Search results for: catalytic oxidation

Authors: Ali Zaker, Zhi Chen

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Due to the concerns about the depletion of fossil fuel sources and the deteriorating environment, the attempt to investigate the production of renewable energy will play a crucial role as a potential to alleviate the dependency on mineral fuels. One particular area of interest is the generation of bio-oil through sewage sludge (SS) pyrolysis. SS can be a potential candidate in contrast to other types of biomasses due to its availability and low cost. However, the presence of high molecular weight hydrocarbons and oxygenated compounds in the SS bio-oil hinders some of its fuel applications. In this context, catalytic pyrolysis is another attainable route to upgrade bio-oil quality. Among different catalysts (i.e., zeolites) studied for SS pyrolysis, activated chars (AC) are eco-friendly alternatives. The beneficial features of AC derived from SS comprise the comparatively large surface area, porosity, enriched surface functional groups, and presence of a high amount of metal species that can improve the catalytic activity. Hence, a sludge-based AC catalyst was fabricated in a single-step pyrolysis reaction with NaOH as the activation agent and was compared with HZSM5 zeolite in this study. The thermal decomposition and kinetics were invested via thermogravimetric analysis (TGA) for guidance and control of pyrolysis and catalytic pyrolysis and the design of the pyrolysis setup. The results indicated that the pyrolysis and catalytic pyrolysis contains four obvious stages, and the main decomposition reaction occurred in the range of 200-600°C. The Coats-Redfern method was applied in the 2nd and 3rd devolatilization stages to estimate the reaction order and activation energy (E) from the mass loss data. The average activation energy (Em) values for the reaction orders n = 1, 2, and 3 were in the range of 6.67-20.37 kJ for SS; 1.51-6.87 kJ for HZSM5; and 2.29-9.17 kJ for AC, respectively. According to the results, AC and HZSM5 both were able to improve the reaction rate of SS pyrolysis by abridging the Em value. Moreover, to generate and examine the effect of the catalysts on the quality of bio-oil, a fixed-bed pyrolysis system was designed and implemented. The composition analysis of the produced bio-oil was carried out via gas chromatography/mass spectrometry (GC/MS). The selected SS to catalyst ratios were 1:1, 2:1, and 4:1. The optimum ratio in terms of cracking the long-chain hydrocarbons and removing oxygen-containing compounds was 1:1 for both catalysts. The upgraded bio-oils with AC and HZSM5 were in the total range of C4-C17, with around 72% in the range of C4-C9. The bio-oil from pyrolysis of SS contained 49.27% oxygenated compounds, while with the presence of AC and HZSM5 dropped to 13.02% and 7.3%, respectively. Meanwhile, the generation of benzene, toluene, and xylene (BTX) compounds was significantly improved in the catalytic process. Furthermore, the fabricated AC catalyst was characterized by BET, SEM-EDX, FT-IR, and TGA techniques. Overall, this research demonstrated AC is an efficient catalyst in the pyrolysis of SS and can be used as a cost-competitive catalyst in contrast to HZSM5.

Keywords: catalytic pyrolysis, sewage sludge, activated char, HZSM5, bio-oil

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Authors: Mulatu Kassie Birhanu

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Electrochemical reduction of CO₂ is an emerging and current issue for its conversion in to valuable product upon minimization of its atmospheric level for contribution of maintaining within the range of permissible limit. Among plenty of electro-catalysts gold and copper are efficient and effective catalysts, which are synthesized and applicable for this research work. The two metal catalysts were prepared in inert environment with different compositions through co-reduction process from their corresponding precursors and then by adding multi-walled carbon nano-tube as a supporter and enhanced the conductivity. The catalytic performance of CO₂ reduction for each composition was performed and resulted an outstanding catalytic activity with generation of high current density (70 mA/cm² at 0.91V vs. RHE) and relatively small onset potential. The catalytic performance, compositions, morphologies, structure and geometric arrangements were evaluated by electrochemical analysis (LSV, impedance, chronoamperometry & tafel plot), EDS, SEM and XAS respectively. The composite metals showed better selectivity of products and faradaic efficiencies due to the synergetic effects of the combined nano-particles in addition to the impact of grain size in reduction of CO₂. Carbon monoxide, hydrogen, formate and ethanol are the reduction products, which are detected and quantifiable by chromatographic techniques considering their physical state of each product.

Keywords: carbondioxide, faradaic efficiency, electrocatalyst, current density

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Authors: Siyang Wang, Yujin Hu, Xuelin Wang, Wenqian Zhang

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Austenitic stainless steels are widely used in nuclear industry to manufacture critical components owing to their excellent corrosion resistance at high temperatures. Almost all the components used in nuclear power plants are produced by surface finishing (surface cold work) such as milling, grinding and so on. The change of surface states induced by machining has great influence on the corrosion behavior. In the present study, long time oxidation behavior of machined 316 austenitic stainless steel exposed to simulated pressure water reactor environment was investigated considering different surface states. Four surface finishes were produced by electro-polishing (P), grinding (G), and two milling (M and M1) processes respectively. Before oxidation, the surface Vickers micro-hardness, surface roughness of each type of sample was measured. Corrosion behavior of four types of sample was studied by using oxidation weight gain method for six oxidation periods. The oxidation time of each period was 120h, 216h, 336h, 504h, 672h and 1344h, respectively. SEM was used to observe the surface morphology of oxide film in several period. The results showed that oxide film on austenitic stainless steel has a duplex-layer structure. The inner oxide film is continuous and compact, while the outer layer is composed of oxide particles. The oxide particle consisted of large particles (nearly micron size) and small particles (dozens of nanometers to a few hundred nanometers). The formation of oxide particle could be significantly affected by the machined surface states. The large particle on cold worked samples (grinding and milling) appeared earlier than electro-polished one, and the milled sample has the largest particle size followed by ground one and electro-polished one. For machined samples, the large particles were almost distributed along the direction of machining marks. Severe exfoliation was observed on one milled surface (M) which had the most heavily cold worked layer, while rare local exfoliation occurred on the ground sample (G) and the other milled sample (M1). The electro-polished sample (P) entirely did not exfoliate.

Keywords: austenitic stainless steel, oxidation, machining, SEM

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Authors: Ali Bahri Lubis

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The study of dioxygenase enzymatic mechanism on tryptophan oxidation has been a wide interest since the reaction is rate-limiting step of kynurenine pathway. In this research, observation of tryptophan oxidation through h-IDO enzyme along with synthesis of enzyme products was conducted in order to comprehend how the enzyme works on distinct substrates. UV-vis spectrophotometry, LC-MS, H-NMR and HSQC measurement were carried out to characterise enzyme product. It is found that while tryptophan was oxidised to form Nformylkynurenine (NFK) as a major product and hydroxypyrroloindole amine carboxylic acid (HPIC) in cis and trans confirmed in HSQC, N-methyl tryptophan substrate was converted to NFK and trans HPIC only. Other intriguing results showed that 5-hydroxy- tryptophan and Stryptophan was degraded to become NFK and epoxide cyclic respectively. The formation of NFK was considered through dioxygenation pathway, however HPIC was formed via monooxygenation. The epoxide cyclic—considered as intermediate compound in the mechanism— from S-tryptophan was not able to cleave the epoxide ring since bond energy of epoxide was probably much stronger. This validates the enzymatic mechanism where the intermediate compound in the enzymatic mechanism is epoxide cyclic.

Keywords: tryptophan oxidation, heme-dioxygenases, N-formylkynurenine, hydroxypyrrroloindoleamine, monooxidation

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Authors: Kuan Lun Pan, Moo Been Chang

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Volatile organic compounds (VOCs) are one of major air contaminants, and they can react with nitrogen oxides (NOx) in atmosphere to form ozone (O3) and peroxyacetyl nitrate (PAN) with solar irradiation, leading to environmental hazards. In addition, some VOCs are toxic at low concentration levels and cause adverse effects on human health. How to effectively reduce VOCs emission has become an important issue. Thermal catalysis is regarded as an effective way for VOCs removal because it provides oxidation route to successfully convert VOCs into carbon dioxide (CO2) and water (H2O(g)). Single perovskite-type catalysts are promising for VOC removal, and they are of good potential to replace noble metals due to good activity and high thermal stability. Single perovskites can be generally described as ABO3 or A2BO4, where A-site is often a rare earth element or an alkaline. Typically, the B-site is transition metal cation (Fe, Cu, Ni, Co, or Mn). Catalytic properties of perovskites mainly rely on nature, oxidation states and arrangement of B-site cation. Interestingly, single perovskites could be further synthesized to form double perovskite-type catalysts which can simply be represented by A2B’B”O6. Likewise, A-site stands for an alkaline metal or rare earth element, and the B′ and B′′ are transition metals. Double perovskites possess unique surface properties. In structure, three-dimensional of B-site with ordered arrangement of B’O6 and B”O6 is presented alternately, and they corner-share octahedral along three directions of the crystal lattice, while cations of A-site position between the void of octahedral. It has attracted considerable attention due to specific arrangement of alternating B-site structure. Therefore, double perovskites may have more variations than single perovskites, and this greater variation may promote catalytic performance. It is expected that activity of double perovskites is higher than that of single perovskites toward VOC removal. In this study, double perovskite-type catalyst (La2CoMnO6) is prepared and evaluated for VOC removal. Also, single perovskites including LaCoO3 and LaMnO3 are tested for the comparison purpose. Toluene (C7H8) is one of the important VOCs which are commonly applied in chemical processes. In addition to its wide application, C7H8 has high toxicity at a low concentration. Therefore, C7H8 is selected as the target compound in this study. Experimental results indicate that double perovskite (La2CoMnO6) has better activity if compared with single perovskites. Especially, C7H8 can be completely oxidized to CO2 at 300oC as La2CoMnO6 is applied. Characterization of catalysts indicates that double perovskite has unique surface properties and is of higher amounts of lattice oxygen, leading to higher activity. For durability test, La2CoMnO6 maintains high C7H8 removal efficiency of 100% at 300oC and 30,000 h-1, and it also shows good resistance to CO2 (5%) and H2O(g) (5%) of gas streams tested. For various VOCs including isopropyl alcohol (C3H8O), ethanal (C2H4O), and ethylene (C2H4) tested, as high as 100% efficiency could be achieved with double perovskite-type catalyst operated at 300℃, indicating that double perovskites are promising catalysts for VOCs removal, and possible mechanisms will be elucidated in this paper.

Keywords: volatile organic compounds, Toluene (C7H8), double perovskite-type catalyst, catalysis

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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: Sonya Barzgar, J. Patrick, A. Hettiaratchi

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Methane (CH4) is reputed as the second largest contributor to greenhouse effect with a global warming potential (GWP) of 34 related to carbon dioxide (CO2) over the 100-year horizon, so there is a growing interest in reducing the emissions of this gas. Methane biofiltration (MBF) is a cost effective technology for reducing low volume point source emissions of methane. In this technique, microbial oxidation of methane is carried out by methane-oxidizing bacteria (methanotrophs) which use methane as carbon and energy source. MBF uses a granular medium, such as soil or compost, to support the growth of methanotrophic bacteria responsible for converting methane to carbon dioxide (CO₂) and water (H₂O). Even though the biofiltration technique has been shown to be an efficient, practical and viable technology, the design and operational parameters, as well as the relevant microbial processes have not been investigated in depth. In particular, limited research has been done on the effects of sulphur on methane bio-oxidation. Since bacteria require a variety of nutrients for growth, to improve the performance of methane biofiltration, it is important to establish the input quantities of nutrients to be provided to the biofilter to ensure that nutrients are available to sustain the process. The study described in this paper was conducted with the aim of determining the influence of sulphur on methane elimination in a biofilter. In this study, a set of experimental measurements has been carried out to explore how the conversion of elemental sulphur could affect methane oxidation in terms of methanotrophs growth and system pH. Batch experiments with different concentrations of sulphur were performed while keeping the other parameters i.e. moisture content, methane concentration, oxygen level and also compost at their optimum level. The study revealed the tolerable limit of sulphur without any interference to the methane oxidation as well as the particular sulphur concentration leading to the greatest methane elimination capacity. Due to the sulphur oxidation, pH varies in a transient way which affects the microbial growth behavior. All methanotrophs are incapable of growth at pH values below 5.0 and thus apparently are unable to oxidize methane. Herein, the certain pH for the optimal growth of methanotrophic bacteria is obtained. Finally, monitoring methane concentration over time in the presence of sulphur is also presented for laboratory scale biofilters.

Keywords: global warming, methane biofiltration (MBF), methane oxidation, methanotrophs, pH, sulphur

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Authors: Feny Mentang, Roike Iwan Montolalu, Henny Adeleida Dien, Kristhina P. Rahael, Tomy Moga, Ayub Meko, Siegfried Berhimpon

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Smoked fish is one of the famous fish products in North Sulawesi, Indonesia. Research in producing smoked fish using smoke liquid, and the use of that product as main taste for a new “natural condiment” have been done, including a series of researches to find materials for sachet. Research aims are to determine the effectiveness of smoked edible sachets, in preventing oxidation of natural condiment, stored in ambient temperature. Two kinds of natural condiment flavors were used, i.e. smoked Skipjack flavor, and Sea Food flavor. Three variables of edible sachets were used for the natural condiments, i.e. non-sachet, edible sachet without smoke liquid, and edible sachet with smoke liquid. The natural condiments were then stored in ambient temperature, for 0, 10, 20, and 30 days. To determine the effectiveness of edible sachets in preventing oxidation, analysis of TBA, water content, and pH were conducted. The results shown that natural condiment with smoked seafood taste had TBA values higher than that of smoked Skipjack. Edible sachet gave a highly significant effect (P > 0.01) on TBA. Natural condiment in smoked edible sachet has a lower TBA than natural condiment non-sachet, and with sachet without smoke liquid. The longer storing time, the higher TBA, especially for non-sachet and with sachet without smoke liquid. There were no significant effect (P > 0.05) of edible sachet on water content and pH.

Keywords: edible sachet, smoke liquid, natural condiment, oxidation

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Authors: Saeed Ghali, Azza Ahmed, Taha Mattar

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Solid Oxide Fuel Cell (SOFC) is a promising solution for the energy resources leakage. Ferritic stainless steel becomes a suitable candidate for the SOFCs interconnects due to the recent advancements. Different steel alloys were designed to satisfy the needed characteristics in SOFCs interconnect as conductivity, thermal expansion and corrosion resistance. Refractory elements were used as alloying elements to satisfy the needed properties. The oxidation behaviour of the developed alloys was studied where the samples were heated for long time period at the maximum operating temperature to simulate the real working conditions. The formed scale and oxidized surface were investigated by SEM. Microstructure examination was carried out for some selected steel grades. The effect of alloying elements on the behaviour of the proposed interconnects material and the performance during the working conditions of the cells are explored and discussed. Refractory metals alloying of chromium steel seems to satisfy the needed characteristics in metallic interconnects.

Keywords: SOFCs, Cr-steel, interconnects, oxidation

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Authors: F. Javier Benitez, Francisco J. Real, Juan Luis Acero, Francisco Casas

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Three emerging contaminants (amitriptyline hydrochloride, methyl salicylate and 2-phenoxyethanol) frequently found in waste-waters were selected to be individually degraded in ultra-pure water by the combined advanced oxidation process constituted by UV radiation and chlorine. The influence of pH, initial chlorine concentration and nature of the contaminants was firstly explored. The trend for the reactivity of the selected compounds was deduced: amitriptyline hydrochloride > methyl salicylate > 2-phenoxyethanol. A later kinetic study was carried out and focused on the specific evaluation of the first-order rate constants and the determination of the partial contribution to the global reaction of the direct photochemical pathway and the radical pathway. A comparison between the rate constant values among photochemical experiments without and with the presence of Cl₂ reveals a clear increase in the oxidation efficiency of the combined process with respect to the photochemical reaction alone. In a second stage, the simultaneous oxidation of mixtures of the selected contaminants in several types of water (ultrapure water, surface water from a reservoir, and two secondary effluents) was also performed by the same combination UV/Cl₂ under more realistic operating conditions. The efficiency of this combined system UV/Cl₂ was compared to other oxidants such as the UV/S₂O₈^2- and UV/H₂O₂ AOPs. Results confirmed that the UV/Cl₂ system provides higher elimination efficiencies among the AOPs tested.

Keywords: emerging contaminants, UV/chlorine advanced oxidation process, amitriptyline, methyl salicylate, 2-phenoxyethanol, chlorination, photolysis

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Authors: Sajid Maqsood, Aysha Al Rashedi, Aisha Abushelaibi, Kusaimah Manheem

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Impact of different natural antioxidants on lipid oxidation, microbial load and sensorial quality in ground camel meat (leg region) during 9 days of refrigerated storage were investigated. Control camel meat showed higher lipid oxidation products (Peroxide value and Thiobarbituric acid reactive substances (TBARS)) during the storage period. Upon addition of different natural antioxidants PV and TBARS were retarded, especially in samples added with tannic acid (TA), catechin (CT) and gallic acid (GA) (p<0.05). Haem iron content decreased with increasing storage period and was found to be lower in samples added with caffeic acid (CA) and gallic acid (GA) at the end of storage period (p<0.05). Furthermore, lower mesophilic bacterial count (MBC) and psychrophilic bacterial counts (PBC) were observed in TA and CT treated samples compared to control and other samples (p<0.05). Camel meat treated with TA and CT also received higher likeness scores for colour, odor and overall appearance compared to control samples (p<0.05). Therefore, adding different natural antioxidants especially TA and CT showed retarding effect on lipid oxidation and microbial growth and were also effective in maintaining sensory attributes (color and odor) of ground camel meat during storage at 4°C. Hence, TA and CT could be considered as the potential natural antioxidant for preserving the quality of the camel meat displayed at refrigerated shelves.

Keywords: natural antioxidants, lipid oxidation, quality, camel meat

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Authors: Prathap S. Raghavendra, Mohamed S. Z. Shamshuddin, Thimmaraju N. Venkatesh

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The transesterification of dimethyl malonate (DMM) with phenol has been studied in vapour phase over cordierite honeycomb coated with solid acid catalysts such as ZrO2,Mo(VI)/ZrO2 and SO42-/ZrO2. The catalytic materials were prepared honeycomb coated and powder forms and characterized for their total surface acidity by NH3-TPD and crystalinity by powder XRD methods. Phenyl methyl malonate (PMM) and diphenyl malonate (DPM) were obtained as the reaction products. A good conversion of DMM (up to 82%) of MPM with 95% selectivity was observed when the reactions were carried out at a catalyst bed temperature of 200 °C and flow-rate of 10 mL/h in presence of Mo(VI)/ZrO2 as catalyst. But over SO42-/ZrO2 catalyst, the yield of DPM was found to be higher. The results have been interpreted based on the variation of acidic properties and powder XRD phases of zirconia on incorporation of Mo(VI) or SO42– ions. Transesterification reactions were also carried out over powder forms of the catalytic materials and the yield of the desired phenyl ester products were compared with that of the HC coated catalytic materials. The solid acids were found to be reusable when used for at least 5 reaction cycles.

Keywords: cordierite honeycomb, methyl phenyl malonate, vapour phase transesterification, zirconia

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Authors: Sahana Selladurai, Christine DeWolf

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Lung surfactant comprises a lipid-protein film that coats the alveolar surface and serves to prevent alveolar collapse upon repeated breathing cycles. Exposure of lung surfactant to high concentrations of airborne pollutants, for example tropospheric ozone in smog, can chemically modify the lipid and protein components. These chemical changes can impact the film functionality by decreasing the film’s collapse pressure (minimum surface tension attainable), altering it is mechanical and flow properties and modifying lipid reservoir formation essential for re-spreading of the film during the inhalation process. In this study, we use Langmuir monolayers spread at the air-water interface as model membranes where the compression and expansion of the film mimics the breathing cycle. The impact of ozone exposure on model lung surfactant films is measured using a Langmuir film balance, Brewster angle microscopy and a pendant drop tensiometer as a function of film and sub-phase composition. The oxidized films are analyzed using mass spectrometry where lipid and protein oxidation products are observed. Oxidation is shown to reduce surface activity, alter line tension (and film morphology) and in some cases visibly reduce the viscoelastic properties of the film when compared to controls. These reductions in functionality of the films are highly dependent on film and sub-phase composition, where for example, the effect of oxidation is more pronounced when using a physiologically relevant buffer as opposed to water as the sub-phase. These findings can lead to a better understanding on the impact of continuous exposure to high levels of ozone on the mechanical process of breathing, as well as understanding the roles of certain lung surfactant components in this process.

Keywords: lung surfactant, oxidation, ozone, viscoelasticity

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Authors: Sewon Kim, Changyeop Lee

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A noble low NOx combustion technology, based on partial oxidation combustion concept in a fuel rich combustion zone, is successfully applied in this research. The burner is designed such that a portion of fuel is heated and pre-vaporized in the furnace then injected into a fuel rich combustion zone so that a partial oxidation reaction occurs. The effects of equivalence ratio, thermal load, and fuel distribution ratio on the emissions of NOx and CO are experimentally investigated. This newly developed combustion technology is successfully applied to industrial furnace, and showed extremely low NOx emission levels.

Keywords: low NOx, combustion, burner, fuel rich

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Authors: Davyd Urbanas, Pranas Baltrenas

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It is well-known that, despite the constant increase of alternative energy sources usage, today combustible fuels are still widely used in power engineering. As a result of fuel combustion, significant amounts of nitrogen oxides (NOx) and carbon monoxide (CO is a product of incomplete combustion) are supplied to the atmosphere. Also, these pollutants are formed in industry (chemical production, refining, and metal production). In this work, the investigation of nitrogen oxides CO-selective catalytic reduction using new grain load-type catalysts was carried out. The catalysts containing the substrate and a thin active coating made of transition metal (Mn, Cu, and Nb) oxides were prepared with the use of electroless chemical deposition method. Chemical composition, chemical state, and morphology of the formed active coating were investigated using ICP-OES, EDX, SEM, and XPS techniques. The obtained results revealed that the prepared catalysts (Cu-Mn-oxide and Cu-Mn-Nb-oxide) have rough and developed surface and can be successfully used for the flue gas catalytic purification. The significant advantage of prepared catalysts is their suitability from technological application point of view, which differs this work from others dedicated to gas purification by SCR.

Keywords: flue gas, nitrogen oxides, selective catalytic reduction, transition metal oxides

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Authors: Anurak Khrueakham, Tassanee Chanphuthin

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Indigo is a well-known natural blue dye that is used hither to even though synthetic ones are commercially available. The removal of indigo from effluents is difficult due to its resistance towards biodegradation which causes an aquatic environment effect. Fenton process is a reaction between hydrogen peroxide H2O2 and Fe2+ to generate •OH (highly reactive oxidant (E◦= 2.8 V)). Additionally, •OH is non-selective oxidant which is capable of destroying wide range of organic pollutants in water and wastewater. The aims of this research were to investigate the effect of H2O2, Fe2+ and pH on indigo wastewater oxidation by Fenton process. A liter reactor was operated in all experiments. The batch reactor was prepared by filling 1 liter of indigo wastewater. The pH was adjusted to the desired value; then, FeSO4 at predetermined amount was added. Finally, H2O2 was immediately added to start the Fenton’s reaction. The Fenton oxidation of indigo wastewater was operated for 60 minutes. Residual H2O2 was analyzed using titanium oxalate method. The Fe2+ concentration was determined by phenanthroline method. COD was determined using closed-reflux titrimetric method to indicate the removal efficiency. The results showed that at pH 2 increasing the initial ferrous concentration from 0.1 mM to 1 mM enhanced the indigo removal from 36% to 59%. Fenton reaction was rapidly due to the high generation rate of •OH. The degradation of indigo increased with increasing pH up to pH 3. This can be explained that the scavenging effect of the •OH by H+ in the condition of low pH is severe to form an oxonium ion, resulting in decrease the production of •OH and lower the decolorization efficiency of indigo. Increasing the initial H2O2 concentration from 5 mM to 20 mM could enhance the decolorization. The COD removal was increased from 35% to 65% with increasing H2O2 concentration from 5 mM to 20 mM. The generations of •OH were promoted by the increase of initial H2O2 concentration. However, the higher concentration of H2O2 resulted in the reduction of COD removal efficiency. The initial ferrous concentrations were studied in the range of 0.05-15.0 mM. The results found that the COD removals increased with increasing ferrous concentrations. The COD removals were increased from 32% to 65% when increase the ferrous concentration from 0.5 mM to 10.0 mM. However, the COD removal did not significantly change at higher 10.0 mM. This is because •OH yielding was lower level of oxidation, therefore, the COD removals were not improved. According to the studies, the Fenton’s reagents were important factors for COD removal by Fenton process. The optimum condition for COD removal of indigo dye wastewater was 10.0 mM of ferrous, 20 mM of H2O2 and at pH 3.

Keywords: indigo dye, fenton oxidation, wastewater treatment, advanced oxidation processes

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Authors: Tae Hyun Ahn, Gyo Woo Lee, Man Young Kim

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Because of high thermal efficiency and low CO2 emission, diesel engines are being used widely in many industrial fields although it makes many PM and NOx which give both human health and environment a negative effect. NOx regulations for diesel engines, however, are being strengthened and it is impossible to meet the emission standard without NOx reduction devices such as SCR (Selective Catalytic Reduction), LNC (Lean NOx Catalyst), and LNT (Lean NOx Trap). Among the NOx reduction devices, urea-SCR system is known as the most stable and efficient method to solve the problem of NOx emission. But this device has some issues associated with the ammonia slip phenomenon which is occurred by shortage of evaporation and thermolysis time, and that makes it difficult to achieve uniform distribution of the injected urea in front of monolith. Therefore, this study has focused on the mixing enhancement between urea and exhaust gases to enhance the efficiency of the SCR catalyst equipped in catalytic muffler by changing inlet gas temperature and spray conditions to improve the spray uniformity of the urea water solution. Finally, it can be found that various parameters such as inlet gas temperature and injector and injection angles significantly affect the evaporation and mixing of the urea water solution with exhaust gases, and therefore, optimization of these parameters are required.

Keywords: UWS (Urea-Water-Solution), selective catalytic reduction (SCR), evaporation, thermolysis, injection

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Authors: Yaxin Tang, Mingao Hou, Qian He, Guangfu Luo

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Bimetallic nanoparticles serve as a promising class of catalysts with tunable properties suitable for diverse catalytic reactions, yet a comprehensive understanding of their actual structures under operating conditions and the optimal design principles remains largely elusive. In this study, we unveil a prevalent surface segregation phenomenon in nearly 100 platinum-group-element-based bimetallic nanoparticles through first principles-based molecular dynamics simulations. Our findings highlight that two components in a nanoparticle with relatively lower surface energy tend to segregate to the surface. Motivated by this discovery, we propose a deliberate exploitation of surface segregation in designing bimetallic nanoparticle catalysts, aiming for heightened stability and reduced consumption of precious metals. To validate this strategy, we further investigate 36 platinum-based bimetallic nanoparticles for propane dehydrogenation catalysis. Through a systematic examination of catalytic sites on nanoparticles, we identify several systems as top candidates with Pt-enriched surfaces, remarkable thermal stability, and superior catalytic activity for propane dehydrogenation. The insights gained garnered from this study are anticipated to provide a valuable framework for the optimal design of other bimetallic nanoparticles.

Keywords: bimetallic nanoparticles, platinum-group element, catalysis, surface segregation, first-principles calculations

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Authors: Ali Noorian

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Crude oil contains various compounds of hydrocarbons but low concentrations of inorganic compounds or metals. Vanadium and Nickel are the most common metals in crude oil. These metals usually exist in solution in the oil and residual fuel oil in the refining process is condensed. Deleterious effects of metals in petroleum have been known for some time. These metals do not only contaminate the product but also cause intoxication and loss of catalyst and corrosion to equipment. In this study, removal of heavy metals and petroleum residues were investigated. These methods include physical, chemical and biological treatment processes. For example, processes such as solvent extraction and hydro-catalytic and catalytic methods are effective and practical methods, but typically often have high costs and cause environmental pollution. Furthermore, biological methods that do not cause environmental pollution have been discussed in recent years, but these methods have not yet been industrialized.

Keywords: removal, metal, heavy oil, nickel, vanadium

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Authors: Annapurna Basavaraju, Andreas Marn, Franz Heitmeir

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The Advisory Council for Aeronautics Research in Europe (ACARE) is cognizant for the overall reduction of NOx emissions by 80% in its vision 2020. Moreover small turbo engines have higher fuel specific emissions compared to large engines due to their limited combustion chamber size. In order to fulfill these requirements, novel combustion concepts are essential. This motivates to carry out the research on the current state of art, catalytic stabilized combustion chamber using hydrogen in small jet engines which are designed and investigated both numerically and experimentally during this project. Catalytic combustion concepts can also be adopted for low caloric fuels and are therefore not constrained to only hydrogen. However, hydrogen has high heating value and has the major advantage of producing only the nitrogen oxides as pollutants during the combustion, thus eliminating the interest on other emissions such as Carbon monoxides etc. In the present work, the combustion chamber is designed based on the ‘Rich catalytic Lean burn’ concept. The experiments are conducted for the characteristic operating range of an existing engine. This engine has been tested successfully at Institute of Thermal Turbomachinery and Machine Dynamics (ITTM), Technical University Graz. One of the facts that the efficient combustion is a result of proper mixing of fuel-air mixture, considerable significance is given to the selection of appropriate mixer. This led to the design of three diverse configurations of mixers and is investigated experimentally and numerically. Subsequently the best mixer would be equipped in the main combustion chamber and used throughout the experimentation. Furthermore, temperatures and pressures would be recorded at various locations inside the combustion chamber and the exhaust emissions will also be analyzed. The instrumented combustion chamber would be inspected at the engine relevant inlet conditions for nine different sets of catalysts at the Hot Flow Test Facility (HFTF) of the institute.

Keywords: catalytic combustion, gas turbine, hydrogen, mixer, NOx emissions

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Authors: Raphaelle Guillou, Matthieu Le Saux, Jean-Christophe Brachet, Thomas Guilbert, Elodie Rouesne, Denis Menut, Caroline Toffolon-Masclet, Dominique Thiaudiere

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In some hypothetical accidental situations, such as during a Loss Of Coolant Accident (LOCA) in pressurized water reactors, fuel cladding tubes made of zirconium alloys can be exposed for a few minutes to steam at High Temperature (HT up to 1200°C) before being cooled and then quenched in water. Under LOCA-like conditions, the cladding undergoes a number of metallurgical changes (phase transformations, oxygen diffusion and growth of an oxide layer...) and is consequently submitted to internal stresses whose state evolves during the transient. These stresses can have an effect on the oxide structure and the oxidation kinetics of the material. They evolve during cooling, owing to differences between the thermal expansion coefficients of the various phases and phase transformations of the metal and the oxide. These stresses may result in the failure of the cladding during quenching, once the material is embrittled by oxidation. In order to progress in the evaluation of these internal stresses, X-ray diffraction experiments were performed in-situ under synchrotron radiation during HT oxidation and subsequent cooling on Zircaloy-4 sheet samples. First, structural evolutions, such as phase transformations, have been studied as a function of temperature for both the oxide layer and the metallic substrate. Then, internal stresses generated within the material oxidized at temperatures between 700 and 900°C have been evaluated thanks to the 2θ diffraction peak position shift measured during the in-situ experiments. Electron backscatter diffraction (EBSD) analysis was performed on the samples after cooling in order to characterize their crystallographic texture. Furthermore, macroscopic strains induced by oxidation in the conditions investigated during the in-situ X-ray diffraction experiments were measured in-situ in a dilatometer.

Keywords: APRP, stains measurements, synchrotron diffraction, zirconium allows

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Authors: Christine Fräulin, Daniela Schurr, Hamed Shahidi Rad, Gerrit Waters, Günter Rinke, Roland Dittmeyer, Michael Nilles

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The reaction mechanisms of many liquid-phase reactions in organic chemistry have not yet been sufficiently clarified. Process conditions of several hundred degrees celsius and pressures to ten megapascals complicate the sampling and the determination of kinetic data. Space resolved in-situ measurements promises new insights. A non-invasive in-situ measurement technique has the advantages that no sample preparation is necessary, there is no change in sample mixture before analysis and the sampling do no lead to interventions in the flow. Thus, the goal of our research was the development of a contact-free spatially resolved measurement technique for kinetic studies of liquid phase reaction under process conditions. Therefore we used laser Raman spectroscopy combined with an optical transparent microchannel reactor. To show the performance of the system we choose the oxidation of cyclohexane as sample reaction. Cyclohexane oxidation is an economically important process. The products are intermediates for caprolactam and adipic acid, which are starting materials for polyamide 6 and 6.6 production. To maintain high selectivities of 70 to 90 %, the reaction is performed in industry at a low conversion of about six percent. As Raman spectroscopy is usually very selective but not very sensitive the detection of the small product concentration in cyclohexane oxidation is quite challenging. To meet these requirements, an optical experimental setup was optimized to determine the concentrations by laser Raman spectroscopy with respect to good detection sensitivity. With this measurement technique space resolved kinetic studies of uncatalysed and homogeneous catalyzed cyclohexane oxidation were carried out to obtain details about the reaction mechanism.

Keywords: in-situ laser raman spectroscopy, space resolved kinetic measurements, homogeneous catalysis, chemistry

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Authors: Nalinee B. Suryawanshi, Vinay M. Bhandari, Laxmi Gayatri Sorokhaibam, Vivek V. Ranade

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Deep desulphurization of transportation fuels is a major environmental concern all over the world and recently prescribed norms for the sulphur content require below 10 ppm sulphur concentrations in fuels such as diesel and gasoline. The existing technologies largely based on catalytic processes such as hydrodesulphurization, oxidation require newer catalysts and demand high cost of deep desulphurization whereas adsorption based processes have limitations due to lower capacity of sulphur removal. The present work is an attempt to provide alternatives for the existing methodologies using a newer non-catalytic process based on hydrodynamic cavitation. The developed process requires appropriate combining of organic and aqueous phases under ambient conditions and passing through a cavitating device such as orifice, venturi or vortex diode. The implosion of vapour cavities formed in the cavitating device generates (in-situ) oxidizing species which react with the sulphur moiety resulting in the removal of sulphur from the organic phase. In this work, orifice was used as a cavitating device and deep desulphurization was demonstrated for removal of thiophene as a model sulphur compound from synthetic fuel of n-octane, toluene and n-octanol. The effect of concentration of sulphur (up to 300 ppm), nature of organic phase and effect of pressure drop (0.5 to 10 bar) was discussed. A very high removal of sulphur content of more than 90% was demonstrated. The process is easy to operate, essentially works at ambient conditions and the ratio of aqueous to organic phase can be easily adjusted to maximise sulphur removal. Experimental studies were also carried out using commercial diesel as a solvent and the results substantiate similar high sulphur removal. A comparison of the two cavitating devices- one with a linear flow and one using vortex flow for effecting pressure drop and cavitation indicates similar trends in terms of sulphur removal behaviour. The developed process is expected to provide an attractive environmental engineering alternative for deep desulphurization of transportation fuels.

Keywords: cavitation, petroleum, separation, sulphur removal

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Authors: Hyun Kyu Lee, Won Zin Oh, June Hyun Kim, Jin Hee Kim, Sang June Choi, Hak Soo Kim

Abstract:

The oxidative dissolution of chromium oxide by manganese oxides including permanganate have been widely studied not only for the chemical decontamination of nuclear power plant, but also for the environmental control of the toxic chromate caused by naturally occurring manganese dioxide. However, little attention has been made for the spontaneous reductive decomposition of permanganate in the water, which is a competing reaction with the oxidation of the chromium oxide by permanganate. The objective of this study is to investigate the spontaneous reductive decomposition behavior of permanganate in the water, depending on the variation of acidity, temperature and concentration. Results of the experiments showed that the permanganate reductive decomposition product is manganese dioxide, and this reaction accompanies with the same molar amount of hydrogen ion consumption. Therefore, at the neutral condition (ex. potassium permanganate solution without acidic chemicals), the permanganate do not reduce by itself at any condition of temperature, concentration within the experimental range. From the results, we confirmed that the oxidation reaction for the permanganate reduction is the water oxidation that is accompanying the oxygen evolution. The experimental results on the reductive decomposition behavior of permanganate in the water also showed that the degree and rate of permanganate reduction increases with the temperature, acidity and concentration. The spontaneous decomposition of the permanganates obtained in the studies would become a good reference to select the operational condition, such as temperature, acidity and concentration, for the chemical decontamination of nuclear power plants.

Keywords: permanganate reduction, spontaneous decomposition, water oxidation, acidity, temperature, permanganate concentration, chemical decontamination, nuclear power plant

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Authors: Kooshan Nayebzadeh, Maryam Enteshari, Abdorreza Mohammadi

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The oxidative stability of mayonnaise under different storage temperatures (4 and 25˚C) during 6-month shelf-life was investigated by different analytical methods. In this study, headspace single-drop microextarction (HS-SDME) combined with gas chromatography-mass spectrometry (GC-MS) as a green, sensitive and rapid technique was applied to evaluate oxidative state in mayonnaise. Oxidation changes of extracted oil from mayonnaise were monitored by analytical parameters including peroxide value (PV), p-Anisidine value (p-An V), thiobarbituric acid value (TBA), and oxidative stability index (OSI). Hexanal and heptanal as secondary volatile oxidation compounds were determined by HS-SDME/GC-MS method in mayonnaise matrix. The rate of oxidation in mayonnaises increased during storage and it was determined greater at 25 ˚C. The values of Anisidine and TBA were gradually enhanced during 6 months, while the amount of OSI decreased. At both temperatures, the content of hexanal was higher than heptanal during all storage periods. Also significant increments in hexanal and heptanal concentrations in the second and sixth month of storage have been observed. Hexanal concentrations in mayonnaises which were stored at 25 ˚C and during storage time showed the highest values. It can be concluded that the temperature and duration of storage time are definitive parameters which affect on quality and oxidative stability of mayonnaise. Additionally, hexanal content in comparison to heptanal is a more reliable oxidative indicator and HS-SDME/GC-MS can be applied in a quick and simple manner.

Keywords: oxidative stability, mayonnaise, headspace single-drop microextarction (HS-SDME), shelf-life

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Authors: Sadia Ameen, M. Nazim, Hyumg-Kee Seo, Hyung-Shik Shin

Abstract:

TiO2 nanotube (NT) arrays were grown on titanium (Ti) foil substrate by electrochemical anodic oxidation and utilized as working electrode to fabricate a highly sensitive and reproducible chemical sensor for the detection of harmful phenyl hydrazine chemical. The fabricated chemical sensor based on TiO2 NT arrays electrode exhibited high sensitivity of ~40.9 µA.mM-1.cm-2 and detection limit of ~0.22 µM with short response time (10s).

Keywords: TiO2 NT, phenyl hydrazine, chemical sensor, sensitivity, electrocatalytic properties

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Authors: Nathalie Elia, Samer Aouad, Jane Estephane, Christophe Poupin, Bilal Nsouli, Edmond Abi Aad

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Carbon dioxide is one of the main contributors to greenhouse effect and hence to climate change. As a result, the methanation reaction CO2(g) + 4H2(g) →CH4(g) + 2H2O (ΔH°298 = -165 kJ/mol), also known as Sabatier reaction, has received great interest as a process for the valorization of the greenhouse gas CO2 into methane which is a hydrogen-carrier gas. The methanation of CO2 is an exothermic reaction favored at low temperature and high pressure. However, this reaction requires a high energy input to activate the very stable CO2 molecule, and exhibits serious kinetic limitations. Consequently, the development of active and stable catalysts is essential to overcome these difficulties. Catalytic methanation of CO2 has been studied using catalysts containing Rh, Pd, Ru, Co and Ni on various supports. Among them, the Ni-based catalysts have been extensively investigated under various conditions for their comparable methanation activity with highly improved cost-efficiency. The addition of promoters are common strategies to increase the performance and stability of Ni catalysts. In this work, a small amount of Ru was used as a promoter for Ni catalysts supported on ceria and tested in the CO2 methanation reaction. The nickel loading was 5 wt. % and ruthenium loading is 0.5wt. %. The catalysts were prepared by successive impregnation method using Ni(NO3)2.6H2O and Ru(NO)(NO3)3 as precursors. The calcined support was impregnated with Ni(NO3)2.6H2O, dried, calcined at 600°C for 4h, and afterward, was impregnated with Ru(NO)(NO3)3. The resulting solid was dried and calcined at 600°C for 4 h. Supported monometallic catalysts were prepared likewise. The prepared solids Ru(0.5%)/CeO2, Ni(5%)/CeO2 and Ru(0.5%)-Ni(5%)/CeO2 were then reduced prior to the catalytic test under a flow of 50% H2/Ar (50 ml/min) for 4h at 500°C. Finally, their catalytic performances were evaluated in the CO2 methanation reaction, in the temperature range of 100–350°C by using a gaseous mixture of CO2 (10%) and H2 (40%) in Ar balanced at a total flow rate of 100 mL/min. The effect of pressure on the CO2 methanation was studied by varying the pressure between 1 and 10 bar. The various catalysts showed negligible CO2 conversion at temperatures lower than 250°C. The conversion of CO2 increases with increasing reaction temperature. The addition of Ru as promoter to Ni/CeO2 improved the CO2 methanation. It was shown that the CO2 conversion increases from 15 to 70% at 350°C and 1 bar. The effect of pressure on CO2 conversion was also studied. Increasing the pressure from 1 to 5 bar increases the CO2 conversion from 70% to 87%, while increasing the pressure from 5 to 10 bar increases the CO2 conversion from 87% to 91%. Ru–Ni catalysts showed excellent catalytic performance in the methanation of carbon dioxide with respect to Ni catalysts. Therefore the addition of Ru onto Ni catalysts improved remarkably the catalytic activity of Ni catalysts. It was also found that the pressure plays an important role in improving the CO2 methanation.

Keywords: CO2, methanation, nickel, ruthenium

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Authors: Abdelmahmod Saad

Abstract:

In this study two amino acids were chosen (DL.alanine,DL.serine) to determine their effect on dissociation of S2O8-2 ino. As the reaction was very slow, Ag+ ino was used as a catalyst. The kinetics measurement showed that the reactions in both cases were found in the first order with respect to S2O8-2, half order with respect to Ag+ and zero order with respect to substrates. Mechanisms were proposed for these reactions according to the determined orders. The energy of activation (AE) was determined for each reaction, and was found to by 30.50 k JmoI-1 in case of DL. Serine and 24.40 k JmoI-1 in case of DL.alanine.

Keywords: mechanism, oxidation, amino acids, peroxodisulphate

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Authors: Fatima Ammari, Meriem Chenouf

Abstract:

Synthesis of gold nano particles has attracted much attention since the pioneering discovery of the high catalytic activity of supported gold nano particles in the reaction of CO oxidation at low temperature. In this research field, we used Na-montmorillonite for gold nanoparticles stabilization; different loading percentage 1, 2 and 5%. The gold nano particles were obtained using chemical reduction method using NaBH4 as reductant agent. The obtained gold nano particles Au-mont stabilized in Na-montmorillonite were used as catalysts for reduction of 4-nitrophenol to aminophenol with sodium borohydride at room temperature. The UV-Vis results confirm directly the gold nano particles formation. The XRD and N2 adsorption results showed the formation of gold nano particles in the pores of montmorillonite with an average size of 5 nm obtained on samples with 2%Au-mont. The gold particles size increased with the increase of gold loading percentage. The reduction reaction of 4-nitrophenol into 4-aminophenol with NaBH4 catalyzed by Au-Na-montmorillonite catalyst exhibits remarkably a high activity; the reaction was completed within 9 min for 1Au-mont and within 3 min for 2Au-mont.

Keywords: chemical reduction, gold, montmorillonite, nano particles, 4-nitrophenol

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Authors: Pelin Yılmaz Çetiner, Metin Mert İlgün, Nazlı Çetindağ, Emine Birci, Gizemnur Yıldız Uysal, Özcan Hatipoğlu, Ehsan Tuzcuoğlu, Gökhan Sır

Abstract:

Water scarcity is an inevitable problem affecting more and more people day by day. It is a worldwide crisis and a consequence of rapid population growth, urbanization and overexploitation. Thus, the solutions providing the reclamation of the wastewater are the desired approach. Wastewater contains various substances such as organic, soaps and detergents, solvents, biological substances, and inorganic substances. The physical properties of the wastewater differs regarding to its origin such as commerical, domestic or hospital usage. Thus, the treatment strategy of this type of wastewater is should be comprehensively investigated and properly treated. The advanced oxidation process comes up as a hopeful method associated with the formation of reactive hydroxyl radicals that are highly reactive to oxidize of organic pollutants. This process has a priority on other methods such as coagulation, flocuation, sedimentation and filtration since it was not cause any undesirable by-products. In the present study, it was aimed to investigate the applicability of advanced oxidation process for the treatment of household appliances wastewater. For this purpose, the laboratory studies providing the effectively addressing of the formed radicals to organic pollutants were carried out. Then the effect of process parameters were comprehensively studied by using response surface methodology, Box-Benhken experimental desing. The final chemical oxygen demand (COD) was the main output to evaluate the optimum point providing the expected COD removal. The linear alkyl benzene sulfonate (LAS), total dissolved solids (TDS) and color were measured for the optimum point providing the expected COD removal. Finally, present study pointed out that advanced oxidation process might be efficiently preffered to treat of the household appliances wastewater and the optimum process parameters provided that expected removal of COD.

Keywords: advanced oxidation process, household appliances wastewater, modelling, water reuse

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