Search results for: spent catalysts

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

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HZSM-5 zeolites modified by iron and phosphorus were applied in catalytic cracking of butene. N2 adsorption and NH3-TPD were employed to measure the structure and acidity of catalysts. The results indicate that increasing phosphorus loading decreased surface area, pore volume and strong acidity of catalysts. The introduction of phosphorus significantly decreased butene conversion and promoted propylene selectivity. The catalytic performance of catalyst was strongly dependent on the reaction conditions. Appropriate reaction conditions could suppress side reactions and enhance propylene selectivity.

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

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Authors: Shuwen Wu, Zhi LI

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Atomically dispersed Fe‒N₄ catalysts are proven as promising alternatives to commercial Pt/C for the oxygen reduction reaction. Most reported Fe‒N₄ catalysts suffer from inferior O‒O bond-breaking capability due to superoxo-like O₂ adsorption, though the isolated dual-atomic metal sites strategy is extensively adopted. Atomic Fe clusters hold greater promise for promoting O‒O bond cleavage by forming peroxo-like O₂ adsorption. However, the excessively strong binding strength between Fe clusters and oxygenated intermediates sacrifices the activity. Here, we first report a Fex/Cu‒N@CF catalyst with atomic Fe clusters functionalized by adjacent single Cu‒N₄ sites anchoring on a porous carbon nanofiber membrane. The theoretical calculation indicates that the single Cu‒N₄ sites can modulate the electronic configuration of Fe clusters to reduce O₂* protonation reaction free energy, which ultimately enhances the electrocatalytic performance. Particularly, the Cu‒N₄ sites can increase the overlaps between the d orbitals of Fe and p orbitals of O to accelerate O‒O cleavage in OOH*. As a result, this unique atomic catalyst exhibits a half potential (E1/2) of 0.944 V in an alkaline medium exceeding that of commercial Pt/C, whereas acidic performance E1/2 = 0.815 V is comparable to Pt/C. This work shows the great potential of single atoms for improvements in atomic cluster catalysts.

Keywords: Hierarchical porous fibers, atomic Fe clusters, Cu single atoms, oxygen reduction reaction; O-O bond cleavage

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Authors: Albert Mufundirwa, Satoru Yoshioka, K. Ogi, Takeharu Sugiyama, George F. Harrington, Bretislav Smid, Benjamin Cunning, Kazunari Sasaki, Akari Hayashi, Stephen M. Lyth

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Polymer electrolyte membrane fuel cells (PEMFCs) are electrochemical energy conversion devices used for portable, residential and vehicular applications due to their low emissions, high efficiency, and quick start-up characteristics. However, PEMFCs generally use expensive, Pt-based electrocatalysts as electrode catalysts. Due to the high cost and limited availability of platinum, research and development to either drastically reduce platinum loading, or replace platinum with alternative catalysts is of paramount importance. A combination of high surface area supports and nano-structured active sites is essential for effective operation of catalysts. We synthesize carbon foam supports by thermal decomposition of sodium ethoxide, using a template-free, gram scale, cheap, and scalable pyrolysis method. This carbon foam has a high surface area, highly porous, three-dimensional framework which is ideal for electrochemical applications. These carbon foams can have surface area larger than 2500 m²/g, and electron microscopy reveals that they have micron-scale cells, separated by few-layer graphene-like carbon walls. We applied this carbon foam as a platinum catalyst support, resulting in the improved electrochemical surface area and mass activity for the oxygen reduction reaction (ORR), compared to carbon black. Similarly, silver-decorated carbon foams showed higher activity and efficiency for electrochemical carbon dioxide conversion than silver-decorated carbon black. A promising alternative to Pt-catalysts for the ORR is iron-impregnated nitrogen-doped carbon catalysts (Fe-N-C). Doping carbon with nitrogen alters the chemical structure and modulates the electronic properties, allowing a degree of control over the catalytic properties. We have adapted our synthesis method to produce nitrogen-doped carbon foams with large surface area, using triethanolamine as a nitrogen feedstock, in a novel bottom-up protocol. These foams are then infiltrated with iron acetate (FeAc) and pyrolysed to form Fe-N-C foams. The resulting Fe-N-C foam catalysts have high initial activity (half-wave potential of 0.68 VRHE), comparable to that of commercially available Pt-free catalysts (e.g., NPC-2000, Pajarito Powder) in acid solution. In alkaline solution, the Fe-N-C carbon foam catalysts have a half-wave potential of 0.89 VRHE, which is higher than that of NPC-2000 by almost 10 mVRHE, and far out-performing platinum. However, the durability is still a problem at present. The lessons learned from X-ray absorption spectroscopy (XAS), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and electrochemical measurements will be used to carefully design Fe-N-C catalysts for higher performance PEMFCs.

Keywords: carbon-foam, polymer electrolyte membrane fuel cells, platinum, Pt-free, Fe-N-C, ORR

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Authors: Dinesh Kumar Sharma, Sanjay Sharma

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Textile manufacturing industry uses a substantial amount of chemicals not only in the production processes but also in manufacturing the raw materials. Dyes are the most significant raw material which provides colour to the fabric and yarn. Dyes are produced by using a large amount of chemicals both organic and inorganic in nature. Dyes are further classified as Reactive or Vat Dyes which are mostly used in cotton textiles. In the process of application of dyes to the cotton fiber, yarn or fabric, several auxiliary chemicals are also used in the solution called dyebath to improve the absorption of dyes. There is a very little absorption of dyes and auxiliary chemicals and a residual amount of all these substances is released as the spent dye bath effluent. Because of the wide variety of chemicals used in cotton textile dyes, there is always a risk of harmful effects which may not be apparent immediately but may have an irreversible impact in the long term. Colour imparted by the dyes to the water also has an adverse effect on its public acceptability and the potability. This study has been conducted with an objective to assess the feasibility of reuse of the spent dye bath. Studies have been conducted in two independent industries manufacturing dyed cotton yarn and dyed cotton fabric respectively. These have been referred as Unit-I and Unit-II. The studies included assessment of reduction in pollution levels and the economic benefits of such reuse. The study conclusively establishes that the reuse of spent dyebath results in prevention of pollution, reduction in pollution loads and cost of effluent treatment & production. This pollution prevention technique presents a good preposition for pollution prevention in cotton textile industry.

Keywords: dyes, dyebath, reuse, toxic, pollution, costs

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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: Victor Chinecherem Ejeke, Raphael Eze Nnam

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The main objective of this research is to produce biodiesel from waste vegetable oil using activated eggshell waste as solid catalysts. A transesterification reaction was performed for the conversion to biodiesel. Waste eggshells were calcined at 700°C, 800°C and 900°C for a time period of 3hrs for the preparation of the renewable catalyst. The calcined waste eggshell catalyst was characterized using X-Ray Florescence (XRF) Spectroscopy, which revealed CaO as the major constituent (90.86%); this was further confirmed by X-Ray Diffraction (XRD) and Fourier Transform Infrared (FTIR) analyses. The prepared catalyst was used for transesterification reaction and the effects of calcination temperature (700 to 900°C), Deep Eutectic Solvent DES loading (3 to 18 wt. %), Waste Egg Shell (WES) catalyst loading (6 to 14 wt. %) on the conversion to biodiesel were studied. The yield of biodiesel using a waste eggshell catalyst (91%) is comparable to conventional catalyst like sodium hydroxide with a yield of 80-90%. The maximum biodiesel production yield was obtained at a specific oil-to methanol molar ratio of 1:10, a temperature of 65°C and a catalyst loading of 14g-wt%. The biodiesel produced was characterized as being composed of methyl Tetradecanoate (C₁₄H₂₈O₂) 30.92% using the Gas Chromatographic (GC-MS) analysis. The fuel properties of the biodiesel (Flashpoint 138ᵒC) were comparable to commercial diesel, and hence it can be used in compression-ignition engines. The results indicated that the catalysts derived from waste eggshell had high potential to be used as biodiesel production catalysts in transesterification of waste vegetable oil with the advantage of reusability and also not requiring water washing steps.

Keywords: waste vegetable oil, catalyst , biodiesel , waste egg shell

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Authors: Patrizia Frontera, Anastasia Macario, Sebastiano Candamano, Fortunato Crea, Pierluigi Antonucci

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The increasing of the world energy demand makes today biomass an attractive energy source, based on the minimizing of CO2 emission and on the global warming reduction purposes. Recently, COP-21, the international meeting on global climate change, defined the roadmap for sustainable worldwide development, based on low-carbon containing fuel. Hydrogen is an energy vector able to substitute the conventional fuels from petroleum. Ethanol for hydrogen production represents a valid alternative to the fossil sources due to its low toxicity, low production costs, high biodegradability, high H2 content and renewability. Ethanol conversion to generate hydrogen by a combination of partial oxidation and steam reforming reactions is generally called auto-thermal reforming (ATR). The ATR process is advantageous due to the low energy requirements and to the reduced carbonaceous deposits formation. Catalyst plays a pivotal role in the ATR process, especially towards the process selectivity and the carbonaceous deposits formation. Bimetallic or trimetallic catalysts, as well as catalysts with doped-promoters supports, may exhibit high activity, selectivity and deactivation resistance with respect to the corresponding monometallic ones. In this work, NiMoCo/GDC, NiMoCu/GDC and NiMoRe/GDC (where GDC is Gadolinia Doped Ceria support and the metal composition is 60:30:10 for all catalyst) have been prepared by impregnation method. The support, Gadolinia 0.2 Doped Ceria 0.8, was impregnated by metal precursors solubilized in aqueous ethanol solution (50%) at room temperature for 6 hours. After this, the catalysts were dried at 100°C for 8 hours and, subsequently, calcined at 600°C in order to have the metal oxides. Finally, active catalysts were obtained by reduction procedure (H2 atmosphere at 500°C for 6 hours). All sample were characterized by different analytical techniques (XRD, SEM-EDX, XPS, CHNS, H2-TPR and Raman Spectorscopy). Catalytic experiments (auto-thermal reforming of ethanol) were carried out in the temperature range 500-800°C under atmospheric pressure, using a continuous fixed-bed microreactor. Effluent gases from the reactor were analyzed by two Varian CP4900 chromarographs with a TCD detector. The analytical investigation focused on the preventing of the coke deposition, the metals sintering effect and the sulfur poisoning. Hydrogen productivity, ethanol conversion and products distribution were measured and analyzed. At 600°C, all tri-metallic catalysts show the best performance: H2 + CO reaching almost the 77 vol.% in the final gases. While NiMoCo/GDC catalyst shows the best selectivity to hydrogen whit respect to the other tri-metallic catalysts (41 vol.% at 600°C). On the other hand, NiMoCu/GDC and NiMoRe/GDC demonstrated high sulfur poisoning resistance (up to 200 cc/min) with respect to the NiMoCo/GDC catalyst. The correlation among catalytic results and surface properties of the catalysts will be discussed.

Keywords: catalysts, ceria, ethanol, gadolinia, hydrogen, Nickel

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Authors: Ainouna Bouziane

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The ability of Electron Tomography to recover the 3D structure of catalysts, with spatial resolution in the subnanometer scale, has been widely explored and reviewed in the last decades. A variety of experimental techniques, based either on Transmission Electron Microscopy (TEM) or Scanning Transmission Electron Microscopy (STEM) have been used to reveal different features of nanostructured catalysts in 3D, but High Angle Annular Dark Field imaging in STEM mode (HAADF-STEM) stands out as the most frequently used, given its chemical sensitivity and avoidance of imaging artifacts related to diffraction phenomena when dealing with crystalline materials. In this regard, our group has developed a methodology that combines image denoising by undecimated wavelet transforms (UWT) with automated, advanced segmentation procedures and parameter selection methods using CS-TVM (Compressed Sensing-total variation minimization) algorithms to reveal more reliable quantitative information out of the 3D characterization studies. However, evaluating the accuracy of the magnitudes estimated from the segmented volumes is also an important issue that has not been properly addressed yet, because a perfectly known reference is needed. The problem particularly complicates in the case of multicomponent material systems. To tackle this key question, we have developed a methodology that incorporates volume reconstruction/segmentation methods. In particular, we have established an approach to evaluate, in quantitative terms, the accuracy of TVM reconstructions, which considers the influence of relevant experimental parameters like the range of tilt angles, image noise level or object orientation. The approach is based on the analysis of material-realistic, 3D phantoms, which include the most relevant features of the system under analysis.

Keywords: electron tomography, supported catalysts, nanometrology, error assessment

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Authors: Abdulrahman M. Alhowikan, Nadra E. Elamin, Sarah S. Aldayel, Sara A. AlSiddiqi, Fai S. Alrowais, Laila Y. Al-Ayadhi

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Background: A growing body of research has suggested that physical activities (PA) have important implications for improving the performance of ASD children. They revealed that the physiological, cognitive, psychological, and behavioral functioning had improved after performing some physical activities. Methods: We compared the sedentary behavior and physical activities between children with autism spectrum disorder (n=21) and age-matched control group (n=30), using the ActiGraph GT3X+ for the assessments. Results: Our results revealed that the total time spent in sedentary activity and the total sedentary activity counts were highly significant in the control group compared to the ASD group (p < 0.001, p=0.001, respectively). ASD spent a significantly longer time than the controls engaging on vigorous physical activity (VPA) (p=0.017). The results also indicated that there were no significant differences between both groups for the total counts and time spent in light physical activity (LPA) and moderate physical activity (MPA). Conclusion: The finding highlights the importance of physical activity intervention for ASD children, using accurate and precise measurement tools to record all activities.

Keywords: Autism spectrum disorders, motor skills, physical activity, ActiGraph GT3X+, moderate-to vigorous-intensity physical activity

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

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

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

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Authors: Mohamed Rashad, Mohamed Hafez, Mohamed Emran, Emad Aboukila, Ibrahim Nassar

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Environment-friendly organic wastes of Brewers' spent grain, a byproduct of the brewing process, have recently used as soil amendment to improve soil fertility and plant production. In this work, treatments of 1% (T1) and 2% (T2) of spent grains, 1% (C1) and 2% (C2) of compost and mix of both sources (C1T1) were used and compared to the control for growing Zea mays L. on sandy soil under arid Mediterranean climate. Soils were previously incubated at 65% saturation capacity for a month. The most relevant soil physical and chemical parameters were analysed. Water holding capacity and soil organic matter (OM) increased significantly along the treatments with the highest values in T2. Soil pH decreased along the treatments and the lowest pH was in C1T1. Bicarbonate decreased by 69% in C1T1 comparing to control. Total nitrogen (TN) and available P varied significantly among all treatments and T2, C1T1 and C2 treatments increased 25, 17 and 11 folds in TN and 1.2, 0.6 and 0.3 folds in P, respectively related to control. Available K showed the highest values in C1T1. Soil micronutrients increased significantly along all treatments with the highest values in T2. After corn germination, significant variation was observed in the velocity of germination coefficients (VGC) among all treatments in the order of C1T1>T2>T1>C2>C1>control. The highest records of final germination and germination index were in C1T1 and T2. The spent grains may compensate deficiencies of macro and micronutrients in newly reclaimed sandy soils without adverse effects to sustain crop production with a rider that excessive or continuous use need to be circumvented.

Keywords: corn and squash germination, environmentally friendly organic wastes, soil carbon sequestration, spent grains as soil amendment, water holding capacity

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Authors: N. Laosiripojana, P. Tepamatr

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The influence of bismuth on the water gas shift activities of Pt on ceria was studied. The flow reactor was used to study the activity of the catalysts in temperature range 100-400°C. The feed gas composition contains 5%CO, 10% H₂O and balance N₂. The total flow rate was 100 mL/min. The outlet gas was analyzed by on-line gas chromatography with thermal conductivity detector. The catalytic activities of bimetallic 1%Pt1%Bi/CeO₂ catalyst were greatly enhanced when compared with the activities of monometallic 2%Pt/CeO₂ catalyst. The catalysts were characterized by X-ray diffraction (XRD), Temperature-Programmed Reduction (TPR) and surface area analysis. X-ray diffraction pattern of Pt/CeO₂ and PtBi/CeO₂ indicated slightly shift of diffraction angle when compared with pure ceria. This result was due to strong metal-support interaction between platinum and ceria solid solution, causing conversion of Ce⁴⁺ to larger Ce³⁺. The distortions inside ceria lattice structure generated strain into the oxide lattice and facilitated the formation of oxygen vacancies which help to increase water gas shift performance. The H₂-Temperature Programmed Reduction indicated that the reduction peak of surface oxygen of 1%Pt1%Bi/CeO₂ shifts to lower temperature than that of 2%Pt/CeO₂ causing the enhancement of the water gas shift activity of this catalyst. Pt played an important role in catalyzing the surface reduction of ceria and addition of Bi alter the reduction temperature of surface ceria resulting in the improvement of the water gas shift activity of Pt catalyst.

Keywords: bismuth, platinum, water gas shift, ceria

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Authors: Y. Chiang, J. R. Wang, J. H. Yang, Y. S. Tseng, C. Shih, S. W. Chen

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Kuosheng nuclear power plant (NPP) is a BWR/6 plant in Taiwan. There is more concern for the safety of Spent Fuel Pools (SFPs) in Taiwan after Fukushima event. In order to estimate the safety of Kuosheng NPP SFP, by using MELCOR2.1 and SNAP, the safety analysis of Kuosheng NPP SFP was performed combined with the mitigation strategy of NEI 06-12 report. There were several steps in this research. First, the Kuosheng NPP SFP models were established by MELCOR2.1/SNAP. Second, the Station Blackout (SBO) analysis of Kuosheng SFP was done by TRACE and MELCOR under the cooling system failure condition. The results showed that the calculations of MELCOR and TRACE were very similar in this case. Second, the mitigation strategy analysis was done with the MELCOR model by following the NEI 06-12 report. The results showed the effectiveness of NEI 06-12 strategy in Kuosheng NPP SFP. Finally, a sensitivity study of SFP quenching was done to check the differences of different water injection time and the phenomena during the quenching. The results showed that if the cladding temperature was over 1600 K, the water injection may have chance to cause the accident more severe with more hydrogen generation. It was because of the oxidation heat and the “Breakaway” effect of the zirconium-water reaction. An animation model built by SNAP was also shown in this study.

Keywords: MELCOR, SNAP, spent fuel pool, quenching

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Authors: Elvis Medina, Alejandro Karelovic, Romel Jiménez

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Catalytic ammonia decomposition represents an attractive alternative due to its high H₂ content (17.8% w/w), a product stream free of COₓ, among others; however, challenges need to be addressed for its consolidation as an H₂ chemical storage technology, especially, those focused on the synthesis of efficient bimetallic catalytic systems, as an alternative to the price and scarcity of ruthenium, the most active catalyst reported. In this sense, from the perspective of rational catalyst design, adjusting the main catalytic activity descriptor, a screening of supported catalysts with different compositional settings of cobalt-molybdenum metals is presented to evaluate their effect on the catalytic decomposition rate of ammonia. Subsequently, a kinetic study on the supported monometallic Co and Mo catalysts, as well as on the bimetallic CoMo catalyst with the highest activity is shown. The synthesis of catalysts supported on γ-alumina was carried out using the Charge Enhanced Dry Impregnation (CEDI) method, all with a 5% w/w loading metal. Seeking to maintain uniform dispersion, the catalysts were oxidized and activated (In-situ activation) using a flow of anhydrous air and hydrogen, respectively, under the same conditions: 40 ml min⁻¹ and 5 °C min⁻¹ from room temperature to 600 °C. Catalytic tests were carried out in a fixed-bed reactor, confirming the absence of transport limitations, as well as an Approach to equilibrium (< 1 x 10⁻⁴). The reaction rate on all catalysts was measured between 400 and 500 ºC at 53.09 kPa NH3. The synergy theoretically (DFT) reported for bimetallic catalysts was confirmed experimentally. Specifically, it was observed that the catalyst composed mainly of 75 mol% cobalt proved to be the most active in the experiments, followed by the monometallic cobalt and molybdenum catalysts, in this order of activity as referred to in the literature. A kinetic study was performed at 10.13 – 101.32 kPa NH3 and at four equidistant temperatures between 437 and 475 °C the data were adjusted to an LHHW-type model, which considered the desorption of nitrogen atoms from the active phase surface as the rate determining step (RDS). The regression analysis were carried out under an integral regime, using a minimization algorithm based on SLSQP. The physical meaning of the parameters adjusted in the kinetic model, such as the RDS rate constant (k₅) and the lumped adsorption constant of the quasi-equilibrated steps (α) was confirmed through their Arrhenius and Van't Hoff-type behavior (R² > 0.98), respectively. From an energetic perspective, the activation energy for cobalt, cobalt-molybdenum, and molybdenum was 115.2, 106.8, and 177.5 kJ mol⁻¹, respectively. With this evidence and considering the volcano shape described by the ammonia decomposition rate in relation to the metal composition ratio, the synergistic behavior of the system is clearly observed. However, since characterizations by XRD and TEM were inconclusive, the formation of intermetallic compounds should be still verified using HRTEM-EDS. From this point onwards, our objective is to incorporate parameters into the kinetic expressions that consider both compositional and structural elements and explore how these can maximize or influence H₂ production.

Keywords: CEDI, hydrogen carrier, LHHW, RDS

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Authors: Gabor Varga, Krisztina Karadi, Zoltan Konya, Akos Kukovecz, Pal Sipos, Istvan Palinko

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Nickel can efficiently replace palladium in the Heck, Suzuki and Negishi reactions. This study focuses on the synthesis and catalytic application of Ni(II)-containing layered double hydroxides (LDHs) and layered triple hydroxides (LTHs). Our goals were to incorporate Ni(II) ions among the layers of LDHs or LTHs, or binding it to their surface or building it into their layers in such a way that their catalytic activities are maintained or even increased. The LDHs and LTHs were prepared by the co-precipitation method using ethylene glycol as co-solvent. In several cases, post-synthetic modifications (e.g., thermal treatment) were performed. After optimizing the synthesis conditions, the composites displayed good crystallinity and were free of byproducts. The success of the syntheses and the post-synthetic modifications was confirmed by relevant characterization methods (XRD, SEM, SEM-EDX and combined IR techniques). Catalytic activities of the produced and well-characterized solids were investigated through the Heck reaction. The composites behaved as efficient, recyclable catalysts in the Heck reaction between 4-bromoanisole and styrene. Through varying the reaction parameters, we were able to obtain acceptable conversions under mild conditions. Our study highlights the possibility of the application of Ni(II)-containing composites as efficient catalysts in coupling reactions.

Keywords: layered double hydroxide, layered triple hydroxide, heterogeneous catalysis, heck reaction

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Authors: William Marquis, Fang Dong

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There has been a growing concern in recent years over the economic and social effects of adult video gaming. It has been estimated that the number of people who played video games during the COVID-19 pandemic is close to three billion, and there is evidence that this form of entertainment is here to stay. Many people are concerned that this growing use of time could crowd out time that could be spent on alternative forms of entertainment with family, friends, sports, and other social activities that build community. For example, recent studies of children suggest that playing videogames crowds out time that could be spent on homework, watching TV, or in other social activities. Similar studies of adults have shown that video gaming is negatively associated with earnings, time spent at work, and socializing with others. The primary objective of this paper is to examine how time adults spend on video gaming could displace time they could spend working and on activities that enhance their health and well-being. We use data from the American Time Use Survey (ATUS), maintained by the Bureau of Labor Statistics, to analyze the effects of time-use decisions on three measures of well-being. We pool the ATUS Well-being Module for multiple years, 2010, 2012, 2013, and 2021, along with the ATUS Activity and Who files for these years. This pooled data set provides three broad measures of well-being, e.g., health, life satisfaction, and emotional well-being. Seven variants of each are used as a dependent variable in different multivariate regressions. We add to the existing literature in the following ways. First, we investigate whether the time adults spend in video gaming crowds out time spent working or in social activities that promote health and life satisfaction. Second, we investigate the relationship between adult gaming and their emotional well-being, also known as negative or positive affect, a factor that is related to depression, health, and labor market productivity. The results of this study suggest that the time adult gamers spend on video gaming has no effect on their supply of labor, a negligible effect on their time spent socializing and studying, and mixed effects on their emotional well-being, such as increasing feelings of pain and reducing feelings of happiness and stress.

Keywords: online gaming, health, social capital, emotional wellbeing

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Authors: Hossein Bayahia, Mohammed Saad Motlaq Al-Gahmdi

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The gas-phase deoxygenation of propionic acid was investigated in the presence of Co-Mo catalysts in N2 or H2 flow at 200-400 °C. In the presence of N2 the main product was 3-pentanone with other deoxygenates and some light gases: ethane and ethene. Using H2 flow, the catalyst was active for decarboxylation and decarbonylation of acid and the yields of ethane and ethene. The decarboxylation and decarbonylation reactions increased with increasing temperature. Cobalt-molybdenum supported on alumina showed better performance than bulk catalyst, especially at 400 °C in the presence of N2 for the ketonisation of propionic acid to form 3-pentanone as the main product. Bulk and supported catalysts were characterized by surface area porosity (BET), thermogravimetric analysis (TGA) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) of pyridine adsorption.

Keywords: deoxygenation, propionic acid, gas-phase, catalyst

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Authors: Sarra Boughaba

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α-aminophosphonates have found a wide range of applications in organic and medicinal chemistry; they are considered as pharmacological agents, anti-inflammatory antitumor agents, and antibiotics. A number of procedures have been developed for their synthesis. However, many of these methods suffer from some disadvantages such as long reaction times, environmental pollution, utilization of organic solvents, and expensive catalysts. In the past few years, heteropolyacids have received great attention as environmentally benign catalysts for organic synthetic processes, they possess unique physicochemical properties, such as super-acidity, high thermal and chemical stability, ability to accept and release electrons and high proton mobility, and the possibility of varying their acidity and oxidizing potential. In this context, an efficient and eco-friendly protocol has been described for the synthesis of α-aminophosphonates via one pot, three component reaction catalyzed by H₆P₂W₁₈O₆₂.14H₂O as reusable catalyst, by condensation of amino acids esters, various aromatic aldehydes and triethylphosphite under solvent-free conditions, the corresponding α-aminophosphonates were formed in good yields as racemic or diastereomericmixture. All the new products were systematically characterized by IR, MS, and ¹H, ¹³C-³¹P-NMR analyses. This method offers advantages such as simplicity workup with the green aspects by avoiding expensive catalysts and toxic solvents, good yields, short reaction times.

Keywords: amino acids esters, α-aminophosphonates, H₆P₂W₁₈O₆₂.14H₂O catalyst, green chemistry

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Authors: Bencharif Meriem, Sersar Ibrahim, Djaafri Zineb

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Introduction and purpose of the study: Education plays a fundamental role in the lives of young people, but what about their physical well-being as they spend long hours sitting at school? School inactivity is a problem that deserves particular attention because it can have significant repercussions on the health and development of students. The aim of this study was to describe and evaluate the physical activity of students in different practices in class, at recess and in the canteen. Material and methods: A physical activity diary and an anthropometric measurement sheet (weight, height) were provided to 123 school-aged adolescents. The measurements were carried out according to international recommendations. The statistical tests were carried out with the R software. 3.2.4. The significance threshold retained was 0.05. Results and Statistical Analysis: One hundred and twenty-three students agreed to participate in the study. Their average age was 16.5±1.60 years. Overweight was present in 8.13% and obesity in 4.06%. For the practice of physical activity, during physical education and sports classes, all students played sports with an average of 1.94±1.00 hours/week, of which 74.00% sweated or were out of breath during these hours of physical activity. It was also noted that boys practiced sports more than girls (p<0.0001). Each day, on average, students spent 39.78±37.85 min walking or running during recess. On the other hand, they spent, on average 4.25±2.65 hours sitting per day in class, at recess, in the canteen, etc., without counting the time spent in front of a screen. The increasing use of screens has become a major concern for parents and educators. On average, students spent approximately 42.90±38.41 min per day using screens in class, at recess, in the canteen and at home. (computer, tablet, telephone, video games, etc.) and therefore to a prolonged sedentary lifestyle. On average, students sat for more than 1.5 hours without moving for at least 2 minutes in a row approximately 1.72±0.71 times per day. Conclusion: These students spent many hours sitting at school. This prolonged inactivity can have negative consequences on their health, including problems with posture and cardiovascular health. It is crucial that schools, educators and parents collaborate to promote more active learning environments where students can move more and thus contribute to their overall well-being. It's time to rethink how we approach education and student health to give them a healthier, more active future.

Keywords: physical acivity, sedentarity, adolescents, school

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Authors: Marius Sebastian Secula, Mihaela Darie, Gabriela Carja

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Persistent organic pollutant discharged by various industries or urban regions into the aquatic ecosystems represent a serious threat to fauna and human health. The endocrine disrupting compounds are known to have toxic effects even at very low values of concentration. The anti-inflammatory agent Ibuprofen is an endocrine disrupting compound and is considered as model pollutant in the present study. The use of light energy to accomplish the latest requirements concerning wastewater discharge demands highly-performant and robust photo-catalysts. Many efforts have been paid to obtain efficient photo-responsive materials. Among the promising photo-catalysts, layered double hydroxides (LDHs) attracted significant consideration especially due to their composition flexibility, high surface area and tailored redox features. This work presents Fe(II) self-supported on ZnMeLDHs (Me =Al3+, Fe3+) as novel efficient photo-catalysts for Fenton-like catalysis. The co-precipitation method was used to prepare ZnAlLDH, ZnFeAlLDH and ZnCrLDH (Zn2+/Me3+ = 2 molar ratio). Fe(II) was self-supported on the LDHs matrices by using the reconstruction method, at two different values of weight concentration. X-ray diffraction (XRD), thermogravimetric analysis (TG/DTG), Fourier transform infrared (FTIR) and transmission electron microscopy (TEM) were used to investigate the structural, textural, and micromorphology of the catalysts. The Fe(II)/ZnMeLDHs nano-hybrids were tested for the degradation of a model pharmaceutical agent, the anti-inflammatory agent ibuprofen, by photocatalysis and photo-Fenton catalysis, respectively. The results point out that the embedment Fe(II) into ZnFeAlLDH and ZnCrLDH lead to a slight enhancement of ibuprofen degradation by light irradiation, whereas in case of ZnAlLDH, the degradation process is relatively low. A remarkable enhancement of ibuprofen degradation was found in the case of Fe(II)/ZnMeLDHs by photo-Fenton process. Acknowledgements: This work was supported by a grant of the Romanian National Authority for Scientific Research and Innovation, CNCS - UEFISCDI, project number PN-II-RU-TE-2014-4-0405.

Keywords: layered double hydroxide, heterogeneous Fenton, micropollutant, photocatalysis

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Authors: Nayana T. Nivangune, Vivek V. Ranade, Ashutosh A. Kelkar

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Organic carbamates are versatile compounds widely employed as pesticides, fungicides, herbicides, dyes, pharmaceuticals, cosmetics and in the synthesis of polyurethanes. Carbamates can be easily transformed into isocyanates by thermal cracking. Isocyantes are used as precursors for manufacturing agrochemicals, adhesives and polyurethane elastomers. Manufacture of polyurethane foams is a major application of aromatic ioscyanates and in 2007 the global consumption of polyurethane was about 12 million metric tons/year and the average annual growth rate was about 5%. Presently Isocyanates/carbamates are manufactured by phosgene based process. However, because of high toxicity of phoegene and formation of waste products in large quantity; there is a need to develop alternative and safer process for the synthesis of isocyanates/carbamates. Recently many alternative processes have been investigated and carbamate synthesis by methoxycarbonylation of aromatic amines using dimethyl carbonate (DMC) as a green reagent has emerged as promising alternative route. In this reaction methanol is formed as a by-product, which can be converted to DMC either by oxidative carbonylation of methanol or by reacting with urea. Thus, the route based on DMC has a potential to provide atom efficient and safer route for the synthesis of carbamates from DMC and amines. Lot of work is being carried out on the development of catalysts for this reaction and homogeneous zinc salts were found to be good catalysts for the reaction. However, catalyst/product separation is challenging with these catalysts. There are few reports on the use of supported Zn catalysts; however, deactivation of the catalyst is the major problem with these catalysts. We wish to report here methoxycarbonylation of aniline to methylphenylcarbamate (MPC) using amino acid complexes of Zn as highly active and selective catalysts. The catalysts were characterized by XRD, IR, solid state NMR and XPS analysis. Methoxycarbonylation of aniline was carried out at 170 °C using 2.5 wt% of the catalyst to achieve >98% conversion of aniline with 97-99% selectivity to MPC as the product. Formation of N-methylated products in small quantity (1-2%) was also observed. Optimization of the reaction conditions was carried out using zinc-proline complex as the catalyst. Selectivity was strongly dependent on the temperature and aniline:DMC ratio used. At lower aniline:DMC ratio and at higher temperature, selectivity to MPC decreased (85-89% respectively) with the formation of N-methylaniline (NMA), N-methyl methylphenylcarbamate (MMPC) and N,N-dimethyl aniline (NNDMA) as by-products. Best results (98% aniline conversion with 99% selectivity to MPC in 4 h) were observed at 170oC and aniline:DMC ratio of 1:20. Catalyst stability was verified by carrying out recycle experiment. Methoxycarbonylation preceded smoothly with various amine derivatives indicating versatility of the catalyst. The catalyst is inexpensive and can be easily prepared from zinc salt and naturally occurring amino acids. The results are important and provide environmentally benign route for MPC synthesis with high activity and selectivity.

Keywords: aniline, heterogeneous catalyst, methoxycarbonylation, methylphenyl carbamate

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Authors: Srinivas Nerella

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A series of new heterodentate N, O-donor ligands derived from condensing 3-amino Coumarins with hydroxy benzaldehydes and acetophenones were used to afford new mononuclear Mn(II), Co(II), Ni(II), Cu(II), Zn(II) and Pd(II) coordination compounds. All the complexes were characterized by IR, 1H-NMR, 13C-NMR, Mass, ESR, Electronic spectra, Conductance, Magnetic and Thermal studies. The ligands show hexa coordination in Mn(II), Co(II), Ni(II), and Pd(II) complexes resulting octahedral geometries, while the ligands in Zn(II) and Cu(II) complexes show tetra coordination resulting tetrahedral and square planar geometries respectively. These mononuclear complexes were investigated as catalysts in the hydrothiolation of aromatic and aliphatic alkynes with thiols. These metal complexes were acted as versatile catalysts and gave good yields.

Keywords: schiff bases, divalent metal complexes of schiff bases, Catalytic activity, hydrothiolation

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Authors: Maksudur Rahman Khan, Kar Min Chan, Huei Ruey Ong, Chin Kui Cheng, Wasikur Rahman

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Microbial fuel cells (MFCs) represent a promising technology for simultaneous bioelectricity generation and wastewater treatment. Catalysts are significant portions of the cost of microbial fuel cell cathodes. Many materials have been tested as aqueous cathodes, but air-cathodes are needed to avoid energy demands for water aeration. The sluggish oxygen reduction reaction (ORR) rate at air cathode necessitates efficient electrocatalyst such as carbon supported platinum catalyst (Pt/C) which is very costly. Manganese oxide (MnO2) was a representative metal oxide which has been studied as a promising alternative electrocatalyst for ORR and has been tested in air-cathode MFCs. However, the single MnO2 has poor electric conductivity and low stability. In the present work, the MnO2 catalyst has been modified by doping Pt nanoparticle. The goal of the work was to improve the performance of the MFC with minimum Pt loading. MnO2 and Pt nanoparticles were prepared by hydrothermal and sol-gel methods, respectively. Wet impregnation method was used to synthesize Pt/MnO2 catalyst. The catalysts were further used as cathode catalysts in air-cathode cubic MFCs, in which anaerobic sludge was inoculated as biocatalysts and palm oil mill effluent (POME) was used as the substrate in the anode chamber. The as-prepared Pt/MnO2 was characterized comprehensively through field emission scanning electron microscope (FESEM), X-Ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and cyclic voltammetry (CV) where its surface morphology, crystallinity, oxidation state and electrochemical activity were examined, respectively. XPS revealed Mn (IV) oxidation state and Pt (0) nanoparticle metal, indicating the presence of MnO2 and Pt. Morphology of Pt/MnO2 observed from FESEM shows that the doping of Pt did not cause change in needle-like shape of MnO2 which provides large contacting surface area. The electrochemical active area of the Pt/MnO2 catalysts has been increased from 276 to 617 m2/g with the increase in Pt loading from 0.2 to 0.8 wt%. The CV results in O2 saturated neutral Na2SO4 solution showed that MnO2 and Pt/MnO2 catalysts could catalyze ORR with different catalytic activities. MFC with Pt/MnO2 (0.4 wt% Pt) as air cathode catalyst generates a maximum power density of 165 mW/m3, which is higher than that of MFC with MnO2 catalyst (95 mW/m3). The open circuit voltage (OCV) of the MFC operated with MnO2 cathode gradually decreased during 14 days of operation, whereas the MFC with Pt/MnO2 cathode remained almost constant throughout the operation suggesting the higher stability of the Pt/MnO2 catalyst. Therefore, Pt/MnO2 with 0.4 wt% Pt successfully demonstrated as an efficient and low cost electrocatalyst for ORR in air cathode MFC with higher electrochemical activity, stability and hence enhanced performance.

Keywords: microbial fuel cell, oxygen reduction reaction, Pt/MnO2, palm oil mill effluent, polarization curve

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Authors: Abdullah S. Alghamdi, Khaled Alghamdi, Richard O. Jenkins, Parvez I. Haris

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Background: Physical activity is an important factor in the treatment and prevention of type 2 diabetes mellitus (T2DM). Reduction in HbA1c level, an important diabetes biomarker, was reported in patients who increased their daily physical activity. Although the ambient temperature was reported to be positively correlated to a negative impact on health and increase the incidences of diabetes, the exposure to bright sunlight was recently found to be associated with enhanced insulin sensitivity and improved beta-cell function. How Ramadan alters physical activity, and especially sunlight exposure, has not been adequately investigated. Aim: This study aimed to assess the physical activity and sun exposure of Saudis with T2DM over different periods (before, during, and after Ramadan) and related this to HbA1c levels. Methods: This study recruited 82 Saudis with T2DM, who chose to fast during Ramadan, from the Endocrine and Diabetic Centre of Al Iman General Hospital, Riyadh, Saudi Arabia. Ethical approvals for this study were obtained from De Montfort University and Saudi Ministry of Health. Physical activity and sun exposure were assessed by a self-administered questionnaire. Physical activity was estimated using the International Physical Activity Questionnaire (IPAQ), while the sun exposure was assessed by asking the patients about their hours per week of direct exposure to the sun, and daily hours spent outdoors. Blood samples were collected in each period for measuring HbA1c. Results: Low physical activity was observed in more than 60% of the patients, with no significant changes between periods. There were no significant variances between periods in the daily hours spent outdoors and the total number of weekly hours of direct exposure to the sun. The majority of patients reported only few hours of exposure to the sun (1h or less per week) and time spent outdoors (1h or less per day). The mean HbA1c significantly changed between periods (P = 0.001), with lowest level during Ramadan. There were significant differences in the mean HbA1c between the groups for the level of physical activity (P < 0.001), with significant lower mean HbA1c in the higher-level group. There were no significant variances in the mean of HbA1c between the groups for the daily hours spent outdoors. The mean HbA1c of the patients, who reported never in their total weekly hours of exposure to the sun, was significantly lower than the mean HbA1c of those who reported 1 hour or less (P = 0.001). Conclusion: Physical inactivity was prevalent among the study population with very little exposure to the sun or time spent outdoors. Higher level of physical activity was associated with lower mean HbA1c levels. Encouraging T2DM patients to achieve the recommended levels of physical activity may help them to obtain greater benefits of Ramadan fasting, such as reducing their HbA1c levels. The impact of low direct exposure to the sun and the time spent outdoors needs to be further investigated in both healthy and diabetic patients.

Keywords: diabetes, fasting, physical activity, sunlight, Ramadan

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Authors: O. P. Yadav

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Nano-size Ag-N co-doped ZnO/CuO composite photo-catalyst has been synthesized by chemical method and characterized using XRD, TEM, FTIR, AAS and UV-Vis spectroscopic techniques. Photo-catalytic activity of as-synthesized nanomaterial has been studied using degradation of methyl orange as a probe under UV as well as visible radiations. Ag-N co-doped ZnO/CuO composite showed higher photo-catalytic activity than Ag- or N-doped ZnO and undoped ZnO-CuO composite photo-catalysts. The observed highest activity of Ag-N co-doped ZnO-CuO among the studied photo-catalysts is attributed to the cumulative effects of lowering of band-gap energy and decrease of recombination rate of photo-generated electrons and holes owing to doped N and Ag, respectively. Effects of photo-catalyst load, pH and substrate initial concentration on degradation of methyl orange have also been studied. Photo-catalytic degradation of methyl orange follows pseudo first order kinetics.

Keywords: degradation, nanocomposite, photocatalyst, spectroscopy, XRD

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Authors: Esther Acha, Jose Cambra, De Chen

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Hydrogen is considered an important energy vector for the 21st century. Nowadays there are some difficulties for hydrogen economy implantation, and one of them is the high purity required for hydrogen. This energy vector is still being mainly produced from fuels, from wich hydrogen is produced as a component of a mixture containing other gases, such as CO, CO2 and H2O. A forthcoming sustainable pathway for hydrogen is steam-reforming of bio-oils derived from biomass, e.g. via fast pyrolysis. Bio-oils are a mixture of acids, alcohols, aldehydes, esters, ketones, sugars phenols, guaiacols, syringols, furans, multi-functional compounds and also up to a 30 wt% of water. The sorption enhanced steam reforming (SESR) process is attracting a great deal of attention due to the fact that it combines both hydrogen production and CO2 separation. In the SESR process, carbon dioxide is captured by an in situ sorbent, which shifts the reversible reforming and water gas shift reactions to the product side, beyond their conventional thermodynamic limits, giving rise to a higher hydrogen production and lower cost. The hydrogen containing mixture has been obtained from the SESR of bio-oil type compounds. Different types of catalysts have been tested. All of them contain Ni at around a 30 wt %. Two samples have been prepared with the wet impregnation technique over conventional (gamma alumina) and non-conventional (olivine) supports. And a third catalysts has been prepared over a hydrotalcite-like material (HT). The employed sorbent is a commercial dolomite. The activity tests were performed in a bench-scale plant (PID Eng&Tech), using a stainless steel fixed bed reactor. The catalysts were reduced in situ in the reactor, before the activity tests. The effluent stream was cooled down, thus condensed liquid was collected and weighed, and the gas phase was analysed online by a microGC. The hydrogen yield, and process behavior was analysed without the sorbent (the traditional SR where a second purification step will be needed but that operates in steady state) and the SESR (where the purification step could be avoided but that operates in batch state). The influence of the support type and preparation method will be observed in the produced hydrogen yield. Additionally, the stability of the catalysts is critical, due to the fact that in SESR process sorption-desorption steps are required. The produced hydrogen yield and hydrogen purity has to be high and also stable, even after several sorption-desorption cycles. The prepared catalysts were characterized employing different techniques to determine the physicochemical properties of the fresh-reduced and used (after the activity tests) materials. The characterization results, together with the activity results show the influence of the catalysts preparation method, calcination temperature, or can even explain the observed yield and conversion.

Keywords: CO2 sorbent, enhanced steam reforming, hydrogen

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Authors: Rajeev Ravindran, Amit K. Jaiswal

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Lignocellulose is the largest reservoir of inexpensive, renewable source of carbon. It is composed of lignin, cellulose and hemicellulose. Cellulose and hemicellulose is composed of reducing sugars glucose, xylose and several other monosaccharides which can be metabolised by microorganisms to produce several value added products such as biofuels, enzymes, aminoacids etc. Enzymatic treatment of lignocellulose leads to the release of monosaccharides such as glucose and xylose. However, factors such as the presence of lignin, crystalline cellulose, acetyl groups, pectin etc. contributes to recalcitrance restricting the effective enzymatic hydrolysis of cellulose and hemicellulose. In order to overcome these problems, pre-treatment of lignocellulose is generally carried out which essentially facilitate better degradation of lignocellulose. A range of pre-treatment strategy is commonly employed based on its mode of action viz. physical, chemical, biological and physico-chemical. However, existing pretreatment strategies result in lower sugar yield and formation of inhibitory compounds. In order to overcome these problems, we proposes a novel pre-treatment, which utilises the superior oxidising capacity of alkaline potassium permanganate assisted by ultra-sonication to break the covalent bonds in spent coffee waste to remove recalcitrant compounds such as lignin. The pre-treatment was conducted for 30 minutes using 2% (w/v) potassium permanganate at room temperature with solid to liquid ratio of 1:10. The pre-treated spent coffee waste (SCW) was subjected to enzymatic hydrolysis using enzymes cellulase and hemicellulase. Shake flask experiments were conducted with a working volume of 50mL buffer containing 1% substrate. The results showed that the novel pre-treatment strategy yielded 7 g/L of reducing sugar as compared to 3.71 g/L obtained from biomass that had undergone dilute acid hydrolysis after 24 hours. From the results obtained it is fairly certain that ultrasonication assists the oxidation of recalcitrant components in lignocellulose by potassium permanganate. Enzyme hydrolysis studies suggest that ultrasound assisted alkaline potassium permanganate pre-treatment is far superior over treatment by dilute acid. Furthermore, SEM, XRD and FTIR were carried out to analyse the effect of the new pre-treatment strategy on structure and crystallinity of pre-treated spent coffee wastes. This novel one-step pre-treatment strategy was implemented under mild conditions and exhibited high efficiency in the enzymatic hydrolysis of spent coffee waste. Further study and scale up is in progress in order to realise future industrial applications.

Keywords: spent coffee waste, alkaline potassium permanganate, ultra-sonication, physical characterisation

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Authors: Andrea Dragu, Solen Kinayyigit, Valerie Colliere, Karin Karin Philippot, Camelia Bala, Vasile I. Parvulescu

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The production of transportation fuels from biomass has gained a growing attention due to diminishing fossil fuel reserves, rising petroleum prices and increasing concern about global warming. In recent years, renewable hydrocarbons that are completely fungible with fossil fuels have been suggested to be efficiently produced by catalytic deoxygenation of fatty acids and their derivatives viadecarboxylation / decarbonylation. Several triglycerides (tall oil fatty acids) and saturated/unsaturated fatty acids and their corresponding esters were used as feedstocks. Their impact together with the influence of the reaction conditions and the catalyst composition on the nature of the reaction pathways of the deoxygenation of vegetable oils and their derivatives were recently reviewed. Following this state of the art the aim of the present study was the investigation of Pd NPs deposited onto mesoporous carbon supports as active and stable catalysts for the deoxygenation of oleic acid. The catalysts were prepared by the deposition of Pd NPs synthesised following an organometallic route on mesoporous carbons with different characteristics. Experiments were carried out under both batch and flow conditions. They demonstrated that under batch conditions (200 atm; 573K), the extent of the reaction depended, firstly, on the Pd loading and then on the metal dispersion and the oxidation state of palladium, both influenced by the way the support has been treated before the NPs deposition and by the preparation/stabilization methodology of Pd NPs. No aromatic compounds were detected in the reaction products but octadecanol and octadecane were observed in large extents. Under flow conditions (4 atm; 573 K), the conversion of stearic acid was superior to that observed in batch conditions. The product mixture contained over 20% heptadecane. No octadecanol, octadecane, and aromatic compounds were detected. The maxima in performances are obtained after only 0.5 h. After that, the yields in heptadecane suffer from a severe decrease until 3h reaction time. However, at that time, stopping feeding the reactor with oleic acid and flushing the catalyst only with mesitylene recovered the activity and the selectivity of the catalysts. With the complete removal of H2, the analysis revealed the presence of heptadecene in high excess compared to heptadecane (almost 7 to 1), thus suggesting decarbonylation as the main route. ICP-OES measurements indicated no leaching of palladium and simple washing of catalysts with mesitylene allowed recycling without any change in conversion or product distribution. Noteworthy, mesitylene as solvent exhibited no effect in this reaction. In conclusion, this study demonstrates the feasibility of such catalysts for the green production of fuels from biomass.

Keywords: fuels from biomass, green catalyst, Pd nano-particles , recycble catalyst

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Authors: Faezeh Aghazadeh

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The catalytic activity of Pt/γ-Al₂O₃ and Pt-Fe/γ-Al₂O₃ catalysts was investigated to bring about the complete oxidation of 2-Propanol. Among them, Pt-Fe/γ-Al₂O₃ was found to be the most promising catalyst based on activity. The catalysts were characterized by (XRD), (SEM), (TEM) and ICP-AES techniques. Iron loadings on Pt/γ-Al₂O₃ had a great effect on catalytic activity, and Pt-Fe/γ-Al₂O₃ (1.75 wt% Fe) catalyst at calcination temperature 300°C was observed to be the most active, which might be contributed to the favorable synergetic effects between Pt and Fe, high activity and the well-dispersed bimetallic phase. The combustion of 2-Propanol in the vapor phase was carried out in a conventional flow U-shape glass reactor used in the differential mode at atmospheric pressure. 2-Propanol was analyzed by a gas chromatograph VARIAN 3800 CX equipped with an FID. As observed, better performance and activity were observed for Pt-Fe/Al₂O₃ bimetallic catalyst. These results indicate that the high dispersion on support gives a positive effect on catalytic activity.

Keywords: volatile organic compounds, bimetallic catalyst, catalytic activity, low temperature

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Authors: Abrar Hussain, Kuen-Song Lin, Sayed Maeen Badshah, Jamshid Hussain

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The conversion of CO₂ into versatile, useful compounds such as fuels and other chemicals remains a challenging frontier in research, demanding the innovation of increasingly effective catalysts. In the present work, a catalyst-incorporating zirconium (Zr) modification within CuO–ZnO–Al₂O₃ (CZA) was synthesized via a co-precipitation method to convert CO₂ into methanol. Furthermore, bio-HZSM-5 was used to promote methanol dehydration to produce dimethyl ether (DME). We prepared the porous hierarchy bio-HZSM-5 with remarkable pore connectivity by utilizing an economical loofah sponge and rice husks as biotemplates. The synthesized catalysts were characterized using Field Emission Scanning Electron Microscopy (FE-SEM), X–ray diffraction (XRD), N₂ adsorption (BET), temperature-programmed desorption (NH₃-TPD) and thermogravimetric analysis (TGA). The Zr addition improved the performance of the CZZA catalyst as a structural promoter, leading to increased DME selectivity and total carbon conversion by enhancing active sites, surface area, and the synergistic interfaces between CuO and ZnO. The presence of silicon in the biomass, notably from the loofah sponge (0.016 wt %) and rice husks (8.3 wt %), also performed a pivotal role in the preparation of bio-HZSM-5. Furthermore, contrasted to the CZZA/com-ZSM-5 catalyst, the integration of CZZA with bio-HZSM-5-L bifunctional catalyst achieved the highest DME yield (12.1 %), DME selectivity (58.6%), CO₂ conversion (22.5%) at 280 °C and 30 bar. The payback time for 5 and 10-tons per day (5 and10-TPD) DME formation using the catalytic process of CO₂ from petrochemical refinery plant waste gas emissions was 2.98 and 2.44 years, respectively.

Keywords: Cost assessment, Dimethyl ether, low-cost bio-HZSM-5, CZZA catalyst, CO₂ hydrogenation

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