Partial oxidation of methane over a ruthenium phthalocyanine catalyst

Yuan Zhu; Robert Barat

doi:10.1016/j.ces.2014.04.028

Partial oxidation of methane over a ruthenium phthalocyanine catalyst

Yuan Zhu, Robert Barat

Chemical and Materials Engineering

Research output: Contribution to journal › Article › peer-review

16 Scopus citations

Abstract

The partial oxidation of He-diluted CH₄ with O₂ has been studied in a laboratory flow reactor packed with fragmented pellets of zeolite-encaged Ru phthalocyanine catalyst. Gas compositions (CH₄, O₂, CO, CO₂, and H₂) were determined by on-line GC/TCD. Absolute system pressure was maintained at 445kPa. Most experiments were performed at a constant gas space velocity=0.717/s. Data were obtained over wide ranges of temperature (523-648K) and CH₄/O₂ feed molar ratio (0.5-6.5). Observed conversion of CH₄ increased with temperature. Product selectivities of H₂ and CO increased, while that of CO₂ decreased, with increasing temperature and feed CH₄/O₂. Based on data analysis with an integral plug flow packed bed reactor model, the power law kinetic rate for CH₄ conversion was observed to be first order in each of O₂ and CH₄. A non-linear Arrhenius plot of the global rate constants, together with a Mears correlation analysis, suggests that an external mass transfer resistance becomes active above 573K in this system.

Original language	English (US)
Pages (from-to)	71-76
Number of pages	6
Journal	Chemical Engineering Science
Volume	116
DOIs	https://doi.org/10.1016/j.ces.2014.04.028
State	Published - Sep 6 2014

All Science Journal Classification (ASJC) codes

General Chemistry
General Chemical Engineering
Industrial and Manufacturing Engineering

Keywords

Catalysis
Gases
Kinetics
Methane
Oxygen
Zeolites

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title = "Partial oxidation of methane over a ruthenium phthalocyanine catalyst",

abstract = "The partial oxidation of He-diluted CH4 with O2 has been studied in a laboratory flow reactor packed with fragmented pellets of zeolite-encaged Ru phthalocyanine catalyst. Gas compositions (CH4, O2, CO, CO2, and H2) were determined by on-line GC/TCD. Absolute system pressure was maintained at 445kPa. Most experiments were performed at a constant gas space velocity=0.717/s. Data were obtained over wide ranges of temperature (523-648K) and CH4/O2 feed molar ratio (0.5-6.5). Observed conversion of CH4 increased with temperature. Product selectivities of H2 and CO increased, while that of CO2 decreased, with increasing temperature and feed CH4/O2. Based on data analysis with an integral plug flow packed bed reactor model, the power law kinetic rate for CH4 conversion was observed to be first order in each of O2 and CH4. A non-linear Arrhenius plot of the global rate constants, together with a Mears correlation analysis, suggests that an external mass transfer resistance becomes active above 573K in this system.",

keywords = "Catalysis, Gases, Kinetics, Methane, Oxygen, Zeolites",

author = "Yuan Zhu and Robert Barat",

note = "Funding Information: The authors appreciate the support of the National Science Foundation, United States ( CBET-1022337 ). The authors also acknowledge Professor Sergiu Gorun of the Chemistry Department of Seton Hall University, South Orange, NJ for supplying the catalyst. ",

year = "2014",

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doi = "10.1016/j.ces.2014.04.028",

language = "English (US)",

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TY - JOUR

T1 - Partial oxidation of methane over a ruthenium phthalocyanine catalyst

AU - Zhu, Yuan

AU - Barat, Robert

N1 - Funding Information: The authors appreciate the support of the National Science Foundation, United States ( CBET-1022337 ). The authors also acknowledge Professor Sergiu Gorun of the Chemistry Department of Seton Hall University, South Orange, NJ for supplying the catalyst.

PY - 2014/9/6

Y1 - 2014/9/6

N2 - The partial oxidation of He-diluted CH4 with O2 has been studied in a laboratory flow reactor packed with fragmented pellets of zeolite-encaged Ru phthalocyanine catalyst. Gas compositions (CH4, O2, CO, CO2, and H2) were determined by on-line GC/TCD. Absolute system pressure was maintained at 445kPa. Most experiments were performed at a constant gas space velocity=0.717/s. Data were obtained over wide ranges of temperature (523-648K) and CH4/O2 feed molar ratio (0.5-6.5). Observed conversion of CH4 increased with temperature. Product selectivities of H2 and CO increased, while that of CO2 decreased, with increasing temperature and feed CH4/O2. Based on data analysis with an integral plug flow packed bed reactor model, the power law kinetic rate for CH4 conversion was observed to be first order in each of O2 and CH4. A non-linear Arrhenius plot of the global rate constants, together with a Mears correlation analysis, suggests that an external mass transfer resistance becomes active above 573K in this system.

AB - The partial oxidation of He-diluted CH4 with O2 has been studied in a laboratory flow reactor packed with fragmented pellets of zeolite-encaged Ru phthalocyanine catalyst. Gas compositions (CH4, O2, CO, CO2, and H2) were determined by on-line GC/TCD. Absolute system pressure was maintained at 445kPa. Most experiments were performed at a constant gas space velocity=0.717/s. Data were obtained over wide ranges of temperature (523-648K) and CH4/O2 feed molar ratio (0.5-6.5). Observed conversion of CH4 increased with temperature. Product selectivities of H2 and CO increased, while that of CO2 decreased, with increasing temperature and feed CH4/O2. Based on data analysis with an integral plug flow packed bed reactor model, the power law kinetic rate for CH4 conversion was observed to be first order in each of O2 and CH4. A non-linear Arrhenius plot of the global rate constants, together with a Mears correlation analysis, suggests that an external mass transfer resistance becomes active above 573K in this system.

KW - Catalysis

KW - Gases

KW - Kinetics

KW - Methane

KW - Oxygen

KW - Zeolites

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Partial oxidation of methane over a ruthenium phthalocyanine catalyst

Abstract

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