Search results for: slurry reactor

Authors: J. R. Wang, H. T. Lin, H. C. Chen, C. Shih, S. W. Chen, S. C. Chiang, C. C. Liu

Abstract:

In this research, TRACE model of Chinshan BWR/4 nuclear power plant (NPP) has been developed for the simulation and analysis of ultimate response guideline (URG).The main actions of URG are the depressurization and low pressure water injection of reactor and containment venting. This research focuses to verify the URG efficiency under Fukushima-like conditions. TRACE analysis results show that the URG can keep the PCT below the criteria 1088.7 K under Fukushima-like conditions. It indicated that Chinshan NPP was safe.

Keywords: BWR, TRACE, safety analysis, URG.

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Authors: A. M. Hassanain, Nader M. A. Mohamed, M. Naguib Aly, Alya A. Badawi, M. A. Gaheen

Abstract:

The thermal, epithermal and fast fluxes were calculated for three irradiation channels at Egypt Second Research Reactor (ETRR-2) using CITVAP code. The validity of the calculations was verified by experimental measurements. There are some deviations between measurements and calculations. This is due to approximations in the calculation models used, homogenization of regions, condensation of energy groups and uncertainty in nuclear data used. Neutron flux data for the three irradiation channels are now available. This would enable predicting the irradiation conditions needed for future radioisotope production.

Keywords: ETRR-2, Neutron flux, Radioisotope production, CITVAP

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Authors: Jožef Ritonja

Abstract:

The biochemical industry is one of the most important modern industries. Biochemical reactors are crucial devices of the biochemical industry. The essential bioprocess carried out in bioreactors is the fermentation process. A thorough insight into the fermentation process and the knowledge how to control it are essential for effective use of bioreactors to produce high quality and quantitatively enough products. The development of the control system starts with the determination of a mathematical model that describes the steady state and dynamic properties of the controlled plant satisfactorily, and is suitable for the development of the control system. The paper analyses the fermentation process in bioreactors thoroughly, using existing mathematical models. Most existing mathematical models do not allow the design of a control system for controlling the fermentation process in batch bioreactors. Due to this, a mathematical model was developed and presented that allows the development of a control system for batch bioreactors. Based on the developed mathematical model, a control system was designed to ensure optimal response of the biochemical quantities in the fermentation process. Due to the time-varying and non-linear nature of the controlled plant, the conventional control system with a proportional-integral-differential controller with constant parameters does not provide the desired transient response. The improved adaptive control system was proposed to improve the dynamics of the fermentation. The use of the adaptive control is suggested because the parameters’ variations of the fermentation process are very slow. The developed control system was tested to produce dairy products in the laboratory bioreactor. A carbon dioxide concentration was chosen as the controlled variable. The carbon dioxide concentration correlates well with the other, for the quality of the fermentation process in significant quantities. The level of the carbon dioxide concentration gives important information about the fermentation process. The obtained results showed that the designed control system provides minimum error between reference and actual values of carbon dioxide concentration during a transient response and in a steady state. The recommended control system makes reference signal tracking much more efficient than the currently used conventional control systems which are based on linear control theory. The proposed control system represents a very effective solution for the improvement of the milk fermentation process.

Keywords: Bioprocess engineering, biochemical reactor, fermentation process, modeling, adaptive control.

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Authors: Shyam Kumar, Nannuri Srinivasulu, Ashok Khanna

Abstract:

Bubble columns have a variety of applications in absorption, bio-reactions, catalytic slurry reactions, and coal liquefaction; because they are simple to operate, provide good heat and mass transfer, having less operational cost. The use of Computational Fluid Dynamics (CFD) for bubble column becomes important, since it can describe the fluid hydrodynamics on both local and global scale. Euler- Euler two-phase fluid model has been used to simulate two-phase (air and water) transient up-flow in bubble column (15cm diameter) using FLUENT6.3. These simulations and experiments were operated over a range of superficial gas velocities in the bubbly flow and churn turbulent regime (1 to16 cm/s) at ambient conditions. Liquid velocity was varied from 0 to 16cm/s. The turbulence in the liquid phase is described using the standard k-ε model. The interactions between the two phases are described through drag coefficient formulations (Schiller Neumann). The objectives are to validate CFD simulations with experimental data, and to obtain grid-independent numerical solutions. Quantitatively good agreements are obtained between experimental data for hold-up and simulation values. Axial liquid velocity profiles and gas holdup profiles were also obtained for the simulation.

Keywords: Bubble column, Computational fluid dynamics, Gas holdup profile, k-ε model.

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Authors: J. Ritonja

Abstract:

The biochemical technology has been developing extremely fast since the middle of the last century. The main reason for such development represents a requirement for large production of high-quality biologically manufactured products such as pharmaceuticals, foods, and beverages. The impact of the biochemical industry on the world economy is enormous. The great importance of this industry also results in intensive development in scientific disciplines relevant to the development of biochemical technology. In addition to developments in the fields of biology and chemistry, which enable to understand complex biochemical processes, development in the field of control theory and applications is also very important. In the paper, the control for the biochemical reactor for the milk fermentation was studied. During the fermentation process, the biophysical quantities must be precisely controlled to obtain the high-quality product. To control these quantities, the bioreactor’s stirring drive and/or heating system can be used. Available commercial biochemical reactors are equipped with open loop or conventional linear closed loop control system. Due to the outstanding parameters variations and the partial nonlinearity of the biochemical process, the results obtained with these control systems are not satisfactory. To improve the fermentation process, the self-tuning adaptive control system was proposed. The use of the self-tuning adaptive control is suggested because the parameters’ variations of the studied biochemical process are very slow in most cases. To determine the linearized mathematical model of the fermentation process, the recursive least square identification method was used. Based on the obtained mathematical model the linear quadratic regulator was tuned. The parameters’ identification and the controller’s synthesis are executed on-line and adapt the controller’s parameters to the fermentation process’ dynamics during the operation. The use of the proposed combination represents the original solution for the control of the milk fermentation process. The purpose of the paper is to contribute to the progress of the control systems for the biochemical reactors. The proposed adaptive control system was tested thoroughly. From the obtained results it is obvious that the proposed adaptive control system assures much better following of the reference signal as a conventional linear control system with fixed control parameters.

Keywords: Adaptive control, biochemical reactor, linear quadratic regulator, recursive least square identification.

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Authors: Jian Huang, Weixin Qian, Haitao Zhang, Weiyong Ying

Abstract:

Cobalt-gadolinium catalyst for Fischer-Tropsch synthesis was prepared by impregnation method with commercial silica gel, and its texture properties were characterized by BET, XRD, and TPR. The catalytic performance of the catalyst was tested in a fixed bed reactor. The results showed that the addition of gadolinium to the cobalt catalyst might decrease the size of cobalt particles, and increased the dispersion of catalytic active cobalt phases. The carbon number distributions for the catalysts was calculated by ASF equation.

Keywords: Fischer-Tropsch synthesis, cobalt-based catalysts, gadolinium, carbon number distributions.

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Authors: Promise Sethembiso Ngema, Freeman Ntuli, Mohamed Belaid

Abstract:

The main objective of this study was to remove and recover Ni, Cu and Fe from a mixed metal system using sodium hypophosphite as a reducing agent and nickel powder as seeding material. The metal systems studied consisted of Ni-Cu, Ni-Fe and Ni-Cu-Fe solutions. A 5 L batch reactor was used to conduct experiments where 100 mg/l of each respective metal was used. It was found that the metals were reduced to their elemental form with removal efficiencies of over 80%. The removal efficiency decreased in the order Fe>Ni>Cu. The metal powder obtained contained between 97-99% Ni and was almost spherical and porous. Size enlargement by aggregation was the dominant particulate process.

Keywords: crystallization, electroless plating, heavy metal removal, wastewater treatment

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Authors: Ke Zhang, Fang Li, Haitao Zhang, Hongfang Ma, Weiyong Ying, Dingye Fang

Abstract:

Three alumina-supported Pt-Sn catalysts have been prepared by means of co-impregnation and characterized by XRD and N2 adsorption. The influence of catalyst composition and reaction conditions on the conversion and selectivity were investigated in the hydrogenation of acetic acid in an isothermal integral fixed bed reactor. The experiments were performed on the temperature interval 468-548 K, liquid hourly space velocity (LHSV) of 0.3-0.7h-1, pressures between 1.0 and 5.0Mpa. A good compromise of 0.75%Pt-1.5%Sn can act as an optimized acetic acid hydrogenation catalyst, and the conversion and selectivity can be tuned through the variation of reaction conditions.

Keywords: Acetic acid, hydrogenation, Pt-Sn catalysts, ethanol.

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Authors: M. Azadi, N. Tahouni, M. H. Panjeshahi

Abstract:

A techno-economic evaluation for efficient use of energy in a large scale industrial plant of methanol is carried out. This assessment is based on integration of a gas turbine with an existing plant of methanol in which the outlet gas products of exothermic reactor is expanded to power generation. Also, it is decided that methanol production rate is constant through addition of power generation system to the existing methanol plant. Having incorporated a gas turbine with the existing plant, the economic results showed total investment of MUSD 16.9, energy saving of 3.6 MUSD/yr with payback period of approximately 4.7 years.

Keywords: Energy saving, Gas turbine, Methanol, Power generation.

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Authors: J. Skrovan, A. Alfantazi, T. Troczynski

Abstract:

For relatively small particles of aluminum (<60 μm), a measurable percentage of the aluminum (>5%) is observed to corrode before passivation occurs at moderate temperatures (>50oC) in de-ionized water within one hour. Physical contact with alumina powder results in a significant increase in both the rate of corrosion and the extent of corrosion before passivation. Whereas the resulting release of hydrogen gas could be of commercial interest for portable hydrogen supply systems, the fundamental aspects of Al corrosion acceleration in presence of dispersed alumina particles are equally important. This paper investigates the effects of various amounts of alumina on the corrosion rate of aluminum powders in water and the effect of multiple additions of aluminum into a single reactor.

Keywords: Alumina, Aluminum, Corrosion, Hydrogen

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Authors: Rohit Gupta, Ruchika

Abstract:

In this paper, a PSO based fractional order PID (FOPID) controller is proposed for concentration control of an isothermal Continuous Stirred Tank Reactor (CSTR) problem. CSTR is used to carry out chemical reactions in industries, which possesses complex nonlinear dynamic characteristics. Particle Swarm Optimization algorithm technique, which is an evolutionary optimization technique based on the movement and intelligence of swarm is proposed for tuning of the controller for this system. Comparisons of proposed controller with conventional and fuzzy based controller illustrate the superiority of proposed PSO-FOPID controller.

Keywords: CSTR, Fractional Order PID Controller, Partical Swarm Optimization.

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Authors: Maria D. Nikolaki, Katerina N. Zerva, Constantine. J. Philippopoulos

Abstract:

The photochemical and photo-Fenton oxidation of 1,3-dichloro-2-propanol was performed in a batch reactor, at room temperature, using UV radiation, H2O2 as oxidant, and Fenton-s reagent. The effect of the oxidative agent-s initial concentration was investigated as well as the effect of the initial concentration of Fe(II) by following the target compound degradation, the total organic carbon removal and the chloride ion production. Also, from the kinetic analysis conducted and proposed reaction scheme it was deduced that the addition of Fe(II) significantly increases the production and the further oxidation of the chlorinated intermediates.

Keywords: 1, 3-dichloro-2-propanol, hydrogen peroxide, photo- Fenton, UV .

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Authors: P. Góes, J. Manzi

Abstract:

This paper focuses on the development of an energy efficiency index that will be applied to reactive systems, which is based in the First and Second Law of Thermodynamics, by giving particular consideration to the concept of maximum entropy. Among the requirements of such energy efficiency index, the practical feasibility must be essential. To illustrate the performance of the proposed index, such an index was used as decisive factor of evaluation for the optimization process of an industrial reactor. The results allow the conclusion to be drawn that the energy efficiency index applied to the reactive system is consistent because it extracts the information expected of an efficient indicator, and that it is useful as an analytical tool besides being feasible from a practical standpoint. Furthermore, it has proved to be much simpler to use than tools based on traditional methodologies.

Keywords: Energy efficiency, maximum entropy, reactive systems.

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Authors: H. Ganji, H. R. Mahdipoor, J. Ahmadpanah, H. Naderi

Abstract:

The modified Claus process is the major technology for the recovery of elemental sulfur from hydrogen sulfide. The chemical reactions that can occur in the reaction furnace are numerous and many byproducts such as carbon disulfide and carbon carbonyl sulfide are produced. These compounds can often contribute from 20 to 50% of the pollutants and therefore, should be hydrolyzed in the catalytic converter. The inlet temperature of the first catalytic reactor should be maintained over than 250 °C, to hydrolyze COS and CS2. In this paper, the various configurations for the first converter reheating of sulfur recovery unit are investigated. As a result, the performance of each method is presented for a typical clause unit. The results show that the hot gas method seems to be better than the other methods.

Keywords: Sulfur recovery unit, reaction converter.

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

Abstract:

In this study of ultimate response guideline (URG), Kuosheng BWR/6 nuclear power plant (NPP) TRACE model was established. The reactor depressurization, low pressure water injection, and containment venting are the main actions of URG. This research focuses to evaluate the efficiency of URG under Fukushima-like conditions. Additionally, the sensitivity study of URG was also performed in this research. The analysis results of TRACE present that URG can keep the peak cladding temperature (PCT) below 1088.7 K (the failure criteria) under Fukushima-like conditions. It implied that Kuosheng NPP was at the safe situation.

Keywords: BWR, TRACE, safety analysis, URG.

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Authors: Mohammad Rezaee, Mohammad Kazemeini, Ali Morad Rashidi, Moslem Fattahi

Abstract:

Selective oxidation of H2S to elemental sulfur in a fixed bed reactor over newly synthesized alumina nanocatalysts was physio-chemically investigated and results compared with a commercial Claus catalyst. Amongst these new materials, Al2O3- supported sodium oxide prepared with wet chemical technique and Al2O3 nanocatalyst prepared with spray pyrolysis method were the most active catalysts for selective oxidation of H2S to elemental sulfur. Other prepared nanocatalysts were quickly deactivated, mainly due to the interaction with H2S and conversion into sulfides.

Keywords: H2S, Claus process, Al2O3, Spray pyrolysis method, Wet chemical technique

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Authors: S. Forkapic, J. Nikolov, N. Todorovic, D. Mrdja, I. Bikit

Abstract:

Tritium activity concentration in Danube river water in Serbia has been determinate using a liquid scintillation counter Quantulus 1220. During December 2010, water samples were taken along the entire course of Danube through Serbia, from Hungarian- Serbian to Romanian-Serbian border. This investigation is very important because of the nearness of nuclear reactor Paks in Hungary. Sample preparation was performed by standard test method using Optiphase HiSafe 3 scintillation cocktail. We used a rapid method for the preparation of environmental samples, without electrolytic enrichment.

Keywords: detection limit, liquid scintillation counter, low-leveltritium analysis, monitoring.

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Authors: Ahmed Mahmoudi, Imen Mejri, Mohamed A. Abbassi, Ahmed Omri

Abstract:

A numerical study based on the Lattice Boltzmann Method (LBM) is proposed to solve one, two and three dimensional heat and mass transfer for isothermal carbonization of thick wood particles. To check the validity of the proposed model, computational results have been compared with the published data and a good agreement is obtained. Then, the model is used to study the effect of reactor temperature and thermal boundary conditions, on the evolution of the local temperature and the mass distributions of the wood particle during carbonization

Keywords: Lattice Boltzmann Method, pyrolysis conduction, carbonization, Heat and mass transfer.

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Authors: M.Rajasimman, S.Subathra

Abstract:

In this work, statistical experimental design was applied for the optimization of medium constituents for Gentamicin production by Micromsonospora echinospora subs pallida (MTCC 708) in a batch reactor and the results are compared with the ANN predicted values. By central composite design, 50 experiments are carried out for five test variables: Starch, Soya bean meal, K2HPO4, CaCO3 and FeSO4. The optimum condition was found to be: Starch (8.9,g/L), Soya bean meal (3.3 g/L), K2HPO4 (0.8 g/L), CaCO3 (4 g/L) and FeSO4 (0.03 g/L). At these optimized conditions, the yield of gentamicin was found to be 1020 mg/L. The R2 values were found to be 1 for ANN training set, 0.9953 for ANN test set, and 0.9286 for RSM.

Keywords: Gentamicin, optimization, Micromonospora echinospora, ANN, RSM

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Authors: A. K. Sayah, Sh. Hosseinabadi, M. Farazar

Abstract:

This study investigates CO2 mitigation by methanol synthesis from flue gas CO2 and H2 generation through water electrolysis. Electrolytic hydrogen generation is viable provided that the required electrical power is supplied from renewable energy resources; whereby power generation from renewable resources is yet commercial challenging. This approach contribute to zero-emission, moreover it produce oxygen which could be used as feedstock for chemical process. At ZPC, however, oxygen would be utilized through partial oxidation of methane in autothermal reactor (ATR); this makes ease the difficulties of O2 delivery and marketing. On the other hand, onboard hydrogen storage and consumption; in methanol plant; make the project economically more competitive.

Keywords: Biomass, CO2 abatement, flue gas recovery, renewable energy, sustainable development.

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Authors: M. Hossain, A. H. Khan, M. A. R. Sarkar

Abstract:

Primary containment structure is one of the five safety layers of a nuclear facility which is needed to be designed in such a manner that it can withstand the pressure and excessive radioactivity during accidental situations. It is also necessary to ensure minimization of cost with maximum possible safety in order to make the design economically feasible and attractive. This paper attempts to identify the optimum design conditions for primary containment structure considering both mechanical and radiation safety keeping the economic aspects in mind. This work takes advantage of commercial simulation software to identify the suitable conditions without the requirement of costly experiments. Generated data may be helpful for further studies.

Keywords: PWR, concrete containment, finite element approach, neutron attenuation, Von Mises Stress.

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Authors: Reihaneh Ahmadzadeh Ghavidel, Mehdi Ghiafeh Davoodi

Abstract:

The usefulness of weaning foods to meet the nutrient needs of children is well recognized, and most of them are precooked roller dried mixtures of cereal and/or legume flours which posses a high viscosity and bulk when reconstituted. The objective of this study was to formulate composite weaning foods using cereals, malted legumes and vegetable powders and analyze them for nutrients, functional properties and sensory attributes. Selected legumes (green gram and lentil) were germinated, dried and dehulled. Roasted wheat, rice, carrot powder and skim milk powder also were used. All the ingredients were mixed in different proportions to get four formulations, made into 30% slurry and dried in roller drier. The products were analyzed for proximate principles, mineral content, functional and sensory qualities. The results of analysis showed following range of constituents per 100g of formulations on dry weight basis, protein, 18.1-18.9 g ; fat, 0.78-1.36 g ; iron, 5.09-6.53 mg; calcium, 265-310 mg. The lowest water absorption capacity was in case of wheat green gram based and the highest was in rice lentil based sample. Overall sensory qualities of all foods were graded as “good" and “very good" with no significant differences. The results confirm that formulated weaning foods were nutritionally superior, functionally appropriate and organoleptically acceptable.

Keywords: malted legumes, weaning foods, nutrition, functional properties

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Authors: Tadashi Watanabe

Abstract:

The LSTF experiment simulating the SGTR accident at the Mihama Unit-2 reactor is analyzed using the RELAP5/MOD3.3 code. In the accident, and thus in the experiment, the ECC water was injected not only into the cold legs but into the upper plenum. Overall transients during the experiment such as pressures and fluid temperatures are simulated well by the code. The cold-leg fluid temperatures are shown to decrease if the upper plenum injection system is connected to the cold leg. It is found that the cold-leg fluid temperatures also decrease if the upper-plenum injection is not used and the cold-leg injection alone is actuated.

Keywords: SGTR, LSTF, RELAP5, ECCS.

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Authors: Abdulsalam I. Rafida

Abstract:

The main objective of this research was to investigate the biosorption capacity for biofilms of sulphate reducing bacteria (SRB) to remove heavy metals, such as Zn, Pb and Cd from rainwater using laboratory-scale reactors containing mixed support media. Evidence showed that biosorption had contributed to removal of heavy metals including Zn, Pb and Cd in presence of SRB and SRB were also found in the aqueous samples from reactors. However, the SRB and specific families (Desulfobacteriaceae and Desulfovibrionaceae) were found mainly in the biomass samples taken from all reactors at the end of the experiment. EDX-analysis of reactor solids at end of experiment showed that heavy metals Zn, Pb and Cd had also accumulated in these precipitates.

Keywords: Sulphate reducing bacteria (SRB), biosorption capacity.

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Authors: M. Bharath, Vasudevan Raghavan, B. V. S. S. S. Prasad, S. R. Chakravarthy

Abstract:

In this experimental study, effects of addition of rice husk on coal gasification in a bubbling fluidized bed gasifier, operating at atmospheric pressure with air as gasifying agent, are reported. Rice husks comprising of 6.5% and 13% by mass are added to coal. Results show that, when rice husk is added the methane yield increases from volumetric percentage of 0.56% (with no rice husk) to 2.77% (with 13% rice husk). CO and H₂ remain almost unchanged and CO₂ decreases with addition of rice husk. The calorific value of the synthetic gas is around 2.73 MJ/Nm³. All performance indices, such as cold gas efficiency and carbon conversion, increase with addition of rice husk.

Keywords: Bubbling fluidized bed reactor, coal gasification, calorific value, rice husk.

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Authors: Hong-fang Ma, Cong-yi He, Hai-tao Zhang, Wei-yong Ying, Ding-ye Fang

Abstract:

A Ni-based catalyst supported by γ-Al₂O₃ was prepared by impregnation method, and the catalyst was used in a low CO and CO₂ concentration methanation system. The effect of temperature, pressure and space velocity on the methanation reaction was investigated in an experimental fixed-bed reactor. The methanation reaction was operated at the conditions of 190-240°C, 3000-24000ml•g^-1•h^-1 and 1.5-3.5MPa. The results show that temperature and space velocity play important role on the reaction. With the increase of reaction temperature the CO and CO₂ conversion increase and the selectivity of CH₄ increase. And with the increase of the space velocity the conversion of CO and CO₂ and the selectivity of CH₄ decrease sharply.

Keywords: Coke oven gas, methanation, catalyst, fixed-bed.

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Authors: Liang Zhang, Hai-Tao Zhang, W ei-Yong Ying, Ding-Ye Fang

Abstract:

Dehydration of methanol to dimethyl ether (DME) over a commercial Al2O3 catalyst was studied in an isothermal integral fixed bed reactor. The experiments were performed on the temperature interval 513-613 K, liquid hourly space velocity (LHSV) of 0.9-2.1h-1, pressures between 0.1 and 1.0 MPa. The effect of different operation conditions on the dehydration of methanol was investigated in a laboratory scale experiment. A new intrinsic kinetics equation based on the mechanism of Langmuir-Hinshelwood dissociation adsorption was developed for the dehydration reaction by fitting the expressions to the experimental data. An activation energy of 67.21 kJ/mol was obtained for the catalyst with the best performance. Statistic test showed that this new intrinsic kinetics equation was acceptable.

Keywords: catalyst, dimethyl ether, intrinsic kinetics, methanol

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Authors: N. Zainol, J. Salihon, R. Abdul-Rahman

Abstract:

Factor analysis was applied to two stages biogas production from banana stem waste allowing a screening of the experimental variables second stage temperature (T), organic loading rates (OLR) and hydraulic retention times (HRT). Biogas production was found to be strongly influenced by all the above experimental variables. Results from factorial analysis have shown that all variables which were HRT, OLR and T have significant effect to biogas production. Increased in HRT and OLR could increased the biogas yield. The performance was tested under the conditions of various T (35oC-60oC), OLR (0.3 g TS/l.d–1.9 gTS/l.d), and HRT (3 d–15 d). Conditions for temperature, OLR and HRT in this study were based on the best range obtained from literature review.

Keywords: Biogas, factor analysis, banana stem waste

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Authors: B. R. Shen, J. R. Wang, J. H. Yang, S. W. Chen, C. Shih, Y. Chiang, Y. F. Chang, Y. H. Huang

Abstract:

In this research, TRACE code with the interface code-SNAP was used to simulate and analyze the SBO (station blackout) accident which occurred in Maanshan PWR (pressurized water reactor) nuclear power plant (NPP). There are four main steps in this research. First, the SBO accident data of Maanshan NPP were collected. Second, the TRACE/SNAP model of Maanshan NPP was established by using these data. Third, this TRACE/SNAP model was used to perform the simulation and analysis of SBO accident. Finally, the simulation and analysis of SBO with mitigation equipments was performed. The analysis results of TRACE are consistent with the data of Maanshan NPP. The mitigation equipments of Maanshan can maintain the safety of Maanshan in the SBO according to the TRACE predictions.

Keywords: PWR, TRACE, SBO, Maanshan.

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Authors: K. Mondal, S. Talapatra, M. Terrones, S. Pokhrel, C. Frizzel, B. Sumpter, V. Meunier, A. L. Elias

Abstract:

Worldwide energy independence is reliant on the ability to leverage locally available resources for fuel production. Recently, syngas produced through gasification of carbonaceous materials provided a gateway to a host of processes for the production of various chemicals including transportation fuels. The basis of the production of gasoline and diesel-like fuels is the Fischer Tropsch Synthesis (FTS) process: A catalyzed chemical reaction that converts a mixture of carbon monoxide (CO) and hydrogen (H₂) into long chain hydrocarbons. Until now, it has been argued that only transition metal catalysts (usually Co or Fe) are active toward the CO hydrogenation and subsequent chain growth in the presence of hydrogen. In this paper, we demonstrate that carbon nanotube (CNT) surfaces are also capable of hydro-deoxygenating CO and producing long chain hydrocarbons similar to that obtained through the FTS but with orders of magnitude higher conversion efficiencies than the present state-of-the-art FTS catalysts. We have used advanced experimental tools such as XPS and microscopy techniques to characterize CNTs and identify C-O functional groups as the active sites for the enhanced catalytic activity. Furthermore, we have conducted quantum Density Functional Theory (DFT) calculations to confirm that C-O groups (inherent on CNT surfaces) could indeed be catalytically active towards reduction of CO with H₂, and capable of sustaining chain growth. The DFT calculations have shown that the kinetically and thermodynamically feasible route for CO insertion and hydro-deoxygenation are different from that on transition metal catalysts. Experiments on a continuous flow tubular reactor with various nearly metal-free CNTs have been carried out and the products have been analyzed. CNTs functionalized by various methods were evaluated under different conditions. Reactor tests revealed that the hydrogen pre-treatment reduced the activity of the catalysts to negligible levels. Without the pretreatment, the activity for CO conversion as found to be 7 µmol CO/g CNT/s. The O-functionalized samples showed very activities greater than 85 µmol CO/g CNT/s with nearly 100% conversion. Analyses show that CO hydro-deoxygenation occurred at the C-O/O-H functional groups. It was found that while the products were similar to FT products, differences in selectivities were observed which, in turn, was a result of a different catalytic mechanism. These findings now open a new paradigm for CNT-based hydrogenation catalysts and constitute a defining point for obtaining clean, earth abundant, alternative fuels through the use of efficient and renewable catalyst.

Keywords: CNT, CO hydro-deoxygenation, DFT, liquid fuels, XPS, XTL.

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