Search results for: methane catalytic combustion

Authors: Doo Ki Lee, Kumaresh Selvakumar, Man Young Kim

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Catalytic combustion is an environmentally friendly technique to combust fuels in gas turbines. In this paper, the behavior of surface reaction rate on catalytic combustion is studied with respect to the heterogeneous oxidation of methane-air mixture in a catalytic reactor. Plug flow reactor (PFR), the simplified single catalytic channel assists in investigating the catalytic combustion phenomenon over the Pt catalyst by promoting the desired chemical reactions. The numerical simulation with multi-step elementary surface reactions is governed by the availability of free surface sites onto the catalytic surface and thereby, the catalytic combustion characteristics are demonstrated by examining the rate of the reaction for lean fuel mixture. Further, two different surface reaction mechanisms are adopted and compared for surface reaction rates to indicate the controlling heterogeneous reaction for better fuel conversion. The performance of platinum catalyst under heterogeneous reaction is analyzed under the same temperature condition, where the catalyst with the higher kinetic rate of reaction would have a maximum catalytic activity for enhanced methane catalytic combustion.

Keywords: catalytic combustion, heterogeneous reaction, plug flow reactor, surface reaction rate

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Authors: Kumaresh Selvakumar, Man Young Kim

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Catalytic combustor substantially reduces emission entailing fuel-air premixing at very low equivalence ratios. The catalytic combustion of natural gas has the potential to become sufficiently active at light off temperature by the convection of heat from the catalyst surface. Only one channel is selected to investigate both the gas and surface reactions in the catalyst bed because of the honeycomb structure of the catalytic combustor. The objective of the present study is to find the methane catalytic combustion behavior inside the catalytic combustor, where the gas phase kinetics is employed by homogeneous methane combustion and surface chemistry is described with the heterogeneous catalysis of the oxidation of methane on a platinum catalyst. The reaction of the premixed mixture in the catalytic regime improves flame stability with complete combustion for lower operating flame temperature. An overview of the flow behavior is presented inside the single channel catalytic combustor including the operation of catalytic combustion with various F/A ratios and premixed inlet temperature.

Keywords: catalytic combustor, equivalence ratios, flame temperature, heterogeneous catalysis, homogeneous combustion

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Authors: Silviya Todorova, Anton Naydenov, Ralitsa Velinova, Alexander Larin

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Catalytic combustion of methane has been extensively investigated for emission control and power generation during the last decades. The alumina-supported palladium catalyst is widely accepted as the most active catalysts for catalytic combustion of methane. The activity of Pd/Al₂O₃ decreases during the time on stream, especially underwater vapor. The following order of activity in the reaction of complete oxidation of methane was established: Co₃O₄> CuO>NiO> Mn₂O₃> Cr₂O₃. It may be expected that the combination between Pd and these oxides could lead to the promising catalysts in the reaction of complete methane. In the present work, we investigate the activity of Pd/Al₂O₃ catalysts promoted with other metal oxides (MOx; M= Ni, Co, Ce). The Pd-based catalysts modified by metal oxide were prepared by sequential impregnation of Al₂O₃ with aqueous solutions of Me(NO₃)₂.6H₂O and Pd(NO₃)₂H₂O. All samples were characterized by X-ray diffraction (XRD), temperature-programmed reduction (TPR), and X-ray photoelectron spectroscopy (XPS). An improvement of activity was observed after modification with different oxides. The results demonstrate that the Pd/Al₂O₃ catalysts modified with Co and Ce by impregnation with a common solution of respective salts, exhibit the most promising catalytic activity for methane oxidation. Most probably, the presence of Co₃O₄ and CeO₂ on catalytic surface increases surface oxygen and therefore leads to the better reactivity in methane combustion.

Keywords: methane combustion, palladium, Co-Ce, Ni-Ce

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Authors: Ahmed I. Osman, Jehad K. Abu-Dahrieh, Jillian M. Thompson, David W. Rooney

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Natural gas (the main constituent is Methane 95%) is considered as an alternative to petroleum for the production of synthetics fuels. Nowadays, methane combustion at low temperature has received much attention however; it is the most difficult hydrocarbon to be combusted. Co/Mo and (4:1 wt/wt) catalysts were prepared from a range of different precursors and used for the low temperature total methane oxidation (TMO). The catalysts were characterized by, XRD, BET and H2-TPR and tested under reaction temperatures of 250-400 °C with a GHSV= 36,000 mL g-1 h-1. It was found that the combustion temperature was dependent on the type of the precursor, and that those containing chloride led to catalysts with lower activity. The optimum catalyst was Co/Mo (4:1wt/wt) where greater than 20% methane conversion was observed at 250 °C. This catalyst showed a high degree of stability for TMO, showing no deactivation during 50 hours of time on stream.

Keywords: methane low temperature total oxidation, oxygen carrier, Co/Mo, Co/Mn

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Authors: Man Young Kim

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Catalytic combustion is generally accepted as an environmentally preferred alternative for the generation of heat and power from fossil fuels mainly due to its advantages related to the stable combustion under very lean conditions with low emissions of NOx, CO, and UHC at temperatures lower than those occurred in conventional flame combustion. Despite these advantages, the commercial application of catalytic combustion has been delayed because of complicated reaction processes and the difficulty in developing appropriate catalysts with the required stability and durability. To develop the catalytic combustors, detailed studies on the combustion characteristics of catalytic combustion should be conducted. To the end, in current research, quantitative studies on the combustion characteristics of the catalytic combustors, with a Pd-based catalyst for MCFC power generation systems, relying on numerical simulations have been conducted. In addition, data from experimental studies of variations in outlet temperatures and fuel conversion, taken after operating conditions have been used to validate the present numerical approach. After introducing the governing equations for mass, momentum, and energy equations as well as a description of catalytic combustion kinetics, the effects of the excess air ratio, space velocity, and inlet gas temperature on the catalytic combustion characteristics are extensively investigated. Quantitative comparisons are also conducted with previous experimental data. Finally, some concluding remarks are presented.

Keywords: catalytic combustion, methane, BOP, MCFC power generation system, inlet temperature, excess air ratio, space velocity

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Authors: Kumaresh Selvakumar, Man Young Kim

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In order to elaborate the main idea of investigating the flow physics inside the catalytic combustor, the characteristics of the catalytic surface reactions are analyzed by employing the CHEMKIN methodology with detailed gas and surface chemistries. The presence of a catalyst inside an engine enables complete combustion at lower temperatures which promotes desired chemical reactions. A single channel from the honeycomb monolith catalytic combustor is preferred to analyze the gas and surface reactions in the catalyst bed considering the fact that every channel in the honeycomb monolith behaves in similar fashion. The simplified approach with single catalyst channel using plug flow reactor can be used to predict the flow behavior inside the catalytic combustor. The hydrogen addition to the combustion reactants offers a way to light-off catalytic combustion of methane on platinum catalyst and aids to reduce the surface ignition temperature. Indeed, the hydrogen adsorption is higher on the uncovered Pt(s) surface sites because the sticking coefficient of hydrogen is larger than that of methane. The location of flame position in the catalyst bed is validated by igniting the methane fuel with the presence of hydrogen for corresponding multistep surface reactions.

Keywords: catalytic combustor, hydrogen adsorption, plug flow reactor, surface ignition temperature

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Authors: Kumaresh Selvakumar, Man Young Kim

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The presence of a catalyst inside an engine enables complete combustion at lower temperatures which promote desired chemical reactions. The objective of this work is to design and simulate a catalytic combustor by using CHEMKIN with detailed gas and surface chemistries. The simplified approach with single catalyst channel using plug flow reactor (PFR) can be used to predict reasonably well with the effect of various operating parameters such as the inlet temperature, velocity and fuel/air ratios. The numerical results are validated by comparing the surface chemistries in single channel catalytic combustor. The catalytic combustor operates at much lower temperature than the conventional combustor since lean-fuel mixture is used where the complete methane conversion is achieved. The coupling between gas and surface reactions in the catalyst bed is studied by investigating the commencement of flame ignition with respect to the surface site species.

Keywords: catalytic combustion, honeycomb monolith, plug flow reactor, surface reactions

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Authors: Deepti Mishra, Arindam Modak, K. K. Pant, Xiu Song Zhao

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The promotional effect of mixed ceria-zirconia oxides (CZO) over the Mo/HZSM-5 catalyst for methane dehydroaromatization (MDA) reaction was studied. The surface and structural properties of the synthesized catalyst were characterized using a range of spectroscopic and microscopic techniques, and the correlation between catalytic properties and its performance for MDA reaction is discussed. The impregnation of CZO solid solution on Mo/HZSM-5 was observed to give an excellent catalytic performance and improved benzene formation rate (4.5 μmol/gcat. s) as compared to the conventional Mo/HZSM-5 (3.1 μmol/gcat. s) catalyst. In addition, a significant reduction in coke formation was observed in the CZO-modified Mo/HZSM-5 catalyst. The prevailing comprehension for higher catalytic activity could be because of the redox properties of CZO deposited Mo/HZSM-5, which acts as a selective oxygen supplier and performs hydrogen combustion during the reaction, which is indirectly probed by O₂-TPD and H₂-TPR analysis. The selective hydrogen combustion prevents the over-oxidation of aromatic species formed during the reaction while the generated steam helps in reducing the amount of coke generated in the MDA reaction. Thus, the advantage of CZO incorporated Mo/HZSM-5 is manifested as it promotes the reaction equilibrium to shift towards the formation of benzene which is favourable for MDA reaction.

Keywords: Mo/HZSM-5, ceria-zirconia (CZO), in-situ combustion, methane dehydroaromatization

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Authors: Przemyslaw J. Jodlowski, Roman J. Jedrzejczyk, Damian K. Chlebda, Anna Dziedzicka, Lukasz Kuterasinski, Anna Gancarczyk, Maciej Sitarz

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The aim of this study was to obtain highly active catalysts based on non-noble metal oxides supported on zirconia prepared via a sonochemical method. In this study, the influence of the stabilizers addition during the preparation step was checked. The final catalysts were characterized by using such characterization methods as X-ray Diffraction (XRD), nitrogen adsorption, X-ray fluorescence (XRF), scanning electron microscopy (SEM) equipped with energy dispersive X-ray spectrometer (EDS), transmission electron microscopy (TEM) and µRaman. The proposed preparation method allowed to obtain uniformly dispersed metal-oxide nanoparticles at the support’s surface. The catalytic activity of prepared catalyst samples was measured in a methane combustion reaction. The activity of the catalysts prepared by the sonochemical method was considerably higher than their counterparts prepared by the incipient wetness method.

Keywords: methane catalytic combustion, nanoparticles, non-noble metals, sonochemistry

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Authors: Ts. Lazarova, V. Tumbalev, S. Atanacova-Vladimirova, G. Ivanov, A. Naydenov, D. Kovacheva

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Methane is a major Greenhouse Gas (GHG) that accounts for 14% of the world’s total amount of GHG emissions, originating mainly from agriculture, Coal mines, land fields, wastewater and oil and gas facilities. Nowadays the problem caused by the methane emissions has been a subject of an increased concern. One of the methods for neutralization of the methane emissions is it's complete catalytic oxidation. The efforts of the researchers are focused on the development of new types of catalysts and optimizing the existing catalytic systems in order to prevent the sintering of the palladium, providing at the same time a sufficient activity at temperatures below 500oC. The aim of the present work is to prepare mixed Cu-Ag-Pd oxide catalysts supported on alumina and to test them for methane complete catalytic oxidation. Cu-Ag-Pd/Al2O3 were prepared on a γ-Al2O3 (BET surface area = 220 m2/g) by the incipient wetness method using the corresponding metal nitrates (Cu:Ag = 90:10, Cu:Pd =97:3, Cu:Ag:Pd= 87:10:3) as precursors. A second set of samples were prepared with addition of urea to the metal nitrate solutions with the above mentioned ratios assuming increased dispersivity of the catalysts. The catalyst samples were dried at 100°C for 3 hours and calcined at 550°C for 30 minutes. Catalysts samples were characterized using X-ray diffraction (XRD), low temperature adsorption of nitrogen (BET) and scanning electron microscopy (SEM). The catalytic activity tests were carried out in a continuous flow type of reactor at atmospheric pressure. The effect of catalyst aging at 500 oC for 120 h on the methane combustion activity was also investigated. The results clearly indicate the synergetic effect of Ag and Pd on the catalytic activity.

Keywords: catalysts, XRD, BET, SEM, catalytic oxidation

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Authors: Yan Zeng, Hongfang Ma, Haitao Zhang, Weiyong Ying

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Ni-based catalysts with different amounts of Na as promoter from 2 to 6 wt % were prepared by solution combustion method. The catalytic activity was investigated in syngas methanation reaction. Carbon oxides conversion and methane selectivity are greatly influenced by sodium loading. Adding 2 wt% Na remarkably improves catalytic activity and long-term stability, attributed to its smaller mean NiO particle size, better distribution, and milder metal-support interaction. However, excess addition of Na results in deactivation distinctly due to the blockage of active sites.

Keywords: nickel catalysts, syngas methanation, sodium, solution combustion method

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Authors: Noor S. Nasri, Eric C. A. Tatt, Usman D. Hamza, Jibril Mohammed, Husna M. Zain

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Climate change has becoming a global environmental issue that may trigger irreversible changes in the environment with catastrophic consequences for human, animals and plants on our planet. Methane, carbon dioxide and nitrous oxide are the greenhouse gases (GHG) and as the main factor that significantly contributes to the global warming. Mainly carbon dioxide be produced and released to atmosphere by thermal industrial and power generation sectors. Methane is dominant component of natural gas releases significant of thermal heat, and the gaseous pollutants when homogeneous thermal combustion takes place at high temperature. Heterogeneous catalytic Combustion (HCC) principle is promising technologies towards environmental friendly energy production should be developed to ensure higher yields with lower pollutants gaseous emissions and perform complete combustion oxidation at moderate temperature condition as comparing to homogeneous high thermal combustion. Hence the principle has become a very interesting alternative total oxidation for the treatment of pollutants gaseous emission especially NOX product formation. Noble metals are dispersed on a support-porous HCC such as γ- Al2O3, TiO2 and ThO2 to increase thermal stability of catalyst and to increase to effectiveness of catalytic combustion. Support-porous HCC material to be selected based on factors of the surface area, porosity, thermal stability, thermal conductivity, reactivity with reactants or products, chemical stability, catalytic activity, and catalyst life. γ- Al2O3 with high catalytic activity and can last longer life of catalyst, is commonly used as the support for Pd catalyst at low temperatures. Sustainable and renewable support-material of bio-mass char was derived from agro-industrial waste material and used to compare with those the conventional support-porous material. The abundant of biomass wastes generated in palm oil industries is one potential source to convert the wastes into sustainable material as replacement of support material for catalysts. Objective of this study was to compare the kinetic rate of reaction the combustion of methane on Palladium (Pd) based catalyst with Al2O3 support and bio-char (Bc) support derived from shell kernel. The 2wt% Pd was prepared using incipient wetness impregnation method and the HCC performance was accomplished using tubular quartz reactor with gas mixture ratio of 3% methane and 97% air. Material characterization was determined using TGA, SEM, and BET surface area. The methane porous-HCC conversion was carried out by online gas analyzer connected to the reactor that performed porous-HCC. BET surface area for prepared 2 wt% Pd/Bc is smaller than prepared 2wt% Pd/ Al2O3 due to its low porosity between particles. The order of catalyst activity based on kinetic rate on reaction of catalysts in low temperature is prepared 2wt% Pd/Bc > calcined 2wt% Pd/ Al2O3 > prepared 2wt% Pd/ Al2O3 > calcined 2wt% Pd/Bc. Hence the usage of agro-industrial bio-mass waste material can enhance the sustainability principle.

Keywords: catalytic-combustion, environmental, support-bio-char material, sustainable and renewable material

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Authors: Liu Yinga, Bai Xingjiab

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The conventional way to exploit coalbed methane is to drop reservoirs pressure through drainage, which means that reducing pressure through water drainage for coalbed methane desorption. However, it has many limitations. In this paper, the recovery by conventional way is low, in order to exploit water-sensitive reservoir, combustion of coal seam is proposed to increase recovery ratio, and then theoretical feasibility is elaborated through four aspects: temperature, pressure, superficial area, competitive adsorption, then given an example of water sensitive reservoir, results can be obtained that recovery is effectively improved through combustion of coal seam. At the same time, the suitability and efficiency of combustion of coal seam determine that it can be widely applied.

Keywords: coalbed methane, drainage decompression, water-sensitive, combustion of coal seams, competitive adsorption

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Authors: Annapurna Basavaraju, Andreas Marn, Franz Heitmeir

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

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

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

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

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

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Authors: Sushil Kumar Saraswat, K. K. Pant

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Co metal supported on SiO2 and Al2O3 catalysts with a metal loading varied from 30 of 70 wt.% were evaluated for decomposition of methane to CO/CO2 free hydrogen and carbon nano materials. The catalytic runs were carried out from 550-800 oC under atmospheric pressure using fixed bed vertical flow reactor. The fresh and spent catalysts were characterized by BET surface area analyzer, TPR, XRD, SEM, TEM, and TG analysis. The data showed that 50% Co/Al2O3 catalyst exhibited remarkable higher activity and stability up to 10 h time-on-stream at 750 oC with respect to H2 production compared to rest of the catalysts. However, the catalytic activity and durability was greatly declined at a higher temperature. The main reason for the catalytic inhibition of Co containing SiO2 catalysts is the higher reduction temperature of Co2SiO4. TEM images illustrate that the carbon materials with various morphologies, carbon nanofibers (CNFs), helical-shaped CNFs, and branched CNFs depending on the catalyst composition and reaction temperature, were obtained. The TG data showed that a higher yield of MWCNTs was achieved over 50% Co/Al2O3 catalyst compared to other catalysts.

Keywords: carbon nanotubes, cobalt, hydrogen production, methane decomposition

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Authors: José Luis Lorenzo Bayona, Ljiljana Medic-Pejic, Isabel Amez Arenillas, Blanca Castells Somoza

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The communication presents the study results carried out by the Official Laboratory J. M. Madariaga (LOM) of the Polytechnic University of Madrid to analyze the reliability of methane detection systems used in underground mining. Poor firedamp control in work can cause from production stoppages to fatal accidents and since there is currently a great variety of equipment with different functional characteristics, a study is needed to indicate which measurement principles have the highest degree of confidence. For the development of the project, a series of fixed, transportable and portable methane detectors with different measurement principles have been selected to subject them to laboratory tests following the methods described in the applicable regulations. The test equipment has been the one usually used in the certification and calibration of these devices, subject to the LOM quality system, and the tests have been carried out on detectors accessible in the market. The conclusions establish the main advantages and disadvantages of the equipment according to the measurement principle used; catalytic combustion, interferometry and infrared absorption.

Keywords: ATEX standards, gas detector, methane meter, mining safety

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Authors: M. Amanipour, J. Towfighi, E. Ganji Babakhani, M. Heidari

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Cylindrical alumina microfiltration membrane (GMITM Corporation, inside diameter=9 mm, outside diameter=13 mm, length= 50 mm) with an average pore size of 0.5 micrometer and porosity of about 0.35 was used as the support for membrane reactor. This support was soaked in boehmite sols, and the mean particle size was adjusted in the range of 50 to 500 nm by carefully controlling hydrolysis time, and calcined at 650 °C for two hours. This process was repeated with different boehmite solutions in order to achieve an intermediate layer with an average pore size of about 50 nm. The resulting substrate was then coated with a thin and dense layer of silica by counter current chemical vapour deposition (CVD) method. A boehmite sol with 10 wt.% of nickel which was prepared by a standard procedure was used to make the catalytic layer. BET, SEM, and XRD analysis were used to characterize this layer. The catalytic membrane reactor was placed in an experimental setup to evaluate the permeation and hydrogen separation performance for a steam reforming reaction. The setup consisted of a tubular module in which the membrane was fixed, and the reforming reaction occurred at the inner side of the membrane. Methane stream, diluted with nitrogen, and deionized water with a steam to carbon (S/C) ratio of 3.0 entered the reactor after the reactor was heated up to 500 °C with a specified rate of 2 °C/ min and the catalytic layer was reduced at presence of hydrogen for 2.5 hours. Nitrogen flow was used as sweep gas through the outer side of the reactor. Any liquid produced was trapped and separated at reactor exit by a cold trap, and the produced gases were analyzed by an on-line gas chromatograph (Agilent 7890A) to measure total CH₄ conversion and H₂ permeation. BET analysis indicated uniform size distribution for catalyst with average pore size of 280 nm and average surface area of 275 m².g^-1. Single-component permeation tests were carried out for hydrogen, methane, and carbon dioxide at temperature range of 500-800 °C, and the results showed almost the same permeance and hydrogen selectivity values for hydrogen as the composite membrane without catalytic layer. Performance of the catalytic membrane was evaluated by applying membranes as a membrane reactor for methane steam reforming reaction at gas hourly space velocity (GHSV) of 10,000 h⁻¹ and 2 bar. CH₄ conversion increased from 50% to 85% with increasing reaction temperature from 600 °C to 750 °C, which is sufficiently above equilibrium curve at reaction conditions, but slightly lower than membrane reactor with packed nickel catalytic bed because of its higher surface area compared to the catalytic layer.

Keywords: catalytic membrane, hydrogen, methane steam reforming, permeance

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Authors: Li Chin Law, Epaminondas Mastorakos, Mohd Roslee Othman, Antonis Trakakis

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The paper introduces an alternative concept of carbon capture for shipping by using pre-combustion carbon capture technology (Pre-CCS), which was proven to be less energy intensive than post-combustion carbon capture from the engine exhaust. Energy assessment on amine-based post-combustion CCS on LNG-fuelled ships showed that the energy efficiency of CCS ships reduced from 48% to 36.6%. Then, an energy assessment was carried out to compare the power and heat requirements of the most used hydrogen production methods and carbon capture technologies. Steam methane reformer (SMR) was found to be 20% more energy efficient and achieved a higher methane conversion than auto thermal reaction and methane decomposition. Next, pressure swing adsorber (PSA) has shown a lower energy requirement than membrane separation, cryogenic separation, and amine absorption in pre-combustion carbon capture. Hence, an integrated system combining SMR and PSA (SMR-PSA) with waste heat integration (WHR) was proposed. This optimized SMR-based integrated system has achieved 65% of CO₂ reduction with less than 7-percentage point of energy penalty (41.7% of energy efficiency). Further integration of post-combustion CCS with the SMR-PSA integrated system improved carbon capture rate to 86.3% with 9-percentage points of energy penalty (39% energy efficiency). The proposed system was shown to be able to meet the carbon reduction targets set by International Maritime Organization (IMO) with certain energy penalties.

Keywords: shipping, decarbonisation, alternative fuels, low carbon, hydrogen, carbon capture

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Authors: Radia Imane Fertout

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In recent years, the reaction of dry reforming of methane (DRM) has attracted much attention due to its environmental and industrial importance. Various catalysts, including Ni-based catalysts, have been investigated for the DRM. Doping Ni/Al₂O₃ by lanthanum and alkaline earth element may strongly influence solid-state reaction and increases the stability of catalysts due to the lower density and high basicity of these oxides. The effect of SrO on the activity and stability of Ni/Al₂O₃-La₂O₃ in dry reforming of methane was investigated. These catalysts have been prepared with the impregnation method, calcined in air at 450 and 650°C, then characterized by BET surface area, X-ray diffraction (XRD), and scanning electron microscopy (SEM) techniques and tested in DRM. The results showed that the addition of strontium to Ni/Al2O₃-La₂O₃ decreased the specific surface area. XRD results revealed the presence of different phases of Al₂O₃, La(OH)₃, La₂O₂CO₃, and SrCO₃. The catalytic evaluation results showed that adding SrO increased the catalytic activity and stability, that explained by the strong basicity of strontium. SEM analysis after the reaction indicates the formation of carbon over the spent catalyst and that the addition of strontium stabilized the surface of the catalyst.

Keywords: dry reforming of methane, Ni/Al₂O₃-La₂O₃ catalyst, strontium, nickel

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Authors: Norhaslina Mat Zian, Hasril Hasini, Nur Irmawati Om

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This study focuses on the flow and combustion behavior inside gas turbine combustor used in thermal power plant. The combustion process takes place using synthetic gas and the baseline solution was made on gas turbine combustor firing natural gas (100% Methane) as the main source of fuel. Attention is given to the effect of the H2/CO ratio on the variation of the flame profile, temperature distribution, and emissions. The H2/CO ratio varies in the range of 10-80 % and the CH4 values are fixed 10% for each case. While keeping constant the mass flow rate and operating pressure, the preliminary result shows that the flow inside the can-combustor is highly swirling which indicates good mixing of fuel and air prior to the entrance of the mixture to the main combustion zone.

Keywords: cfd, combustion, flame, syngas

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Authors: Ali Zazi, Ouiza Cherifi

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

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

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Authors: Jinrui Zhang, Tianlong Yang, Ying Pan

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Methane and carbon dioxide are major greenhouse gases contributor. CO₂ dry reforming of methane (DRM) for syngas production is a promising approach to reducing global CO₂ emission and extensive utilization of natural gas. However, the reported catalysts endured rapid deactivation due to severe carbon deposition at high temperature. Here, CO₂ reduction by CH4 on hexagonal nano-nickel flakes packed by porous SiO₂ (Ni@SiO₂) catalysts driven by thermal and solar light are tested. High resistance to carbon deposition and higher reactive activity are demonstrated under focused solar light at moderate temperature (400-500 ℃). Furthermore, the photocatalytic DRM under different wavelength is investigated, and even IR irradiation can enhance the catalytic activity. The mechanism of light-enhanced reaction reactivity and equilibrium is investigated by Infrared and Raman spectroscopy, and the unique reaction pathway with light is depicted. The photo-enhanced DRM provides a promising method of renewable solar energy conversion and CO₂ emission reduction due to the excellent activity and durability.

Keywords: CO₂ emission reduction, methane, photocatalytic DRM, resistance to carbon deposition, syngas

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Authors: Young Nam Chun, Mun Sup Lim

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Carbon dioxide and methane, the major components of biomass pyrolysis/gasification gas and biogas, top the list of substances that cause climate change, but they are also among the most important renewable energy sources in modern society. The purpose of this study is to convert carbon dioxide and methane into high-quality energy using char and commercial activated carbon obtained from biomass pyrolysis as a microwave receptor. The methane reforming process produces hydrogen and carbon. This carbon is deposited in the pores of the microwave receptor and lowers catalytic activity, thereby reducing the methane conversion rate. The deposited carbon was removed by carbon gasification due to the supply of carbon dioxide, which solved the problem of microwave receptor inactivity. In particular, the conversion rate remained stable at over 90% when the ratio of carbon dioxide to methane was 1:1. When the reforming results of carbon dioxide and methane were compared after fabricating nickel and iron catalysts using commercial activated carbon as a carrier, the conversion rate was higher in the iron catalyst than in the nickel catalyst and when no catalyst was used. 

Keywords: microwave, gas reforming, greenhouse gas, microwave receptor, catalyst

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Authors: Jerome Blackman, Pamela Franklin, Volha Roshchanka

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The US coal mining sector accounts for 6% of total US Methane emissions (2021). 60% of US coal mining methane emissions come from active underground mine ventilation systems. Abandoned mines contribute about 13% of methane emissions from coal mining. While there are thousands of abandoned underground coal mines in the US, the Environmental Protection Agency (EPA) estimates that fewer than 100 have sufficient methane resources for viable methane recovery and use projects. Many abandoned mines are in remote areas far from potential energy customers and may be flooded, further complicating methane recovery. Because these mines are no longer active, recovery projects can be simpler to implement.

Keywords: abandoned mines, coal mine methane, coal mining, methane emissions, methane mitigation, recovery and use

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Authors: Ehsan Heidaryan

Abstract:

Gas hydrate sediments are ice like permafrost in deep see and oceans. Methane production in sequestration process and reducing atmospheric carbon dioxide, a main source of greenhouse gas, has been accentuated recently. One focus is capture, separation, and sequestration of industrial carbon dioxide. As a hydrate former, carbon dioxide forms hydrates at moderate temperatures and pressures. This phenomenon could be utilized to capture and separate carbon dioxide from flue gases, and also has the potential to sequester carbon dioxide in the deep seabeds. This research investigated the effect of synthetic surfactants on carbon dioxide hydrate formation, catalysis and consequently, methane production from hydrate permafrosts in sediments. It investigated the sequestration potential of carbon dioxide hydrates in ocean sediments. Also, the catalytic effect of biosurfactants in these processes was investigated.

Keywords: carbon dioxide, hydrate, sequestration, surfactant

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Authors: Ali Zazi, Ouiza Cherifi

Abstract:

The Catalysts materials Ni-SiO₂, Ni-Co-SiO₂ and Ni-Ce-SiO₂ were synthetized by classical method impregnation and supported by silica. This involves combing the silica with an adequate rate of the solution of nickel nitrates, or nickel nitrate and cobalt nitrate, or nickel nitrate and cerium nitrate, mixed, dried and calcined at 700 ° c. These catalysts have been characterized by different physicochemical analysis techniques. The atomic absorption spectrometry indicates that the real contents of nickel, cerium and cobalt are close to the theoretical contents previously assumed, which let's say that the nitrate solutions have impregnated well the silica support. The BET results show that the surface area of the specific surfaces decreases slightly after impregnation with nickel nitrates or Co and Ce metals and a further slight decrease after the reaction. This is likely due to coke deposition. X-ray diffraction shows the presence of the different SiO₂ and NiO phases for all catalysts—theCoO phase for that promoted by Co and the Ce₂O₂ phase for that promoted by Ce. The methane steam reforming reaction was carried out on a quartz reactor in a fixed bed. Reactants and products of the reaction were analyzed by a gas chromatograph. This study shows that the metal addition of Cerium or Cobalt improves the majority of the catalytic performance of Ni for the steam reforming reaction of methane. And we conclude the classification of our Catalysts in order of decreasing activity and catalytic performances as follows: Ni-Ce / SiO₂ >Ni-Co / SiO₂> Ni / SiO₂ .

Keywords: cerium, cobalt, heterogeneous catalysis, hydrogen, methane, steam reforming, synthesis gas

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Authors: Jozef Mindas, Jana Skvareninova

Abstract:

Wetlands are a main natural source of methane emissions, but they also represent the important biodiversity reservoirs in the landscape. There are about 26 thousands hectares of wetlands in Slovakia identified via the wetlands monitoring program. Created database of wetlands in Slovakia allows to analyze several ecological processes including also the methane emissions estimate. Based on the information from the database, the first estimate of the methane emissions from wetlands in Slovakia has been done. The IPCC methodology (Tier 1 approach) has been used with proposed emission factors for the ice-free period derived from the climatic data. The highest methane emissions of nearly 550 Gg are associated with the category of fens. Almost 11 Gg of methane is emitted from bogs, and emissions from flooded lands represent less than 8 Gg.

Keywords: bogs, methane emissions, Slovakia, wetlands

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Authors: J. P. Chica Cano, G. Cabot, S. de Persis, F. Foucher

Abstract:

Among all possibilities to combat global warming, CO₂ capture and sequestration (CCS) is presented as a great alternative to reduce greenhouse gas (GHG) emission. Several strategies for CCS from industrial and power plants are being considered. The concept of combined oxy-fuel combustion has been the most alternative solution. Nevertheless, due to the high cost of pure O₂ production, additional ways recently emerged. In this paper, an innovative combustion process for a gas turbine cycle was studied: it was composed of methane combustion with oxygen enhanced air (OEA), exhaust gas recirculation (EGR) and H₂O issuing from STIG (Steam Injection Gas Turbine), and the CO₂ capture was realized by membrane separator. The effect on this combustion process was emphasized, and it was shown that a study of the influence of H₂O dilution on the combustion parameters by experimental and numerical approaches had to be carried out. As a consequence, the laminar burning velocities measurements were performed in a stainless steel spherical combustion from atmospheric pressure to high pressure (up to 0.5 MPa), at 473 K for an equivalence ratio at 1. These experimental results were satisfactorily compared with Chemical Workbench v.4.1 package in conjunction with GRIMech 3.0 reaction mechanism. The good correlations so obtained between experimental and calculated flame speed velocities showed the validity of the GRIMech 3.0 mechanism in this domain of combustion: high H₂O dilution, low N₂, medium pressure. Finally, good estimations of flame speed and pollutant emissions were determined in other conditions compatible with real gas turbine. In particular, mixtures (composed of CH₄/O₂/N₂/H₂O/ or CO₂) leading to the same adiabatic temperature were investigated. Influences of oxygen enrichment and H₂O dilution (compared to CO₂) were disused.

Keywords: CO₂ capture, oxygen enrichment, water dilution, laminar burning velocity, pollutants emissions

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Authors: Bedarnia Ishak

Abstract:

In the recent years, the dry reforming of methane has received considerable attention from an environmental view point because it consumes and eliminates two gases (CH4 and CO2) responsible for global warming by greenhouse effect. Many catalysts containing noble metal (Rh, Ru, Pd, Pt and Ir) or transition metal (Ni, Co and Fe) have been reported to be active in this reaction. Compared to noble metals, Ni-materials are cheap but very easily deactivated by coking. Ni-based mixed oxides structurally well-defined like perovskites and spinels are being studied because they possibly make solid solutions and allow to vary the composition and thus the performances properties. In this work, nano-sized nickel ferrite oxides are synthesized using three different methods: Co-precipitation (CP), hydrothermal (HT) and sol gel (SG) methods and characterized by XRD, Raman, XPS, BET, TPR, SEM-EDX and TEM-EDX. XRD patterns of all synthesized oxides showed the presence of NiFe2O4 spinel, confirmed by Raman spectroscopy. Hematite was present only in CP sample. Depending on the synthesis method, the surface area, particle size, as well as the surface Ni/Fe atomic ratio (XPS) and the behavior upon reduction varied. The materials were tested in methane dry reforming with CO2 at 1 atm and 650-800 °C. The catalytic activity of the spinel samples was not very high (XCH4 = 5-20 mol% and XCO2 = 25-40 mol %) when no pre-reduction step was carried out. A significant contribution of RWGS explained the low values of H2/CO ratio obtained. The reoxidation step of the catalyst carried out after reaction showed little amounts of coke deposition. The reducing pretreatment was particularly efficient in the case of SG (XCH4 = 80 mol% and XCO2 = 92 mol%, at 800 °C), with H2/CO > 1. In conclusion, the influence of preparation was strong for most samples and the catalytic behavior could be interpreted by considering the distribution of cations among octahedral (Oh) and tetrahedral (Td) sites as in (Ni2+1-xFe3+x) Td (Ni2+xFe3+2-x) OhO2-4 influenced the reducibility of materials and thus their catalytic performance.

Keywords: NiFe2O4, dry reforming of methane, spinel oxide, oxide zenc

Procedia PDF Downloads 252