Search results for: catalytic oxidation

Authors: J. Bolobajev, M. Trapido, A. Goi

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The practical application of the Fenton-based treatment method for organic compounds-contaminated water purification is limited mainly because of the large amount of ferric sludge formed during the treatment, where ferrous iron (Fe(II)) is used as the activator of the hydrogen peroxide oxidation processes. Reuse of ferric sludge collected from clarifiers to substitute Fe(II) salts allows reducing the total cost of Fenton-type treatment technologies and minimizing the accumulation of hazardous ferric waste. Dissolution of ferric iron (Fe(III)) from the sludge to liquid phase at acidic pH and autocatalytic transformation of Fe(III) to Fe(II) by phenolic compounds (tannic acid, lignin, phenol, catechol, pyrogallol and hydroquinone) added or present as water/wastewater constituents were found to be essentially involved in the Fenton-based oxidation mechanism. Observed enhanced formation of highly reactive species, hydroxyl radicals, resulted in a substantial organic contaminant degradation increase. Sludge reuse at acidic pH and in the presence of ferric iron reductants is a novel strategy in the Fenton-based treatment application for organic compounds-contaminated water purification.

Keywords: ferric sludge recycling, ferric iron reductant, water treatment, organic pollutant

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Authors: Menouar Hanafi

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The original function of the process of platforming is to develop heavy naphtha (HSRN), coming from the atmospheric unit of distillation with a weak octane number (NO=44), to obtain a mixture of fuels â number octane raised by catalytically supporting specific groups of chemical reactions. The installation is divided into two sections: Section hydrobon. Section platforming. The rafinat coming from the bottom of column 12C2 to feed the section platforming, is divided into two parts whose flows are controlled and mixed with gas rich in hydrogen. Bottom of the column, we obtain stabilized reformat which is aspired by there pump to ensure the heating of the column whereas a part is sent towards storage after being cooled by the air cooler and the condenser. In catalytic catalyst of reforming, there is voluntarily associated a hydrogenating function-dehydrogenating, brought by platinum deposited, with an acid function brought by the alumina support (Al 2 0 3). The mechanism of action of this bifunctional catalyst depends on the severity of the operation, of the quality of the load and the type of catalyst. The catalyst used in the catalytic process of reforming is a very elaborate bifunctional catalyst whose performances are constantly improved thanks to the experimental research supported on an increasingly large comprehension of the phenomena. The American company Universel 0i1 petroleum (UOP) marketed several series of bimetallic catalysts such as R16, R20, R30, and R62 consisted Platinum/Rhenium on an acid support consisted the alumina added with a halogenous compound (chlorine).

Keywords: platforming, amelioration, octane number, catalyst

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Authors: Usha N. Murthy, H. B. Rekha, Mahaveer Devoor

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The introduction of more stringent pollution regulations, in relation to financial and social pressures for sustainable development, has pressed toward limiting the volumes of industrial and domestic effluents discharged into the environment-as well as to increase the efforts within research and development of new or more efficient wastewater treatment technologies. Considering both discharge volume and effluent composition, wastewater generated by the textile industry is rated as the most polluting among all industrial sectors. The pollution load is mainly due to spent dye baths, which are composed of unreacted dyes, dispersing agents, surfactants, salts and organics. In the present investigation, the textile dye wastewater was characterized by high colour, chemical oxygen demand (COD), total dissolved solids (TDS) and pH. Electrochemical oxidation process for four plate electrodes was carried out at five different current intensities, out of which 0.14A has achieved maximum percentage removal of COD with 75% and 83% of colour. The COD removal rate in kg COD/h/m2 decreases with increase in the current intensity. The energy consumption increases with increase in the current intensity. Hence, textile dye wastewater can be effectively pre-treated by electrochemical oxidation method where the process limits objectionable colour while leaving the COD associated with organics left for natural degradation thus causing a sustainable reduction in pollution load.

Keywords: electrochemical treatment, COD, colour, environmental engineering

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Authors: Didem Ildırar, Serap Fındık

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Baker’s yeast industry uses molasses as a raw material. Molasses wastewater contains high molecular weight polymers called melanoidins. Melanoidins are obtained after the reactions between the amino acids and carbonyl groups in molasses. The molasses wastewater has high biochemical and chemical oxygen demand and dark brown color. If it is discharged to receiving bodies without any treatment, it prevents light penetration and dissolved oxygen level of the surface water decreases. Melanoidin compounds are toxic effect to the microorganism in water and there is a resistance to microbial degradation. Before discharging molasses wastewater, adequate treatment is necessary. In addition to changing environmental regulations, properties of treated wastewater must be improved. Advanced oxidation processes can be used to improve existing properties of wastewater. Sonochemical oxidation is one of the alternative methods. Sonochemical oxidation employs the use of ultrasound resulting in cavitation phenomena. In this study, decolorization and chemical oxygen demand removal (COD) of baker’s yeast effluent was investigated by using ultrasound. Baker’s yeast effluent was supplied from a factory which is located in the north of Turkey. An ultrasonic homogenizator was used for this study. Its operating frequency is 20kHz. SnO2/TiO2 catalyst has been used as sonocatalyst. The effects of the composite preparation method, mixing time while composite prepared, the molar ratio of SnO2/TiO2, the calcination temperature, and time, the catalyst amount were investigated on the treatment of baker’s yeast effluent. . According to the results, the prepared composite SnO2/TiO2 by using ultrasonic probe gave a better result than prepared composite by using an ultrasonic bath. Prepared composite by using an ultrasonic probe with a 4:1 molar ratio treated at 800°C for 60min gave a better result. By using this composite, optimum catalyst amount was 0.2g/l. At these conditions 26.6% decolorization was obtained. There was no COD removal at the studied conditions.

Keywords: baker’s yeast effluent, COD, decolorization, sonocatalyst, ultrasonic irradiation

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Authors: Zahid Shafiq, Li Liu, Dong Wang, Yong-Jun Chen

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As synthetic organic methods are increasingly concerned with the growing importance of sustainable chemistry, iodine recently has emerged as an inexpensive, non-toxic, readily available and environmentally benign catalyst for various organic transformations to afford the corresponding products in high yields with high regio- and chemoselectivity. Iodine has found widespread applications in various organic synthesis such as Michael addition, coupling reaction and also in the multicomponent synthesis where it can efficiently activate C=C, C=O, C=N, and so forth. Iodine not only has been shown to be an efficient mild Lewis acid in various processes, but also due to its moderate nature, and water tolerance, reactions catalyzed by iodine can be effectively carried out in neutral media under very mild conditions. We have successfully described an efficient procedure for the nucleophilic substitution of the Baylis-Hillman (BH) adducts and their corresponding acetates with indoles to get α-substitution product using catalytic Silver Triflate (AgOTf) as Lewis acid. At this point, we were interested to develop an environmentally benign catalytic system to effect this substitution reaction and to avoid the use of metal Lewis acid as a catalyst. Since, we observed the formation of -product during the course of the reaction, we also became interested to explore the reaction conditions in order to control regioselectivity and to obtain both regioisomers. The developed methodology resulted in regioselective substitution products with controlled selectivity. Further, the substitution products were used to synthesize various Tri- and Tetracyclo Azepino indole derivatives via reductive amination.

Keywords: indole, regioselective, Baylis-Hillman, substitution

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Authors: Sri Rahayu, M. Dwi Susan, Aris Soewondo, W. M. Agung Pramana

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Semen is an organic fluid (seminal plasma) that contain spermatozoa. Proteins are one of the major seminal plasma components that modulate sperm functionality, influence sperm capacitation and maintaining the stability of the membrane. Semen freezing is a procedure to preserve sperm cells. The process causes decrease in sperm viability due to temperature shock and oxidation stress. Oxidation stress is a disturbance on phosphorylation that increases ROS concentration, and it produces lipid peroxide in spermatozoa membrane resulted in high MDA (malondialdehyde) concentration. The objective of this study was to examine the effect of freezing on protein and MDA profile of bovine sperm cell and seminal plasma after freezing. Protein and MDA of sperm cell and seminal plasma were isolated from 10 sample. Protein profiles was analyzed by SDS PAGE with separating gel 12,5 %. The concentration of MDA was measured by spectrophotometer. The results of the research indicated that freezing of semen cause lost of the seminal plasma proteins with molecular with 20, 10, and 9 kDa. In addition, the result research showed that protein of the sperm (26, 10, 9, 7, and 6 kDa) had been lost. There were difference MDA concentration of seminal plasma and sperm cell were increase after freezing. MDA concentration of seminal plasma before and after freezing were 2.2 and 2.4 nmol, respectively. MDA concentration of sperm cell before and after freezing were 1,5 and 1.8 nmol, respectively. In conclusion, there were differences protein profiles of spermatozoa before and after semen freezing and freezing cause increasing of the MDA concentration.

Keywords: MDA, semen freezing, SDS PAGE, protein profile

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Authors: Dong Zhao

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Even though the recent claim of room temperature superconductivity by LK-99 was confirmed an unsuccessful attempt, this work reawakened people’s century striving to get applicable superconductors with Tc of room temperature or higher and under ambient pressure. One of the efforts was focusing on exploring the thorium salts. This is because certain thorium compounds revealed an unusual property of having both high electrical conductivity and diamagnetism or the so-called “coexistence of high electrical conductivity and diamagnetism.” It is well known that this property of the coexistence of high electrical conductivity and diamagnetism is held by superconductors because of the electron pairings. Consequently, the likelihood for these thorium compounds to have superconducting properties becomes great. However, as a surprise, these thorium salts possess this property at room temperature and atmosphere pressure. This gives rise to solid evidence for these thorium compounds to be room-temperature superconductors without a need for external pressure. Among these thorium compound superconductors claimed in that work, thorium di-iodide (ThI₂) is a unique one and has received comprehensive discussion. ThI₂ was synthesized and structurally analyzed by the single crystal diffraction method in the 1960s. Its special property of coexistence of high electrical conductivity and diamagnetism was revealed. Because of this unique property, a special molecular configuration was sketched. Except for an ordinary oxidation of +2 for the thorium cation, the thorium’s oxidation state in ThI₂ is +4. According to the experimental results, ThI₂‘s actual molecular configuration was determined as an unusual one of [Th4+(e-)2](I-)2. This means that the ThI₂ salt’s cation is composed of a [Th4+(e-)2]2+ cation core. In other words, the cation of ThI₂ is constructed by combining an oxidation state +4 of the thorium atom and a pair of electrons or an electron lone pair located on the thorium atom. This combination of the thorium atom and the electron lone pair leads to an oxidation state +2 for the [Th4+(e-)2]2+ cation core. This special construction of the thorium cation is very distinctive, which is believed to be the factor that grants ThI₂ the room temperature superconductivity. Actually, the key for ThI₂ to become a room-temperature superconductor is this characteristic electron lone pair residing on the thorium atom along with the formation of a network constructed by the thorium atoms. This network specializes in a way that allows the electron lone pairs to hop over it and, thus, to generate the supercurrent. This work will discuss, in detail, the special electrical and magnetic properties of ThI₂ as well as its structural features at ambient conditions. The exploration of how the electron pairing in combination with the structurally specialized network works together to bring ThI₂ into a superconducting state. From the experimental results, strong evidence has definitely pointed out that the ThI₂ should be a superconductor, at least at room temperature and under atmosphere pressure.

Keywords: co-existence of high electrical conductivity and diamagnetism, electron lone pair, room temperature superconductor, special molecular configuration of thorium di-iodide ThI₂

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Authors: Shrikant Randhavane, Anjali Khambete

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Use of Pesticides is vital in attaining food security and protection from harmful pests and insects in living environment. Chlorpyrifos, an organophosphate pesticide is widely used worldwide for various purposes. Due to its wide use and applications, its residues are found in environmental matrices and persist in nature for long duration of time. This has an adverse effect on human, aquatic and living bodies. Use of different methodologies is need of an hour to treat such type of recalcitrant compound. The paper focuses on Hydrodynamic Cavitation (HC), a hybrid Advanced Oxidation Potential (AOP) method to degrade Chlorpyrifos in aqueous water. Obtained results show that optimum inlet pressure of 5 bars gave maximum degradation of 99.25% for lower concentration and 87.14% for higher concentration Chlorpyrifos solution in 1 hour treatment time. Also, with known initial concentrations, comparing treatment time with optimum pressure of 5 bars, degradation efficiency increases with Hydrodynamic Cavitation. The potential application of HC in removal of Chemical Oxygen Demand (COD) from real effluent with venturi as cavitating device reveals around 40% COD removal with 1 hour of treatment time.

Keywords: advanced oxidation potential, cavitation, chlorpyrifos, COD

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Authors: Souvik Das, Janak Lal, Arthita Dey, Goutam Mukhopadhyay, Sandip Bhattacharya

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Telescopic Front Fork (TFF) used in two wheelers, mainly motorcycle, is made from high strength steel, and is manufactured by high frequency induction welding process wherein hot rolled and pickled coils are used as input raw material for rolling of hollow tubes followed by heat treatment, surface treatment, cold drawing, tempering, etc. The final application demands superior quality TFF tubes w.r.t. surface finish and dimensional tolerances. This paper presents the investigation of two different types of failure of fork during operation. The investigation consists of visual inspection, chemical analysis, characterization of microstructure, and energy dispersive spectroscopy. In this paper, comprehensive investigations of two failed tube samples were investigated. In case of Sample #1, the result revealed that there was a pre-existing crack, known as hook crack, which leads to the cracking of the tube. Metallographic examination exhibited that during field operation the pre-existing hook crack was surfaced out leading to crack in the pipe. In case of Sample #2, presence of internal oxidation with decarburised grains inside the material indicates origin of the defect from slab stage.

Keywords: telescopic front fork, induction welding, hook crack, internal oxidation

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Authors: S. Belakry, D. Fasquelle, A. Rolle, E. Capoen, R. N. Vannier, J. C. Carru

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Solid oxide fuel cells (SOFCs) are promising devices for energy conversion due to their high electrical efficiency and eco-friendly behavior. Their performance is not only influenced by the microstructural and electrical properties of the electrodes and electrolyte but also depends on the interactions at the interfaces. Nowadays, commercial SOFCs are electrically efficient at high operating temperatures, typically between 800 and 1000 °C, which restricts their real-life applications. The present work deals with the objectives to reduce the operating temperature and to develop cost-effective intermediate-temperature solid oxide fuel cells (IT-SOFCs). This work focuses on the development of metal-supported solid oxide fuel cells (MS-IT-SOFCs) that would provide cheaper SOFC cells with increased lifetime and reduced operating temperature. In the framework, the local company TIBTECH brings its skills for the manufacturing of porous metal supports. This part of the work focuses on the physical, chemical, and electrical characterizations of porous metallic supports (stainless steel 316 L and FeCrAl alloy) under different exposure conditions of temperature and atmosphere by studying oxidation, mechanical resistance, and electrical conductivity of the materials. Within the target operating temperature (i.e., 500 to 700 ° C), the stainless steel 316 L and FeCrAl alloy slightly oxidize in the air and H2, but don’t deform; whereas under Ar atmosphere, they oxidize more than with previously mentioned atmospheres. Above 700 °C under air and Ar, the two metallic supports undergo high oxidation. From 500 to 700 °C, the resistivity of FeCrAl increases by 55%. But nevertheless, the FeCrAl resistivity increases more slowly than the stainless steel 316L resistivity. This study allows us to verify the compatibility of electrodes and electrolyte materials with metallic support at the operating requirements of the IT-SOFC cell. The characterizations made in this context will also allow us to choose the most suitable fabrication process for all functional layers in order to limit the oxidation of the metallic supports.

Keywords: stainless steel 316L, FeCrAl alloy, solid oxide fuel cells, porous metallic support

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Authors: Afrouz Yousefi, Mohtada Sadrzadeh

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The widespread presence of poly- and perfluoroalkyl substances (PFAS) poses a significant concern due to their ability to accumulate in living organisms and their persistence in the environment, thanks to their robust carbon-fluorine (C-F) bonds, which require substantial energy to break (485 kJ/mol). The prevalence of toxic PFAS compounds can be highly detrimental to ecosystems, wildlife, and human health. Ongoing efforts are dedicated to investigating methods for fully breaking down and eliminating PFAS from the environment. Among the various techniques employed, advanced oxidation processes have shown promise in completely breaking down emerging contaminants in wastewater. However, the drawback lies in the relatively slow reaction rates of these processes and the substantial energy input required, which currently impedes their widespread commercial adoption. We developed a hybrid process, comprising electro-Fenton as an advanced oxidation process and membrane distillation, to simultaneously degrade organic PFAS pollutants and extract pure water from the mixture. In this study, environmentally persistent perfluorooctanoic acid (PFOA), as an emerging contaminant, was used to study the effectiveness of the electro-Fenton/membrane distillation hybrid system. The PFOA degradation studies were conducted in two modes: electro-Fenton and electro-Fenton coupled with membrane distillation. High-performance liquid chromatography with ultraviolet detection (HPLC-UV), ion-chromatography (measuring fluoride ion concentration), total organic carbon (TOC) decay, mineralization current efficiency (MCE), and specific energy consumption (SEC) were evaluated for a single EF and hybrid EF-MD processes. In contrast to a single EF reaction, TOC decay improved significantly in the EF-MD process. Overall, the MCE of hybrid processes surpassed 100% while it remained under 50% for a single EF reaction. Calculations of specific energy consumption (SEC) demonstrated a substantial decrease of nearly one-third in energy usage when integrating the EF reaction with the MD process.

Keywords: water treatment, PFAS, membrane distillation, electro-Fenton, advanced oxidation

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Authors: Radia Bagtache, Karima Boudjedien, Ahmed Malek Djaballah, Mohamed Trari

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The compounds with a spinel structure have received special attention because of their numerous applications in electronics, magnetism, catalysis, electrocatalysis, photocatalysis, etc. Among these oxides, CuCo₂O₄ was selected because of its optimal band gap, very close to the ideal value for solar devices, its low cost, and a potential candidate in the field of energy storage. Herein, we reported the junction Ag/CuCo₂O₄ (5/95 % wt.) prepared by co-precipitation, characterized physically and photo electrochemically. Moreover, its performance was evaluated for the oxidation of methyl orange (MO) under solar light. The X-ray diffraction exhibited narrow peaks ascribed to the spinel CuCo₂O₄ and Ag. The SEM analysis displayed grains with regular shapes. The band gap of CuCo₂O₄ (1.38 eV) was deducted from the diffuse reflectance, and this value decreased down to 1.15 eV due to the synergy effect in the junction. The current-potential (J-E) curve plotted in Na₂SO₄ electrolyte showed a medium hysteresis, characteristic of good chemical stability. The capacitance-2 – potential (C⁻² – E) graph displayed that the spinel behaves as a p-type semiconductor, a property supported by chrono-amperometry. The conduction band, located at 4.05 eV (-0.94 VNHE), was made up of Co³⁺: 3d orbital. The result showed a total discoloration of MO after 2 h of illumination under solar light.

Keywords: junction Ag/CuCo₂O₄, semiconductor, environment, sunlight, characterization, depollution

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Authors: Rehin Sulay, Anandhu Krishna, Jintumol Mathew, Vibin Ipe Thomas

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N-Nitrosodimethyl amine, the simplest member of the N-Nitrosoamine family, is a carcinogenic and mutagenic agent that has gained considerable research interest owing to its toxic nature. Ozonation of industrially important hydrazines such as unsymmetrical dimethylhydrazine (UDMH) or monomethylhydrazine (MMH) has been associated with NDMA formation and accumulation in the environment. UDMH/MMH - ozonation also leads to several other transformation products such as acetaldehyde dimethyl hydrazone (ADMH), tetramethyl tetra azene (TMT), diazomethane, methyl diazene, etc, which can be either precursors or competitors for NDMA formation.In this work, we explored the formation mechanism of ADMH and TMT from UDMH-ozonation and their further oxidation to NDMA using the second-order Moller Plesset perturbation theory employing the 6-311G(d) basis set. We have also investigated how MMH selectively forms methyl diazene and diazomethane under normal conditions and NDMA in the presence of excess ozone. Our calculations indicate that the reactions proceed via an initial H abstraction from the hydrazine –NH2 group followed by the oxidation of the generated N-radical species. The formation of ADMH from the UDMH-ozone reaction involves an acetaldehyde intermediate, which then reacts with a second UDMH molecule to generate ADMH. The preferable attack of ozone molecule on N=C bond of ADMH generates DMAN intermediate, which subsequently undergoes oxidation to form NDMA. Unlike other transformation products, TMT formation occurs via the dimerization of DMAN. Though there exist a N=N bonds in the TMT, which are preferable attacking sites for ozone, experimental studies show the lower yields of NDMA formation, which corroborates with the high activation barrier required for the process(42kcal/mol).Overall, our calculated results agree well with the experimental observations and rate constants. Computational calculations bring insights into the electronic nature and kinetics of the elementary reactions of this pathway, enabled by computed energies of structures that are not possible to access experimentally.

Keywords: reaction mechanism, ozonation, substituted hydrazine, transition state

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Authors: Abdullah Alhajoj, Bassam Alowaiesh

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This work aims to reduce the risks of discharging olive mill waste directly to the environment without treatment in Sakaka City, KSA. The organic loads expressed by chemical oxygen demand (COD) and biological oxygen demand (BOD) of the produced wastewater (OMWW) as well as the solid waste (OMW) were evaluated. The wastes emitted from the three-phase centrifuge decanters was found to be higher than that emitted from the two-phase centrifuge decanters. The olive mill wastewater (OMWW) was treated using advanced oxidation combined with filtration treatment. The results indicated that the concentration of COD, BOD, TSS, oil and grease and phenol was reduced by using complex sand filtration from 72150, 21660 10256, 36430, and 1470 mg/l to 980, 421, 58, 68, and 0.35 mg/l for three-phase OMWW and from 150562, 17955, 15325, 19658 and 2153 mg/l to 1050, 501, 29, 0.75, and 0.29 mg/l, respectively. While, by using modified trickling filter (packed with the neck of waste plastic bottles the concentration of the previously mentioned parameters was reduced to 1190, 570, 55, 0.85, and 0.3 mg/l, respectively. This work supports the application of such treatment technique for reducing the environmental threats of olive mill waste effluents in Saudi Arabia.

Keywords: two-phase, three-phase, olive mill, olive oil, waste treatment, filtration, advanced oxidation, waste plastic bottles

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Authors: Seyed Mohamad Rasool Mirkarimi, David Chiaramonti, Samir Bensaid

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Catalytic methane decomposition (CMD, reaction 4) is a one-step process for hydrogen production where carbon in the methane molecule is sequestered in the form of stable and higher-value carbon materials. Metallic catalysts and carbon-based catalysts are two major types of catalysts utilized for the CDM process. Although carbon-based catalysts have lower activity compared to metallic ones, they are less expensive and offer high thermal stability and strong resistance to chemical impurities such as sulfur. Also, it would require less costly separation methods as some of the carbon-based catalysts may not have an active metal component in them. Since the regeneration of metallic catalysts requires burning of the C on their surfaces, which emits CO/CO2, in some cases, using carbon-based catalysts would be recommended because regeneration can be completely avoided, and the catalyst can be directly used in other processes. This work focuses on the effect of biochar as a carbon-based catalyst for the conversion of methane into hydrogen and carbon. Biochar produced from the pyrolysis of poplar wood and activated biochar are used as catalysts for this process. In order to observe the impact of carbon-based catalysts on methane conversion, methane cracking in the absence and presence of catalysts for a gas stream with different levels of methane concentration should be performed. The results of these experiments prove conversion of methane in the absence of catalysts at 900 °C is negligible, whereas in the presence of biochar and activated biochar, significant growth has been observed. Comparing the results of the tests related to using char and activated char shows the enhancement obtained in BET surface area of the catalyst through activation leads to more than 10 vol.% methane conversion.

Keywords: hydrogen production, catalytic methane decomposition, biochar, activated biochar, carbon-based catalyts

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Authors: Rajashekar Badam, Vedarajan Raman, Noriyoshi Matsumi

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Efficiency of energy converting and storage systems like fuel cells and Li-Air battery principally depended on oxygen reduction reaction (ORR) which occurs at cathode. As the kinetics of the ORR is very slow, it becomes the rate determining step. Exploring carbon substrates for enhancing the dispersion and activity of the metal catalyst and commercially viable simple preparation method is a very crucial area of research in the field of energy materials. Hence, many researchers made large number of carbon-based ORR materials today. But, there are hardly few studies on the effect of interaction between Pt-carbon and carbon-electrolyte on activity. In this work, we have prepared functionalized carbon-based Pt catalyst (Pt-FAB) with enhanced interfacial properties that lead to efficient ORR catalysis. The present work deals with a single-pot method to exfoliate and functionalized acetylene black with enhanced interaction with Pt as well as electrolyte. Acetylene black was functionalized and exfoliated using a facile single pot acid treatment method. The resulted FAB was further decorated with Pt-nano particles (Pt-np). The TEM images of Pt-FAB with uniformly decorated Pt-np of ~3 nm. Further, XPS studies of Pt 4f peak revealed that Pt0 peak was shifted by 0.4 eV in Pt-FAB compared to binding energy of typical Pt⁰ found in Pt/C. The shift can be ascribed to the modulation of electronic state and strong electronic interaction of Pt with carbon. Modulated electronic structure of Pt and strong electronic interaction of Pt with FAB enhances the catalytic activity and durability respectively. To understand the electrode electrolyte interface, electrochemical impedance spectroscopy was carried out. These measurements revealed that the charge transfer resistance of electrode to electrolyte for Pt-FAB is 10 times smaller than that of conventional Pt/C. The interaction with electrolyte helps reduce the interface boundaries, which in turn affects the overall catalytic performance of the electrode. Cyclic voltammetric measurements in 0.1M HClO₄ aq. at a potential scan rate of 50 mVs-1 was employed to evaluate electrochemical surface area (ECSA) of Pt. ECSA of Pt-FAB was found to be as high as 67.2 m²g⁻¹. The three-electrode system showed very high ORR catalytic activity. Mass activity at 0.9 V vs. RHE showed 460 A/g which is much higher than the DOE target values for the year 2020. Further, it showed enhanced performance by showing 723 mW/cm² of highest power density and 1006 mA/cm² of current density at 0.6 V in fuel cell single cell type configuration and 1030 mAhg⁻¹ of rechargeable capacity in Li air battery application. The higher catalytic activity can be ascribed to the improved interaction of FAB with Pt and electrolyte. The aforementioned results evince that Pt-FAB will be a promising cathode material for efficient ORR with significant cyclability for its application in fuel cells and Li-Air batteries. In conclusion, a disordered material was prepared from AB and was systematically characterized. The extremely high ORR activity and ease of preparation make it competent for replacing commercially available ORR materials.

Keywords: functionalized acetylene black, oxygen reduction reaction, fuel cells, Functionalized battery

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Authors: Ádám Vass, István Bakos, Irina Borbáth, Zoltán Pászti, István Sajó, András Tompos

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Important requirements for the anode side electrocatalysts of polymer electrolyte membrane (PEM) fuel cells are CO-tolerance, stability and corrosion resistance. Carbon is still the most common material for electrocatalyst supports due to its low cost, high electrical conductivity and high surface area, which can ensure good dispersion of the Pt. However, carbon becomes degraded at higher potentials and it causes problem during application. Therefore it is important to explore alternative materials with improved stability. Molybdenum-oxide can improve the CO-tolerance of the Pt/C catalysts, but it is prone to leach in acidic electrolyte. The Mo was stabilized by isovalent substitution of molybdenum into the rutile phase titanium-dioxide lattice, achieved by a modified multistep sol-gel synthesis method optimized for preparation of Ti0.7Mo.3O2-C composite. High degree of Mo incorporation into the rutile lattice was developed. The conductivity and corrosion resistance across the anticipated potential/pH window was ensured by mixed oxide – activated carbon composite. Platinum loading was carried out using NaBH4 and ethylene glycol; platinum content was 40 wt%. The electrocatalyst was characterized by both material investigating methods (i.e. XRD, TEM, EDS, XPS techniques) and electrochemical methods (cyclic-voltammetry, COads stripping voltammetry, hydrogen oxidation reaction on rotating disc electrode). The electrochemical activity of the sample was compared to commercial 40 wt% Pt/C (Quintech) and PtRu/C (Quintech, Pt= 20 wt%, Ru= 10 wt%) references. Enhanced CO tolerance of the electrocatalyst prepared using the Ti0.7Mo.3O2-C composite material was evidenced by the appearance of a CO-oxidation related 'pre-peak' and by the pronounced shift of the maximum of the main CO oxidation peak towards less positive potential compared to Pt/C. Fuel cell polarization measurements were also carried out using Bio-Logic and Paxitech FCT-150S test device. All details on the design, preparation, characterization and testing by both electrochemical measurements and fuel cell test device of electrocatalyst supported on Ti0.7Mo.3O2-C composite material will be presented and discussed.

Keywords: anode electrocatalyst, composite material, CO-tolerance, TiMoOx

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Authors: Ahmed Tawfik

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Oxidation of 1,4 dioxane produces metabolites by-products involving glycolaldehyde and acids that have geno- and cytotoxicity impact on microbial degradation. Thereby, the incorporation of algae with bacteria in the treatment system would eliminate and overcome the accumulation of metabolites that are utilized as a carbon source for the build-up of biomass. Therefore, the aim of the present study is to assess the potential of algae/bacteria-based membrane bioreactor (AB-MBR) for biodegradation of 1,4 dioxane-rich wastewater at a high imposed loading rate. Three identical reactors, i.e., AB-MBR1, AB-MBR2, and AB-MBR3, were operated in parallel at 1,4 dioxane loading rates of 641.7, 320.9, and 160.4 mg/L. d., and HRTs of 6.0, 12 and 24 h. respectively. The AB-MBR1 achieved 1,4 dioxane removal rate of 263.7 mg/L.d., where the residual value in the treated effluent amounted to 94.4±22.9 mg/L. Reducing the 1,4 dioxane loading rate (LR) to 320.9 mg/L.d in the AB-MBR2 maximized the removal rate efficiency of 265.9 mg/L.d., with a removal efficiency of 82.8±3.2%. The minimum value of 1,4 dioxane of 17.3±1.8 mg/L in the treated effluent of AB-MBR3 was obtained at an HRT of 24.0 h and loading rate of 160.4 mg/L.d. The mechanism of 1,4 dioxane degradation in AB-MBR was a combination of volatilization (8.03±0.6%), UV oxidation (14.1±0.9%), microbial biodegradation (49.1±3.9%) and absorption/uptake and assimilation by algae (28.8±2.%). Further, the Thioclava, Afipia, and Mycobacterium genera oxidized and produced the required enzymes for hydrolysis and cleavage of the dioxane ring into 2-hydroxy-1,4 dioxane. Moreover, the fungi, i.e., Basidiomycota and Cryptomycota, played a big role in the degradation of the 1,4 dioxane into 2-hydroxy-1,4 dioxane. Xanthobacter and Mesorhizobium were involved in the metabolism process by secreting alcohol dehydrogenase (ADH), aldehyde dehydrogenase (ALDH), and glycolate oxidase. Bacteria and fungi produced dehydrogenase (DH) for the transformation of 2-hydroxy-1,4 dioxane into 2-hydroxy-ethoxyacetaldehyde. The latter is converted into Ethylene glycol by Aldehyde hydrogenase (ALDH). Ethylene glycol is oxidized into acids using Alcohol hydrogenase (ADH). The Diatomea, Chlorophyta, and Streptophyta utilize the metabolites for biomass assimilation and produce the required oxygen for further oxidation of the dioxane and its metabolites by-products of bacteria and fungi. The major portion of metabolites (ethylene glycol, glycolic acid, and oxalic acid were removed due to uptake and absorption by algae (43±4.3%), followed by adsorption (18.4±0.9%). The volatilization and UV oxidation contribution for the degradation of metabolites were 8.7±0.7% and 12.3±0.8%, respectively. The capabilities of genera Defluviimonas, Thioclava, Luteolibacter, and Afipia. The genera of Defluviimonas, Thioclava, Luteolibacter, and Mycobacterium were grown under a high 1,4 dioxane LR of 641.7 mg/L.d. The Chlorophyta (4.1-43.6%), Streptophyta (2.5-21.7%), and Diatomea (0.8-1.4%) phyla were dominant for degradation of 1,4 dioxane. The results of this study strongly demonstrated that the bioremediation and bioaugmentation process can safely remove 1,4 dioxane from industrial wastewater while minimizing environmental concerns and reducing economic costs.

Keywords: wastewater, membrane bioreactor, bacterial community, algal community

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Authors: Sajad A. Rather, F. A. Masoodi, Rehana Akhter, S. M. Wani, Adil Gani

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Modern trend towards convenience foods has resulted in increased production and consumption of restructured meat products and are of great importance to the meat industry. In meat products fat plays an important role in cooking properties, texture & sensory scores, however, high fat contents in particular animal fats provide high amounts of saturated fatty acids and cholesterol and are associated with several types of non communicable diseases such as obesity, hypertension and coronary heart diseases. Thus, fat reduction has generally been seen as an important strategy to produce healthier meat products. This study examined the effects of reducing fat level from 20% to 10% and substituting mutton back fat with guar gum (0.5%, 1% & 1.5%) on cooking properties, proximate composition, lipid and protein oxidation, texture, microstructure and sensory characteristics of goshtaba- a traditional meat product of J & K, India were investigated and compared with high fat counterparts. Reduced- fat goshtaba samples containing guar gum had significantly (p ≤ 0.05) higher yield, less shrinkage, more moisture retention and more protein content than the control sample. TBARs and protein oxidation (carbonyl content) values of the control was significantly (p ≤ 0.05) higher than reduced fat goshtaba samples and showed a positive correlation between lipid and protein oxidation. Hardness, gumminess & chewiness of the control (20%) were significantly higher than reduced fat goshtaba samples. Microstructural differences were significant (p ≤ 0.05) between control and treated samples due to an increased moisture content in the reduced fat samples. Sensory evaluation showed significant (p ≤ 0.05) reduction in texture, flavour and overall acceptability scores of treatment products; however the scores for 0.5% and 1% treated samples were in the range of acceptability. Guar gum may also be used as a source of soluble dietary fibre in food products and a number of clinical studies have shown a reduction in postprandial glycemia and insulinemia on consumption of guar gum, with the mechanism being attributed to an increased transit time in the stomach and small intestine, which may have been due to the viscosity of the meal hindering the access of glucose to the epithelium.

Keywords: goshtaba, guar gum, traditional, fat reduction, acceptability

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Authors: Merouani Djilali Redha, F. Abdelmalek, A. A. Addou

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Advanced oxidation processes (AOPs) utilizing Homogenous photocatalysis (Fenton and photo-Fenton reactions), and Heterogeneous photocatalyse (TiO2 and ZnO) were investigated for the degradation of commercial azo dye ‘Orange G’ wastewater. Fenton and photo-Fenton experimental conditions were: Hydrogen peroxide concentration (10-2 M), Ferrous ions concentration (5.10-4 M), pH (2.8 – 3), UV lamp power (6 watt). Adding more ferrous ions enhanced the oxidation rate for the H2O2/Fe2+ and UV/H2O2/Fe2+ processes. The optimum catalyst loading was found 2.0 g.L-1 in our case for both catalysts TiO2 and ZnO. A comparative study of the photocatalytic degradation showed that these two catalysts have a comparable reactivity; it follows a pseudo-first-order kinetics. The degradation trends followed the order: UV365/Fenton > UV365/TiO2 > Solar Fenton > Solar TiO2 > Fenton ~UV365/ZnO. Among AOPs, processes using Fenton type reagent are relatively cheap and easy to operate and maintain. Moreover, UV365/Fenton process has been shown as effective in the treatment of OG dye. Dye was degraded following second-order kinetics. The rate constants was 0,041 .10+6 L.M-1.min-1. The degradation was followed by spectrophotometric method, chemical oxygen demand (COD) measures and high performance liquid chromatography analyses (HPLC). Some aromatic and aliphatic degradation compounds were identified. Degradation of Orange G by UV Fenton mechanism was also proposed.

Keywords: AOPs, homogeneous catalysis, heterogeneous catalysis, acid orange 10, hydroxyl radical

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Authors: Masood Otarod, Ronald M. Supkowski

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This abstract discusses a method that reduces the general dispersion model in cylindrical coordinates to a second order linear ordinary differential equation with constant coefficients so that it can be utilized to conduct kinetic studies in packed bed tubular catalytic reactors at a broad range of Reynolds numbers. The model was tested by 13CO isotope transient tracing of the CO adsorption of Boudouard reaction in a differential reactor at an average Reynolds number of 0.2 over Pd-Al2O3 catalyst. Detailed experimental results have provided evidence for the validity of the theoretical framing of the model and the estimated parameters are consistent with the literature. The solution of the general dispersion model requires the knowledge of the radial distribution of axial velocity. This is not always known. Hence, up until now, the implementation of the dispersion model has been largely restricted to the plug-flow regime. But, ideal plug-flow is impossible to achieve and flow regimes approximating plug-flow leave much room for debate as to the validity of the results. The reduction of the general dispersion model transpires as a result of the application of a factorization theorem. Factorization theorem is derived from the observation that a cross section of a catalytic bed consists of a solid phase across which the reaction takes place and a void or porous phase across which no significant measure of reaction occurs. The disparity in flow and the heterogeneity of the catalytic bed cause the concentration of reacting compounds to fluctuate radially. These variabilities signify the existence of radial positions at which the radial gradient of concentration is zero. Succinctly, factorization theorem states that a concentration function of axial and radial coordinates in a catalytic bed is factorable as the product of the mean radial cup-mixing function and a contingent dimensionless function. The concentration of adsorbed compounds are also factorable since they are piecewise continuous functions and suffer the same variability but in the reverse order of the concentration of mobile phase compounds. Factorability is a property of packed beds which transforms the general dispersion model to an equation in terms of the measurable mean radial cup-mixing concentration of the mobile phase compounds and mean cross-sectional concentration of adsorbed species. The reduced model does not require the knowledge of the radial distribution of the axial velocity. Instead, it is characterized by new transport parameters so denoted by Ωc, Ωa, Ωc, and which are respectively denominated convection coefficient cofactor, axial dispersion coefficient cofactor, and radial dispersion coefficient cofactor. These cofactors adjust the dispersion equation as compensation for the unavailability of the radial distribution of the axial velocity. Together with the rest of the kinetic parameters they can be determined from experimental data via an optimization procedure. Our data showed that the estimated parameters Ωc, Ωa Ωr, are monotonically correlated with the Reynolds number. This is expected to be the case based on the theoretical construct of the model. Computer generated simulations of methanation reaction on nickel provide additional support for the utility of the newly conceptualized dispersion model.

Keywords: factorization, general dispersion model, isotope transient kinetic, partial differential equations

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Authors: Bilal Murtaza, Xiaoyu Li, Liming Dong, Muhammad Kashif Saleemi, Gen Li, Bowen Jin, Lili Wang, Yongping Xu

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Fusarium spp. produce numerous mycotoxins, such as zearalenone (ZEN), deoxynivalenol (DON), and its acetylated compounds, 3-acetyl-deoxynivalenol (3-ADON) and 15-acetyl-deoxynivalenol (15-ADON) (15-ADON). In a co-culture system, the soil-derived Escherichia marmotae strain degrades ZEN and DON into 3-keto-DON and DOM-1 via enzymatic deep-oxidation. When pure mycotoxins were subjected to Escherichia marmotae in culture flasks, degradation, and detoxification were also attained. DON and ZEN concentrations, ambient pH, incubation temperatures, bacterium concentrations, and the impact of acid treatment on degradation were all evaluated. The results of the ELISA and high-performance liquid chromatography-electrospray ionization-high resolution mass spectrometry (HPLC-ESI-HRMS) tests demonstrated that the concentration of mycotoxins exposed to Escherichia marmotae was significantly lower than the control. ZEN levels were reduced by 43.9%, while zearalenone sulfate ([M/z 397.1052 C18H21O8S1) was discovered as a derivative of ZEN converted by microbes to a less toxic molecule. Furthermore, Escherichia marmotae appeared to metabolize DON 35.10% into less toxic derivatives (DOM-1 at m/z 281 of [DON - O]+ and 3-keto-DON at m/z 295 of [DON - 2H]+). These results show that Escherichia marmotae can reduce Fusarium mycotoxins production, degrade pure mycotoxins, and convert them to less harmful compounds, opening up new possibilities for study and innovation in mycotoxin detoxification.

Keywords: mycotoxins, zearalenone, deoxynivalenol, bacterial degradation

Procedia PDF Downloads 79

Authors: G. Imran, A. Pandurangan

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Epoxides constitute important intermediates for the production of fine and bulk chemicals as well as valuable building blocks for the synthesis of a variety of bioactive molecules. Manganese oxides are used as selective catalyst for various redox type reactions and also effectively used in the field of catalytic disposal of pollutants. Non-toxic, cost efficient factor and more over existence of wide range of oxidation state (+2 to +7) makes catalyst more interesting for both academic research and industrial applications. However, the serious drawback lying is the lower surface area. Exceedingly dispersed manganese oxide grafted over mesoporous solid material KIT-6 through ALD (Atomic Layer Deposition) technique effectively catalyze cyclohexene with H2O2 (30% in water) to corresponding epoxides. Highly selective epoxide >99% with 55.7% conversion of cyclohexene was achieved using huge dispersed active sites of MnOx species containing catalysts. Various weight percent such as (1, 3, 5, 7 & 10 wt %) of manganese (II) acetylacetonate complex was employed as Mn source to post-graft via active silanol groups of KIT-6 and are designated as (Mn-G-KIT-6). XRD, N2 sorption, HR-TEM, DRS-UV-VIS, EPR and H2-TPR were employed for structural and textural properties. Immense Mn species of about 95% proportion on silica matrix obtained was evident from ICP-OES.The resulting materials exhibited Type IV adsorption isotherms indiacting mesopore in nanorange. Si-KIT-6 and Mn-G-KIT-6 materials exhibited surface area of 519-289 m2/g and with decrease in pore volume of 0.96-0.49 cm3/g with pore diameter ranging 7.9- 7.2 with increase in wt%. DRS-UV-VIS spectroscopy and EPR studies reveal that manganese coexists as Mn2+/3+ species as extra-framework sites and frame-work sites that result in dispersion on surface of silica matrix of KIT-6 and incorporated manganese sites with silanol groups along with small sized MnO cluster, evident from HR-TEM which increase with Mn content. Conventional production of epoxides by the intramolecular etherification of chlorohydrins formed by the reaction of alkenes with hypochlorous acid is the major drawbacks obtained recently. The most efficient synthesis of oxiranes (epoxides) is obtained by mesoporous catalysts (Mn-G-KIT-6) are presented here and discussed.

Keywords: ALD, epoxidation, mesoporous, MnOx

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Authors: D. Tassalit, N. Chekir, O. Benhabiles, N. A. Laoufi, F. Bentahar

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In the setting of the waters purification, some molecules appear recalcitrant to the traditional treatments. The exploitation of the properties of some catalysts permits to amplify the oxidization performances with ultraviolet radiance and to remove this pollution by a non biological way. This study was conducted to investigate the effect of a photocatalysis oxidation system for organic pollutants treatment using a new reactor design and ZnO/TiO2 as a catalyst under UV light. Oxidative degradation of tylosin by hydroxyl radicals (OH°) was studied in aqueous medium using suspended forms of ZnO and TiO2. The results improve that the treatment was affected by many factors such as flow-rate of solution, initial pollutant concentration and catalyst concentration. The rate equation for the tylosin degradation followed first order kinetics and the rate-constants were determined. The reaction rate fitted well with Langmuir–Hinshelwood model and the removed ratio of tylosin was 97 % in less than 60 minutes. To determine the optimum catalyst loading, a series of experiments were carried out by varying the amount of catalyst from 0.05 to 0.5 g/L. The results demonstrate that the rate of photodegradation is optimum with catalyst loading of 0.1 g/L, reaction flow rate of 3.79 mL/s and solution natural pH. The rate was found to increase with the decrease in tylosin concentration from 30 to 5 mg/L. Therefore, this simple photoreactor design for the removal of organic pollutants has the potential to be used in wastewater treatment.

Keywords: advanced oxidation, photocatalysis, TiO2, ZnO, UV light, pharmaceuticals pollutants, Spiramycin, tylosin, wastewater treatment

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Authors: Sibel Dikmen Kucuk, Yusuf Guner

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In recent years, petroleum-based polymers began to be limited due to the effects on the human and environmental point of view in many countries. Thus, organic-based biodegradable materials have attracted much interest in the composite industry because of environmental concerns. As a result of this, it has been asked that inorganic and petroleum-based materials should be reduced and altered with biodegradable materials. In this point, in this study, it is aimed to investigate the potential of the use of TEMPO (2,2,6,6- tetramethylpiperidine 1-oxyl)-mediated oxidation nano-fibrillated cellulose instead of EPDM (ethylene-propylene-diene monomer) rubber, which is a petroleum-based material. Thus, the exchange of petroleum-based EPDM rubber with organic-based cellulose nanofibers, which are environmentally friendly (green) and biodegradable, will be realized. The effect of tempo-oxidized cellulose nanofibers (TCNF) instead of EPDM rubber was analyzed by rheological, mechanical, chemical, thermal, and aging analyses. The aged surfaces were visually scrutinized, and surface morphological changes were examined via scanning electron microscopy (SEM). The results obtained showed that TEMPO oxidation nano-fibrillated cellulose could be used at an amount of 1.0 and 2.2 phr resulting the values stay within tolerance according to customer standard and without any chemical degradation, crack, color change or staining.

Keywords: EPDM, lignin, green materials, biodegradable fillers

Procedia PDF Downloads 114

Authors: Zhao Bo

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The TiO2-Na2SO3 and SiO2-Na2SO3 nano-fluids were prepared using ultrasonic dispertion method without any surfactant addition to study the influence of nano-fluids on the mass transfer during forced sulfite oxidation in a thermostatic stirred tank, and the kinetic viscosity of nano-fluids was measured. The influence of temperature (30 ℃ ~ 50 ℃), solid loading of fine particle (0 Kg/m³~1.0 Kg/m³), stirring speed (50 r/min ~ 400 r/min), and particle size (10 nm~100 nm) on the average oxygen absorption rate were investigated in detail. Both TiO2 nano-particles and SiO2 nano-particles could remarkably improve the gas-liquid mass transfer. Oxygen absorption enhancement factor increases with the increase of solid loading of nano-particles to a critical value and then decreases with further increase of solid loading under 30℃. Oxygen absorption rate together with absorption enhancement factor increases with stirring speed. However, oxygen absorption enhancement factor decreases with the increase of temperature due to aggregation of nano-particles. Further inherent relationship between particle size, loading, surface area, viscosity, stirring speed, temperature, adsorption, desorption, and mass transfer was discussed in depth by analyzing the interaction mechanism.

Keywords: fine particles, nano-fluid, mass transfer enhancement, solid loading

Procedia PDF Downloads 226

Authors: Chaoqun Tan, Naiyun Gao, Xiaoyan Xin

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Perxymonosulfate (PMS)-based oxidation processes, as an alternative of hydrogen peroxide-based oxidation processes, are more and more popular because of reactive radical species (SO4-•, OH•) produced in systems. Magnetic nano-scaled particles Fe3O4 and ferrous anion (Fe2+) were studied for the activation of PMS for degradation of acetaminophen (APAP) in water. The Fe3O4 MNPs were found to effectively catalyze PMS for APAP and the reactions well followed a pseudo-first-order kinetics pattern (R2 > 0.95), while the degradation of APAP in PMS-Fe2+ system proceeds through two stages: a fast stage and a much slower stage. Within 5 min, approximately 7% and 18% of 10 ppm APAP was accomplished by 0.2 mM PMS in Fe3O4 (0.8g/L) and Fe2+ (0.1mM) activation process. However, as reaction proceed to 120 min, approximately 75% and 35% of APAP was removed in Fe3O4 activation process and Fe2+ activation process, respectively. Within 120 min, the mineralization of APAP was about 7.5% and 5.0% (initial APAP of 10 ppm and [PMS]0 of 0.2 mM) in Fe3O4-PMS and Fe2+-PMS system, while the mineralization could be greatly increased to about 31% and 40% as [PMS]0 increased to 2.0 mM in in Fe3O4-PMS and Fe2+-PMS system, respectively. At last, the production of reactive radical species were validated directly from Electron Paramagnetic Resonance (ESR) tests with 0.1 M 5,5-dimethyl-1-pyrrolidine N-oxide (DMPO). Plausible mechanisms on the radical generation from Fe3O4 and Fe2+ activation of PMS are proposed on the results of radial identification tests. The results demonstrated that Fe3O4 MNPs activated PMS and Fe2+ anion activated PMS systems are promising technologies for water pollution caused by contaminants such as pharmaceutical. Fe3O4-PMS system is more suitable for slowly remediation, while Fe2+-PMS system is more suitable for fast remediation.

Keywords: acetaminophen, peroxymonosulfate, radicals, Fe3O4

Procedia PDF Downloads 243

Authors: Karima Benfadel, Lamia Talbi, Sabiha Anas Boussaa, Afaf Brik, Assia Boukezzata, Yahia Ouadah, Samira Kaci

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In order to prevent global warming, which is mainly caused by the increase in carbon dioxide levels in the atmosphere, it is interesting to produce renewable energy in the form of chemical energy by converting carbon dioxide into alternative fuels and other energy-dense products. Photoelectrochemical reduction of carbon dioxide to value-added products and fuels is a promising and current method. The objective of our study is to develop Cu₂S-based photoélectrodes, in which Cu₂S is used as a CO₂ photoelectrocatalyst deposited on nanostructured silicon substrates. Cu₂S thin layers were deposited using the chemical bath deposition (CBD) technique. Silicon nanowires and nanopyramids were obtained by alkaline etching. SEM and UV-visible spectroscopy was used to analyse the morphology and optical characteristics. By using a potentiostat station, we characterized the photoelectrochemical properties. We performed cyclic voltammetry in the presence and without CO₂ purging as well as linear voltammetry (LSV) in the dark and under white light irradiation. We perform chronoamperometry to study the stability of our photocathodes. The quality of the nanowires and nanopyramids was visible in the SEM images, and after Cu₂S deposition, we could see how the deposition was distributed over the textured surfaces. The inclusion of the Cu₂S layer applied on textured substrates significantly reduces the reflectance (R%). The catalytic performance towards CO₂ conversion of Cu₂S/Si-based photocathodes revealed that the texturing of the silicon surface with nanowires and pyramids has a better photoelectrochemical behavior than those without surface modifications.

Keywords: CO₂ conversion, Cu₂S photocathode, silicone nanostructured, electrochemistry

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Authors: Noreen Sajjad Ghulam Hussain

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Catalysts are prepared by simple physical mixing and thermal treatment of support and metal acetate precursors.The effect of metal ratio and metal loading to produce highly active catalyst for the oxidation of benzyl alcohol are studied.

Keywords: catalyst, acetates, benzyl alcohols

Procedia PDF Downloads 421

Authors: Matthew E. Potter, Daniel J. Stewart, Lindsay M. Armstrong, Pier J. A. Sazio, Robert R. Raja

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Rising CO₂ levels in the atmosphere means that CO₂ is a highly desirable feedstock. This requires specific catalysts to be designed to activate this inert molecule, combining a catalytic site tailored for CO₂ transformations with a support that can readily adsorb CO₂. Metal organic frameworks (MOFs) are regularly used as CO₂ sorbents. The organic nature of the linker molecules, connecting the metal nodes, offers many post-synthesis modifications to introduce catalytic active sites into the frameworks. However, the metal nodes may be coordinatively unsaturated, allowing them to bind to organic moieties. Imidazoles have shown promise catalyzing the formation of cyclic carbonates from epoxides with CO₂. Typically, this synthesis route employs toxic reagents such as phosgene, liberating HCl. Therefore an alternative route with CO₂ is highly appealing. In this work we design active sites for CO₂ activation, by tethering substituted-imidazole organocatalytic species to the available Cr3+ metal nodes of a Cr-MIL-101 MOF, for the first time, to create a tailored species for carbon capture utilization applications. Our tailored design strategy combining a CO₂ sorbent, Cr-MIL-101, with an anchored imidazole results in a highly active and selective multifunctional catalyst, achieving turnover frequencies of over 750 hr-1. These findings demonstrate the synergy between the MOF framework and imidazoles for CO₂ utilization applications. Further, the effect of substrate variation has been explored yielding mechanistic insights into this process. Through characterization, we show that the structural and compositional integrity of the Cr-MIL-101 has been preserved on functionalizing the imidazoles. Further, we show the binding of the imidazoles to the Cr3+ metal nodes. This can be seen through our EPR study, where the distortion of the Cr3+ on binding to the imidazole shows the CO₂ binding site is close to the active imidazole. This has a synergistic effect, improving catalytic performance. We believe the combination of MOF support and organocatalyst allows many possibilities to generate new multifunctional catalysts for CO₂ utilisation. In conclusion, we have validated our design procedure, combining a known CO₂ sorbent, with an active imidazole species to create a unique tailored multifunctional catalyst for CO₂ utilization. This species achieves high activity and selectivity for the formation of cyclic carbonates and offers a sustainable alternative to traditional synthesis methods. This work represents a unique design strategy for CO₂ utilization while offering exciting possibilities for further work in characterization, computational modelling, and post-synthesis modification.

Keywords: carbonate, catalysis, MOF, utilisation

Procedia PDF Downloads 168