• Journal of Hydrogen and New Energy
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• v.25 no.4
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• pp.425-435
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• 2014

Simulation studies on catalytic methanation reaction in externally cooled tubular reactor filled with monolithic catalysts were carried out using a general purpose modelling tool $gPROMS^{(R)}$. We investigated the effects of operating parameters such as gas space velocity, temperature and pressure of feeding gas on temperature distribution inside the reactor, overall CO conversion, and chemical composition of product gas. In general, performance of methanation reaction is favored under low temperature and high pressure for a wide range of their values. However, methane production becomes negligible at temperatures below 573K when the reactor temperature is not high enough to ignite methanation reaction. Capacity enhancement of the reactor by increasing gas space velocity and/or gas inlet pressure resulted no significant reduction in reactor performance and heat transfer property of catalyst.

• New & Renewable Energy
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• v.6 no.4
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• pp.30-40
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• 2010

Syngas from gasification of coal can be converted to SNG(Synthesis Natural Gas) through gas cleaning, water gas shift, $CO_2$ removal, and methanation. One of the key technologies involved in the production of SNG is the methanation process. In the methanation process, carbon oxide is converted into methane by reaction with hydrogen. Major factors of methanation are hydrogen-carbon oxide ratio, reaction temperature and space velocity. In order to understand the catalytic behavior, temperature programmed surface reaction (TPSR) experiments and reaction in a fixed bed reactor of carbon monoxide have been performed using two commercial catalyst with different Ni contents (Catalyst A, B). In case of catalyst A, CO conversion was over 99% at the temperature range of $350{\sim}420^{\circ}C$ and CO conversions and $CH_4$ selectivity were lower at the space condition over 3000 1/h. In case of catalyst B, CO conversion was 100% at the temperature over $370^{\circ}C$ and CO conversions and $CH_4$ selectivity were lower at the space condition over 4700 1/h. Also, conditions to satisfy $CH_4$ productivity over 500 ml/h.g-cat were over 2000 1/h of space velocity in case of catalyst A and over 2300 1/h of space velocity in case of catalyst B.

• Korean Chemical Engineering Research
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• v.52 no.5
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• pp.678-687
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• 2014

The catalytic performance of silicon carbide supported nickel catalysts modified with or without second metal (Co, Cu and Zn) for the methanation of CO has been investigated in a fixed-bed reactor using a feed consisting of 25% CO and 75% $H_2$ without any diluent gas. It has been found that the introduction of Co species can clearly improve the catalytic activity of Ni/SiC catalyst, whereas the addition of Cu or Zn can result in a significant decrease in the catalytic activity. The characterizations by means of XRD, TEM, XPS, CO-TPD and $H_2$-TPR indicate that the addition of Co could decrease the particle size of active metal, increase active sites on the surface of methanation catalyst, improve the chemisorption of CO and enhance the reducibility of methanation catalysts. Additionally, the special interaction between Co species and Ni species is likely favorable for the dissociation of adsorbed CO on the surface of catalyst, and this may also contribute to the high activity of 5Co-Ni/SiC catalyst for CO methanation reaction. For 5Cu-Ni/SiC catalyst and 5Zn-Ni/SiC catalyst, Cu and Zn species could cover partial nickel particles and decrease the chemisorption amount of CO. These could be responsible for the low methanation activity. In addition, a 150h stability test under 2 MPa and $300^{\circ}C$ showed that 5Co-Ni/SiC catalyst was very stable for CO methanation reaction.

• Applied Chemistry for Engineering
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• v.23 no.6
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• pp.572-576
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• 2012

This study presents the $CO_2$ methanation reaction on Pt catalysts for reducing the amount of $CO_2$, one of greenhouse gases. The AlO(OH) of $Al_2O_3$precusor was used as a support via a thermal treatment and the Pt was used as an active metal. In XRD results, it was confirmed that the Pt was well dispersed and the support existed as the gamma $Al_2O_3$phase. The $Pt/Al_2O_3$ catalyst calcined at $600^{\circ}C$ showed the highest conversion efficiency and selectivity.

• Journal of Hydrogen and New Energy
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• v.26 no.3
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• pp.260-270
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• 2015

One-dimensional packed bed reactor model accounting for interfacial and intra-particle gradients was developed and based on it numerical analyses were performed to investigate the dynamic behavior of a commercial scale methanation reactor. Methanation reaction was almost complete near the reactor inlet and gases with equilibrated composition were discharged from the reactor. Both the intra-particle temperature gradient and differential surface temperature rise were found to be severe near the reactor inlet. To reduce the possible degradation or fracture of catalyst particles and prevent local overheating on the catalyst, addition of inert material can be an effective way.

• Clean Technology
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• v.20 no.1
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• pp.57-63
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• 2014

In this work, we performed the methanation with steam and synthesis gas of a low $H_2/CO$ ratio to develop a process for producing SNG (synthetic natural gas). In this experiment conditions, the water gas shift reaction and the methanation reaction take place at the same time, and insufficient supply of steam might cause the deactivation of the catalyst. Therefore, the reaction characteristics with the amount of steam was performed, and the methanation on syngas containing $CO_2$ of the high concentration were studied. As a result, the temperature in the catalyst bed decreased by the supply of steam, and the methanation and the water gas shift reaction occurred at the same time. Although methane yield slightly decreased at the methanation using syngas containing $CO_2$ of the high concentration, the long-term operation (1,000 h) in the experimental conditions of this study indicates that this condition is suitable for the new commercial scale SNG process.

• 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.

• Korean Chemical Engineering Research
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• v.56 no.2
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• pp.269-274
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• 2018

All the $Ni-Co-Ce-ZrO_2$ mixed oxides are prepared by co-precipitations methods. Methanation of CO and $H_2$ reaction is screened tested over different fractions of cerium (2, 4, 7 and 12 wt.%) over $Ni-Co/ZrO_2$ bimetallic catalysts are investigated. The mixed oxides are characterized by XRD, CO-Chemisorption, TGA and screened methanation of CO and $H_2$ at $360^{\circ}C$ for 3000 min on stream at typical ratio $CO:H_2=1:1$. In $Ni-Co/CeZrO_2$ series 2 wt.% Ce loading catalyst shows most promising catalyst for $CH_4$ selectivity than $CO_2$, which directs more stability with less coke formation. The high activity is attributed to the better bimetallic synergy and the well-developed crystalline phases of NiO, $ZrO_2$ and $Ce-ZrO_2$. Other bimetallic mixed oxides NCoZ, $NCoC^{4-12}Z$ has faster deactivation with low methanation activity. Finally, 2 wt.% Ce loading catalyst was found to be optimal coke resistant catalyst.

• Journal of Hydrogen and New Energy
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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.

• Journal of the Korean Institute of Gas
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• v.13 no.5
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• pp.33-38
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• 2009

Synthetic natural gas was producd by the reaction of carbon monoxide and hydrogen via methanation. Ni-Co bimetallic catalyst supported on $Al_2O_3$ for methanation was prepared using deposition-precipitation method. For the comparison, Ni, Co monometallic catalyst was prepared using the same method. The prepared catalysts were characterized by TEM, XRD and TPR and applied to methanation reaction. The catalysts prepared using deposition-precipitation method showed the high metal dispersion. The activity of Ni-Co bimetallic catalyst was higher than that of Ni, Co monometallic catalyst. TPR measurements indicated that Ni-Co bimetallic catalyst had more active hydrogen species than Ni, Co monometallic catalyst due to the synergetic effect in the presence of Ni and Co.