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Conflict of Interest: In relation to this article, we declare that there is no conflict of interest.

Publication history: Received July 29, 2003
Accepted September 16, 2003

This is an Open-Access article distributed under the terms of the Creative Commons Attribution Non-Commercial License (http://creativecommons.org/licenses/bync/3.0) which permits unrestricted non-commercial use, distribution, and reproduction in any medium, provided the original work is properly cited.

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Reaction Mechanism of Partial Oxidation of Methane to Synthesis Gas over Supported Ni Catalysts

Sang-Bum Kim Young-Kook Kim Yun-Su Lim Myung-Soo Kim Hyun-Sik Hahm^†

Division of Ceramic and Chemical Engineering, Myongji University, Yongin 449-728, Korea

hahm@mju.ac.kr

Korean Journal of Chemical Engineering, November 2003, 20(6), 1023-1025(3), 10.1007/BF02706931

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Abstract

A mechanistic study on the partial oxidation of methane to synthesis gas (H₂ and CO) was conducted with supported nickel catalysts. To investigate the reaction mechanism, pulse experiments, O₂-TPD, and a comparison of the moles of reactants and products were carried out. From the O₂-TPD experiment, it was observed that the active catalyst in the synthesis gas production desorbed oxygen at a lower temperature. In the pulse experiment, the temperature of the top of the catalyst bed increased with the pulses, whereas the temperature of the bottom decreased. This suggests that there are two kinds of reactions, that is, the total oxidation of methane (exothermic) at the top and reforming reactions (endothermic) at the bottom. From the comparison of the moles of reactants and products, it was found that the moles of CO₂, CH₄ and H₂O decreased as the moles of H₂ and CO increased. The results support the mechanism that synthesis gas is produced through a two-step reaction mechanism: the total oxidation of methane to CO₂ and H₂O takes place first, followed by the reforming reaction of the produced CO₂ and H₂O with residual CH₄ to form synthesis gas.

Keywords

Supported Nickel Catalyst Synthesis Gas Oxidation of Methane (Partial) TPD Pulse Reaction Mechanistic Study

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