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Title: Transient response of catalyst bed temperature in the pulsed reaction of partial oxidation of methane to synthesis gas over supported rhodium and iridium catalysts

Abstract

Mechanisms of partial oxidation of methane were studied using a pulsed reaction technique and temperature jump measurement. Catalyst bed temperatures were directly measured by introducing a pulse of a mixture of methane and oxygen (2/1). With Ir/TiO{sub 2} catalyst, a sudden temperature increase at the front edge of the catalyst bed was observed upon introduction of the pulse, but the temperature of the rear end of the catalyst bed increased only slightly. The synthesis gas production basically proceeded via a two-step path consisting of highly exothermic methane complete oxidation to give H{sub 2}O and CO{sub 2}, followed by the endothermic reforming of methane with H{sub 2}O and CO{sub 2} over Ir/TiO{sub 2} catalyst. However, with Rh/TiO{sub 2} and Rh/Al{sub 2}O{sub 3} catalysts, the temperature at the front edge of the catalyst bed decreased upon introduction of the CH{sub 4}/O{sub 2} (2/1) pulse, and a small increase in the temperature at the rear end was observed. At first, endothermic decomposition of CH{sub 4} to H{sub 2} and deposited carbon or CH{sub x} probably took place at the front edge of the catalyst bed and then deposited carbon or generated CH{sub x} species would be oxidized into CO{sub x}. However, on Rh/SiO{submore » 2}, synthesis gas was produced via a two-step path similar to the case of Ir/TiO{sub 2} catalyst. The reaction pathway of partial oxidation of methane with Rh-loaded catalysts depended strongly on the support materials.« less

Authors:
; ;  [1]; ;  [2]
  1. Kansai Univ., Suita, Osaka (Japan)
  2. Osaka National Research Inst., Ikeda, Osaka (Japan)
Publication Date:
OSTI Identifier:
687748
Resource Type:
Journal Article
Journal Name:
Journal of Catalysis
Additional Journal Information:
Journal Volume: 186; Journal Issue: 2; Other Information: PBD: 10 Sep 1999
Country of Publication:
United States
Language:
English
Subject:
03 NATURAL GAS; 10 SYNTHETIC FUELS; METHANE; PARTIAL OXIDATION PROCESSES; SYNTHESIS GAS; RHODIUM; IRIDIUM; CATALYTIC EFFECTS; CHEMICAL REACTION KINETICS; CATALYSTS; TEMPERATURE MEASUREMENT; CATALYST SUPPORTS

Citation Formats

Nakagawa, Kiyoharu, Ikenaga, Naoki, Suzuki, Toshimitsu, Teng, Yonghong, and Kobayashi, Tetsuhiko. Transient response of catalyst bed temperature in the pulsed reaction of partial oxidation of methane to synthesis gas over supported rhodium and iridium catalysts. United States: N. p., 1999. Web. doi:10.1006/jcat.1999.2576.
Nakagawa, Kiyoharu, Ikenaga, Naoki, Suzuki, Toshimitsu, Teng, Yonghong, & Kobayashi, Tetsuhiko. Transient response of catalyst bed temperature in the pulsed reaction of partial oxidation of methane to synthesis gas over supported rhodium and iridium catalysts. United States. doi:10.1006/jcat.1999.2576.
Nakagawa, Kiyoharu, Ikenaga, Naoki, Suzuki, Toshimitsu, Teng, Yonghong, and Kobayashi, Tetsuhiko. Fri . "Transient response of catalyst bed temperature in the pulsed reaction of partial oxidation of methane to synthesis gas over supported rhodium and iridium catalysts". United States. doi:10.1006/jcat.1999.2576.
@article{osti_687748,
title = {Transient response of catalyst bed temperature in the pulsed reaction of partial oxidation of methane to synthesis gas over supported rhodium and iridium catalysts},
author = {Nakagawa, Kiyoharu and Ikenaga, Naoki and Suzuki, Toshimitsu and Teng, Yonghong and Kobayashi, Tetsuhiko},
abstractNote = {Mechanisms of partial oxidation of methane were studied using a pulsed reaction technique and temperature jump measurement. Catalyst bed temperatures were directly measured by introducing a pulse of a mixture of methane and oxygen (2/1). With Ir/TiO{sub 2} catalyst, a sudden temperature increase at the front edge of the catalyst bed was observed upon introduction of the pulse, but the temperature of the rear end of the catalyst bed increased only slightly. The synthesis gas production basically proceeded via a two-step path consisting of highly exothermic methane complete oxidation to give H{sub 2}O and CO{sub 2}, followed by the endothermic reforming of methane with H{sub 2}O and CO{sub 2} over Ir/TiO{sub 2} catalyst. However, with Rh/TiO{sub 2} and Rh/Al{sub 2}O{sub 3} catalysts, the temperature at the front edge of the catalyst bed decreased upon introduction of the CH{sub 4}/O{sub 2} (2/1) pulse, and a small increase in the temperature at the rear end was observed. At first, endothermic decomposition of CH{sub 4} to H{sub 2} and deposited carbon or CH{sub x} probably took place at the front edge of the catalyst bed and then deposited carbon or generated CH{sub x} species would be oxidized into CO{sub x}. However, on Rh/SiO{sub 2}, synthesis gas was produced via a two-step path similar to the case of Ir/TiO{sub 2} catalyst. The reaction pathway of partial oxidation of methane with Rh-loaded catalysts depended strongly on the support materials.},
doi = {10.1006/jcat.1999.2576},
journal = {Journal of Catalysis},
number = 2,
volume = 186,
place = {United States},
year = {1999},
month = {9}
}