• Transactions of the Korean hydrogen and new energy society
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• v.33 no.4
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• pp.451-461
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• 2022

CFD analysis including optimization process was conducted to design shell and tube CO₂ methanation reactor cooling system. The high-pressure saturated water flowed into the cooling system and was evaporated by heat flux from reacting tubes. The optimization process decided the gap between tubes and reactor diameter to satisfy objective functions related to temperature. The results showed that the gap and diameter reduced about 30% and 3.6% respectively. Averaged surface temperature satisfied the target value and the min-max deviation was minimized.

• Transactions of the Korean hydrogen and new energy society
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• v.34 no.3
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• pp.316-326
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• 2023

Development of carbon-neutral fuel production technologies to solve climate change issues is progressing worldwide. Among them, methane can be produced through the synthesis of hydrogen produced by renewable energy and carbon dioxide captured through a CO₂ methanation reaction, and the fuel produced in this way is called synthetic methane or e-methane. The CO₂ methanation reaction can be conducted via biological or thermochemical methods. In this study, a 30 Nm³/h thermochemical CO₂ methanation process consisting of an isothermal reactor and an adiabatic reactor was used. The CO₂ conversion rate and methane concentration according to the temperature measurement results at the center and outside of the adiabatic reactor were analyzed. The gas flow into the adiabatic reactor was found to reach equilibrium after about 1.10 seconds or more by evaluating the residence time. Furthermore, experimental and analysis results were compared to evaluate performance of the reactor.

• Clean Technology
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• v.19 no.2
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• pp.156-164
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• 2013

In this study, we analyzed the operational characteristics of a 0.25 MW methanation pilot plant. Isothermal reactor controled the heat released from methanation reaction by saturated water in shell side. Methanation process consisting of isothermal reactor and adiabatic reactor had advantages with no recycle compressor and more less reactors compared with methanation process with only adiabatic reactors. In case that $H_2$/CO ratio of syngas was under 3, carbon deposition occurred on catalyst in tube side of isothermal reactor and the pressure of reactors increased. In case that $H_2$/CO ratio was maintained around 3, no carbon deposition on catalyst in tube side of isothermal reactor was found by monitoring the differential pressure of reactors and by measuring the differential pressure of several of tubes filled with catalyst before and after operating. It was shown that CO conversion and $CH_4$selectivity were over 99, 97%, respectively, and the maximum $CH_4$productivity was $695ml/h{\cdot}g-cat$.

• Applied Chemistry for Engineering
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• v.31 no.3
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• pp.323-327
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• 2020

The reaction characteristics of Ni/CeO_2-X which is highly efficient at a low temperature was investigated for an application to carbon dioxide methanation process. The CeO_2-X support was obtained by the heat treatment of Ce(NO₃)₃ at 400 ℃ and the catalyst was prepared by impregnation process. The operating parameters of the experiment were the internal pressure of the reactor, the composition of oxygen, methane, and hydrogen sulfide in the inlet gas and the reaction temperature. When Ni/CeO_2-X was used for the carbon dioxide methanation reaction, the CO₂ conversion rate increased by more than 25% as the pressure increased from 1 to 3 bar. The increase was large at a low reaction temperature. When both oxygen and methane were in the inlet gas, the CO₂ conversion rate of the catalyst decreased by up to 16 and 4%, respectively. As the concentration of oxygen and methane increased, the reduction rate of the CO₂ conversion rate tended to increase. In addition, the hydrogen sulfide in the inlet gas reduced the CO₂ conversion rate by up to 7% and caused catalyst deactivation. The results of this study will be useful as basic data for the carbon dioxide methanation process.

• Transactions of the Korean hydrogen and new energy society
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• v.30 no.1
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• pp.14-20
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• 2019

The power to gas (P2G) is one of the energy storage technologies that can increase the storage period and storage capacity compared to the existing battery type. One of P2G technologies produces hydrogen by decomposing water from renewable energy (electricity) and the other produces $CH_4$ by reacting hydrogen with $CO_2$. The objective of this study is the reaction of $CO_2$ methanation which synthesized methane by reacting carbon dioxide and hydrogen. The effect of $CO_2$ conversion and $CH_4$ selectivity on reaction temperature, pressure, and methane contents over 40% Ni catalyst was mainly investigated throughout this study. As a result, the activity of this catalyst appeared to be the highest in $CH_4$ yield at around $400^{\circ}C$ and the selectivity of $CH_4$ increased with increasing reaction pressure. The methane content was not significantly influenced below 3% of all componets. As the space velocity increases from 10,000 to 30,000/hr, the $CO_2$ conversion rate tends to decrease.

• Transactions of the Korean hydrogen and new energy society
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• v.22 no.2
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• pp.249-256
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• 2011

In this study, the Ni-based catalysts for the production of synthetic natural gas were prepared by various preparation methods such as the co-precipitation, precipitation, impregnation and physical mixing methods. The ranges of the reaction conditions were the temperatures of 250~$350^{\circ}C$, $H_2$/CO mole ratio of 3.0, the pressures of 1 atm and the space velocity of 20000 $ml/g_{-cat{\cdot}}{\cdot}h$. It was found that the catalyst prepared by precipitation method had higher CO conversion than the catalyst prepared by co-precipitation method. While the catalyst prepared by precipitation method had the formation of NiO structure, the catalyst prepared by co-precipitation method had the formation of $NiAl_2O_4$ structure. It was confirmed that Ni-based catalyst prepared by the physical mixing method had the lowest CO conversion because it was deactivated by the production of $Ni_3C$ during the methanation. As a result, it was shown clearly that Ni-based catalysts prepared by impregnation method expressed the highest catalytic activity in CO methanation.

• Transactions of the Korean hydrogen and new energy society
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• v.31 no.5
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• pp.419-428
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• 2020

The kinetics of direct methanation over activated charcoal-supported molybdenum catalyst at 30 bar was studied in a cylindrical fixed-bed reactor. When the temperature was not higher than 400℃, the CO conversion increased with increasing temperature according to the Arrhenius law of reaction kinetics. While XRD and Raman analysis showed that Mo was present as Mo oxides after reduction or methanation, TEM and XPS analysis showed that Mo₂C was formed after methanation depending on the loading of Mo precursor. When the temperature was as high as 500℃, the CO conversion was dependent not only on the Arrhenius law but also on the catalyzed reaction by nanoparticles, which came off from the reactor and thermocouple by metal dusting. These nanoparticles were made of Ni, Fe, Cr and alloy, and attributed to the formation of carbon deposit on the wall of the reactor and on the surface of the thermocouple. The carbon deposit consisted of amorphous and disordered carbon filaments.

• Clean Technology
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• v.24 no.2
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• pp.99-104
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• 2018

In this work, we performed the methanation reaction using synthesis gas ($H_2/CO_2$) for the process to produce synthetic natural gas (SNG) for $4^{th}$ methanation reactor in SNG process proposed by RIST-IAE. Experimental conditions were changed with temperature, pressure and space velocity. At this time, $CO_2$ conversion, $CH_4$ selectivity and $H_2$ concentration after reaction were investigated. As a result, $CH_4$ selectivity by the $CO_2$ methanation increased with lower space velocity and higher pressure. On the other hand, in the case of temperature, the maximum value was shown at $320^{\circ}C$. From these results, it was found that the optimum condition of the fourth reactor suitable for the SNG process was obtained.

• Applied Chemistry for Engineering
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• v.4 no.2
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• pp.365-372
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• 1993

$CO_2$ methanation was performed over Ni supported on cation-exchanged Y zeolites under atmospheric pressure at $250{\sim}550^{\circ}C$ and $H_2/CO_2$ mole ratio of 4. Adsorption strength between carbon dioxide and nickel was found to be Influenced by the cation exchanged in the zeolite. TPD(Temperature-programmed desorption) results show that the adsorption strength decreases in the order of Ni/NaY>Ni/MaY>Ni/HY. TPSR(Temperature-programmed surface reaction) results indicate that enhanced methanation activity is obtained when the adsorption strength between carbon dioxide and nickel is stroing. As the reduction temperature increases, the methantion activity of the catalyst increase. From this result the larger size nickel particle seems advantageous for $CO_2$ methanation reaction. The maximum activity is obtained when nickel loading is 3.3wt%. Carbon monoxide is produced as a by-product throughout the reaction temperature range, and as the contact time increases, the selectivity to methane increases and the selectivity to carbon monoxide decreases steadily. Thus methane seems to be produced from $CO_2$ via CO as an intermediate species. In the temperature range of $410{\sim}450^{\circ}C$, the methane production rate is found to be dependent on the orders of 3.3~-0.5 and 1.4~3.6 with respect to $CO_2$ and $H_2$ partial pressures, respectively. This clearly shows that $CO_2$ and $H_2$ are competing for adsorption sites and as the reaction temperature increases, it becomes increasingly difficult for $H_2$ to be adsorbed on the catalyst surface.

• Transactions of the Korean hydrogen and new energy society
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• v.32 no.5
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• pp.388-400
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• 2021

Power to gas (P2G) is one of the energy storage technologies that can increase the storage period and storage capacity compared to the existing battery type. One of P2G technology produces hydrogen by decomposing water from renewable energy (electricity) and the other produces CH4 by reacting hydrogen with CO2. This study is an experimental study to produce CH4 by reacting CO2 of biogas with hydrogen using a 40 wt% Ni-Mg-Al catalyst and a commercial catalyst. Catalyst characteristics were analyzed through H2-TPR, XRD, and XPS instruments of 40% Ni catalyst and commercial catalyst. The effect on the CO2 conversion rate and CH4 selectivity was analyzed, and the activities of a 40% Ni catalyst and a commercial catalyst were compared. As a result of experiment, In the case of a 40 wt% catalyst, the maximum CO2 conversion rate showed 77% at the reaction temperature of 400℃. Meanwhile, the commercial catalyst showed a maximum CO2 conversion rate of 60% at 450℃. When 50% of CO was added to the CO2 methanation reaction, the CO2 conversion rate was increased by about 5%. This is considered to be due to the atmosphere in which the CO reaction can occur without the process of converting to CH4 after forming carbon and CO as intermediates in terms of the CO2 mechanism on the catalyst surface.