of cerium to the nickel improves the catalytic performances of the nickel. And that these performances also depend on the parameters of the reaction, namely the temperature, the rate of the reaction mixture, and the ratio (H₂O / CH₄).

Keywords: heterogeneous catalysis, steam reforming, Methane, Nickel, Cerium, synthesis gas, hydrogen

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Authors: M. S. Kilic, S. Korkut, B. Hazer

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Newly synthesized Polypropylene-g-Polyethylene glycol polymer was first time used for a compartment-less enzymatic fuel cell. Working electrodes based on Polypropylene-g-Polyethylene glycol were operated as unmediated and mediated system (with ferrocene and gold/cobalt oxide nanoparticles). Glucose oxidase and bilirubin oxidase was selected as anodic and cathodic enzyme, respectively. Glucose was used as fuel in a single-compartment and membrane-less cell. Maximum power density was obtained as 0.65 nW cm-2, 65 nW cm-2, and 23500 nW cm-2 from the unmediated, ferrocene and gold/cobalt oxide modified polymeric film, respectively. Power density was calculated to be ~16000 nW cm-2 for undiluted wastewater sample with gold/cobalt oxide nanoparticles including system.

Keywords: bilirubin oxidase, enzymatic fuel cell, glucose oxidase, nanoparticles

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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: Seong Woon Lee, Soo Min Lim, Sung Sik Jeong, Jung Hoon Park

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The atmospheric concentration of greenhouse gas (GHG, Green House Gas) is increasing continuously as a result of the combustion of fossil fuels and industrial development. In response to this trend, many researches have been conducted on the reduction of GHG. Landfill gas (LFG, Land Fill Gas) is one of largest sources of GHG emissions containing the methane (CH₄) as a major constituent and can be considered renewable energy sources as well. In order to use LFG by connecting to the city pipe network, it required a process for removing impurities. In particular, oxygen must be removed because it can cause corrosion of pipes and engines. In this study, methane oxidation was used to eliminate oxygen from LFG and perovskite-type ceramic catalysts of La-Sr-Co-Fe-O composition was selected as a catalyst. Hollow fiber catalysts (HFC, Hollow Fiber Catalysts) have attracted attention as a new concept alternative because they have high specific surface area and mechanical strength compared to other types of catalysts. HFC was prepared by a phase-inversion/sintering technique using commercial La-Sr-Co-Fe-O powder. In order to measure the catalysts' activity, simulated LFG was used for feed gas and complete oxidation reaction of methane was confirmed. Pore structure of the HFC was confirmed by SEM image and perovskite structure of single phase was analyzed by XRD. In addition, TPR analysis was performed to verify the oxygen adsorption mechanism of the HFC. Acknowledgement—The project is supported by the ‘Global Top Environment R&D Program’ in the ‘R&D Center for reduction of Non-CO₂ Greenhouse gases’ (Development and demonstration of oxygen removal technology of landfill gas) funded by Korea Ministry of Environment (ME).

Keywords: complete oxidation, greenhouse gas, hollow fiber catalyst, land fill gas, oxygen removal, perovskite catalyst

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Authors: Jianwen Li, Hongfang Ma, Haitao Zhang, Qiwen Sun, Weiyong Ying

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Catalytic cracking of butene to propylene was carried out in a continuous-flow fixed-bed reactor over HZSM-5 catalysts modified by nickel and phosphorus. The structure and acidity of catalysts were measured by N2 adsorption, NH3-TPD and XPS. The results revealed that surface area and strong acid sites both decreased with increasing phosphorus loadings. The increment of phosphorus loadings reduced the butene conversion but enhanced the propylene selectivity and catalyst stability.

Keywords: butene, catalytic cracking, HZSM-5, modification

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Authors: Y. A. Prada, Fanny Guzman, Rafael Cabanzo, John J. Castillo, Enrique Mejia-Ospino

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In this work, we show the important results about of synthesis of photoluminiscents gold nanoclusters using a small peptide as template for biosensing applications. Interestingly, we design one peptide (NBC2854) homologue to conservative domain from 215 250 residue of a galactolectin protein which can recognize the proteophosphoglycans (PPG) from Leishmania. Peptide was synthetized by multiple solid phase synthesis using FMoc group methodology in acid medium. Finally, the peptide was purified by High-Performance Liquid Chromatography using a Vydac C-18 preparative column and the detection was at 215 nm using a Photo Diode Array detector. Molecular mass of this peptide was confirmed by MALDI-TOF and to verify the α-helix structure we use Circular Dichroism. By means of the methodology used we obtained a novel fluorescents gold nanoclusters (AuNC) using NBC2854 as a template. In this work, we described an easy and fast microsonic method for the synthesis of AuNC with ≈ 3.0 nm of hydrodynamic size and photoemission at 630 nm. The presence of cysteine residue in the C-terminal of the peptide allows the formation of Au-S bond which confers stability to Peptide-based gold nanoclusters. Interactions between the peptide and gold nanoclusters were confirmed by X-ray Photoemission and Raman Spectroscopy. Notably, from the ultrafine spectra shown in the MALDI-TOF analysis which containing only 3-7 KDa species was assigned to Au₈-₁₈[NBC2854]₂ clusters. Finally, we evaluated the Peptide-gold nanocluster as an optical biosensor based on fluorescence spectroscopy and the fluorescence signal of PPG (0.1 µg-mL⁻¹ to 1000 µg-mL⁻¹) was amplified at the same wavelength emission (≈ 630 nm). This can suggest that there is a strong interaction between PPG and Pep@AuNC, therefore, the increase of the fluorescence intensity can be related to the association mechanism that take place when the target molecule is sensing by the Pep@AuNC conjugate. Further spectroscopic studies are necessary to evaluate the fluorescence mechanism involve in the sensing of the PPG by the Pep@AuNC. To our best knowledge the fabrication of an optical biosensor based on Pep@AuNC for sensing biomolecules such as Proteophosphoglycans which are secreted in abundance by parasites Leishmania.

Keywords: biosensing, fluorescence, Leishmania, peptide-gold nanoclusters, proteophosphoglycans

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Authors: Francisco Espinosa, Juan Chavarría

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Glycerol is a byproduct of biodiesel production that can be used for aqueous-phase reforming to obtain hydrogen. Iridium is a material that has high activity and hydrogen selectivity for steam phase reforming. Nevertheless, a drawback for the use of iridium in aqueous-phase reforming is the low activity in water-gas shift reaction. Therefore, in this work, it is proposed the use of nickel and copper as a second metal in the catalyst to reach a synergetic effect. Iridium, iridium-nickel and iridium-copper catalysts were prepared by incipient wetness impregnation and evaluated in the aqueous-phase reforming of glycerol using CeO₂ or La₂O₃ as support. The catalysts were characterized by XRD, XPS, and EDX. The reactions were carried out in a fixed bed reactor feeding a solution of glycerol 10 wt% in water at 270°C, and reaction products were analyzed by gas chromatography. It was found that IrNi/CeO₂ reached highest glycerol conversion and hydrogen production, slightly above 70% and 43 vol% respectively. In terms of conversion, iridium is a promising metal, and its activity for hydrogen production can be enhanced when adding a second metal.

Keywords: aqueous-phase reforming, glycerol, hydrogen production, iridium

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Authors: L. Spitaleri, C. M. A. Gangemi, R. Purrello, G. Nicotra, G. Trusso Sfrazzetto, G. Casella, M. Casarin, A. Gulino

Abstract:

Hybrid molecular–nanoparticle materials, obtained with a bottom-up approach, are suitable for the fabrication of functional nanostructures showing structural control and well-defined properties, i.e., optical, electronic or catalytic properties, in the perspective of applications in different fields of nanotechnology. Gold nanoparticles (Au NPs) exhibit important chemical, electronic and optical properties due to their size, shape and electronic structures. In fact, Au NPs containing no more than 30-40 atoms are only luminescent because they can be considered as large molecules with discrete energy levels, while nano-sized Au NPs only show the surface plasmon resonance. Hence, it appears that gold nanoparticles can alternatively be luminescent or plasmonic, and this represents a severe constraint for their use as an optical material. The aim of this work was the fabrication of nanoscale assembly of Au NPs covalently anchored to each other by means of novel bi-functional porphyrin molecules that work as bridges between different gold nanoparticles. This functional architecture shows a strong surface plasmon due to the Au nanoparticles and a strong luminescence signal coming from porphyrin molecules, thus, behaving like an artificial organized plasmonic and fluorescent network. The self-assembly geometry of this porphyrin on the Au NPs was studied by investigation of the conformational properties of the porphyrin derivative at the DFT level. The morphology, electronic structure and optical properties of the conjugated Au NPs – porphyrin system were investigated by TEM, XPS, UV–vis and Luminescence. The present nanostructures can be used for plasmon-enhanced fluorescence, photocatalysis, nonlinear optics, etc., under atmospheric conditions since our system is not reactive to air nor water and does not need to be stored in a vacuum or inert gas.

Keywords: gold nanoparticle, porphyrin, surface plasmon resonance, luminescence, nanostructures

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Authors: Dorothea Voß, Tobias Esser, Michael Huber, Jakob Albert

Abstract:

The growing world population and the associated increase in demand for energy and consumer goods, as well as increasing waste production, requires the development of sustainable processes. In addition, the increasing environmental awareness of our society is a driving force for the requirement that processes must be as resource and energy efficient as possible. In this context, the use of polyoxometalate catalysts (POMs) has emerged as a promising approach for the development of green processes. POMs are bifunctional polynuclear metal-oxo-anion cluster characterized by a strong Brønsted acidity, a high proton mobility combined with fast multi-electron transfer and tunable redox potential. In addition, POMs are soluble in many commonly known solvents and exhibit resistance to hydrolytic and oxidative degradation. Due to their structure and excellent physicochemical properties, POMs are efficient acid and oxidation catalysts that have attracted much attention in recent years. Oxidation processes with molecular oxygen are worth mentioning here. However, the fact that the POM catalysts are homogeneous poses a challenge for downstream processing of product solutions and recycling of the catalysts. In this regard, nanofiltration membranes have gained increasing interest in recent years, particularly due to their relative sustainability advantage over other technologies and their unique properties such as increased selectivity towards multivalent ions. In order to establish an efficient downstream process for the highly selective separation of homogeneous POM catalysts from aqueous solutions using nanofiltration membranes, a laboratory-scale membrane system was designed and constructed. By varying various process parameters, a sensitivity analysis was performed on a model system to develop an optimized method for the recovery of POM catalysts. From this, process-relevant key figures such as the rejection of various system components were derived. These results form the basis for further experiments on other systems to test the transferability to serval separation tasks with different POMs and products, as well as for recycling experiments of the catalysts in processes on laboratory scale.

Keywords: downstream processing, nanofiltration, polyoxometalates, homogeneous catalysis, green chemistry

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Authors: Joudia Akil, Stephane Siffert, Laurence Pirault-Roy, Renaud Cousin, Christophe Poupin

Abstract:

Oxyfuel combustion is a promising method that enables to obtain a CO2 rich stream, with water vapor ( ̴10%), unburned components such as CO and NO, which must be cleaned before the use of CO2. Our objective is then the final treatment of CO and NO by catalysis. Three-way catalysts are well-developed material for simultaneous conversion of NO, CO and hydrocarbons. Pt and/or Rh ensure a quasi-complete removal of NOx, CO and HC and there is also a growing interest in partly replacing Pt with less-expensive Pd. The use of alumina and ceria as support ensures, respectively, the stabilization of such species in active state and discharging or storing oxygen to control the oxidation of CO and HC and the reduction of NOx. In this work, we will compare different metals (Pd, Rh and Pt) supported on Al2O3 and CeO2, for CO2 purification from oxyfuel combustion. The catalyst must reduce NO by CO in an oxidizing environment, in the presence of CO2 rich stream and resistant to water. In this study, Al2O3 and CeO2 were used as support materials of the catalysts. 1wt% M/Support where M = Pd, Rh or Pt catalysts were obtained by wet impregnation on supports with a precursor of palladium [Pd(acac)2], rhodium [Rh(NO3)3] and platinum [Pt(NO2)2(NO3)2]. Materials were characterized by BET surface area, H2 chemisorption, and TEM. Catalytic activity was evaluated in CO2 purification which is carried out in a fixed-bed flow reactor containing 150 mg of catalyst at atmospheric pressure. The flow of the reactant gases is composed of: 20% CO2, 10% O2, 0.5% CO, 0.02% NO and 8.2% H2O (He as eluent gas) with a total flow of 200 mL.min−1, with same GHSV (2.24x104 h-1). The catalytic performances of the samples were investigated with and without water. It shows that the total oxidation of CO occurred over the different materials. This study evidenced an important effect of the nature of the metals, supports and the presence or absence of H2O during the reduction of NO by CO in oxyfuel combustions conditions. Rh based catalysts show that the addition of water has a very positive influence especially on the Rh catalyst on CeO2. Pt based catalysts keep a good activity despite the addition of water on the both supports studied. For the NO reduction, addition of water act as a poison with Pd catalysts. The interesting results of Rh based catalysts with water can be explained by a production of hydrogen through the water gas shift reaction. The produced hydrogen acts as a more effective reductant than CO for NO removal. Furthermore, in TWCs, Rh is the main component responsible for NOx reduction due to its especially high activity for NO dissociation. Moreover, cerium oxide is a promotor for WGSR.

Keywords: carbon dioxide, environmental chemistry, heterogeneous catalysis

Procedia PDF Downloads 158

Authors: Zahra Asgar Pour

Abstract:

Two types of Ti-Al-containing zeolitic beads with an average diameter of 450 to 750 µm and hierarchical porosity were synthesized using a hard template method and tested as heterogeneous catalysts in the epoxidation of cycloalkenes (i.e. cyclohexene and cis-cyclooctene) with aqueous hydrogen peroxide (H₂O₂) or tert-butyl hydroperoxide(TBHP) as the oxidant agent. The first type of zeolitic beads was prepared by hydrothermal treatment of a primarygel (containing the Si, Ti, and Al precursors) in the presence of porous anion-exchange resin beads as the hard shaping template. After calcination, these beads (Ti-Al-Beta-HDT-B) consisted of both crystalline zeolite Beta and an amorphous silicate phase. The second type of zeolitic beads (Ti-Beta-PS-deAl-14.4-B) was obtained by post-synthesis dealumination of Al-containing zeolite Beta beads using 14.4 M HNO₃, followed by Ti grafting (3 wt% per gram of zeolite). The prepared materials were characterised by means of XRD, N2-physisorption, UV-vis, XRF, SEM, and TEM and tested as heterogeneous epoxidation catalysts. This post-synthetically prepared catalyst demonstrated higher activity (cyclohexene conversion of 22.7 % and epoxide selectivity of 33.5 %) after 5 h at60 °C, which emanates from the crystalline structure and higher degrees of hydrophobicity. In addition, the post-synthetically prepared beads were prone to partial Ti leaching in the presence of H₂O₂, whereas they showed to be resistant against Ti leaching using tert-butyl hydroperoxide as the oxidant agent.

Keywords: epoxidation, structured catalysts, hierarchical porosity, bead-shape catalysts

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Authors: Mingchuan Zhou, Haitao Zhang, Hongfang Ma, Weiyong Ying

Abstract:

Alumina supported PtSn catalysts with cylindrical particles were prepared and characterized by using low temperature N2 adsorption/desorption and X-ray diffraction. Low temperature N2 adsorption/desorption demonstrate that the tableting changed the texture properties of catalysts. XRD pattern indicate that the crystal structure of supports had no change after reaction. The performances over particles of PtSn/Al2O3 catalysts were investigated with regards to reaction temperature, pressure, and H2/AcOH mole ratio. After tableting, the conversion of acetic acid and selectivity of ethanol and acetyl acetate decreased. High reaction temperature and pressure can improve conversion of acetic acid. H2/AcOH mole ratio of 9.36 showed the best performance on acetic acid hydrogenation. High pressure had benefits for the selectivity of ethanol and other two parameters had no obvious effect on selectivity.  

Keywords: acetic acid hydrogenation, cylindrical particles, ethanol, PtSn

Procedia PDF Downloads 291