Ni/CeO2 promoted Ru and Pt supported on FeCrAl gauze for cycling methane catalytic partial oxidation—CPOX

Gianluca Pauletto; Nicole Libretto; Daria C. Boffito; Jeffrey T. Miller; Andreas Jentys; Gregory S. Patience; Johannes A. Lercher

doi:10.1016/j.apcatb.2020.119849

Ni/CeO₂ promoted Ru and Pt supported on FeCrAl gauze for cycling methane catalytic partial oxidation—CPOX

Gianluca Pauletto, Nicole Libretto, Daria C. Boffito, Jeffrey T. Miller, Andreas Jentys, Gregory S. Patience, Johannes A. Lercher

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

15 Scopus citations

Abstract

Stranded natural gas is economically unattractive due to high operating and investment costs of conventional technologies necessary to bring it to market. However, milli-second reactors operating at a GHSV up to 200 000 h⁻¹ reduce investment. The first step of a gas-to-liquids process produces syngas—a mixture of CO and H₂. Here, we propose promoted Ni-based catalysts supported on FeCrAl knitted gauze to partially oxidize CH₄ in air to syngas. High syngas selectivities at 1 bar, 700 °C and CH₄/O₂ ratios of 2.5 to 5 suggests an apparent direct reaction path to CO and H₂. Ru promoted catalysts had higher turnover rates in CH₄ activation compared to Ni, Ni-Pt and Ni-Pt-Ru. All catalysts containing Pt formed carbon species refractory to air regeneration at 700 °C. 2.25% Ni with 0.1% Ru had the highest CH₄ turnover rate (155 mol s⁻¹ mol⁻¹) and CO selectivity (80%) at a CH₄/O₂ ratio 2.5. CH₄ conversion and CO production were constant after 50 reaction-regeneration cycles that dosed the catalyst for 25 min with methane/air followed by an equal time in air at the same reaction temperature.

Original language	English
Article number	119849
Journal	Applied Catalysis B: Environmental
Volume	286
DOIs	https://doi.org/10.1016/j.apcatb.2020.119849
State	Published - 5 Jun 2021

Keywords

CPOX
FeCrAl
Gauze
Natural gas
Ni/CeO
Syngas

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title = "Ni/CeO2 promoted Ru and Pt supported on FeCrAl gauze for cycling methane catalytic partial oxidation—CPOX",

abstract = "Stranded natural gas is economically unattractive due to high operating and investment costs of conventional technologies necessary to bring it to market. However, milli-second reactors operating at a GHSV up to 200 000 h−1 reduce investment. The first step of a gas-to-liquids process produces syngas—a mixture of CO and H2. Here, we propose promoted Ni-based catalysts supported on FeCrAl knitted gauze to partially oxidize CH4 in air to syngas. High syngas selectivities at 1 bar, 700 °C and CH4/O2 ratios of 2.5 to 5 suggests an apparent direct reaction path to CO and H2. Ru promoted catalysts had higher turnover rates in CH4 activation compared to Ni, Ni-Pt and Ni-Pt-Ru. All catalysts containing Pt formed carbon species refractory to air regeneration at 700 °C. 2.25% Ni with 0.1% Ru had the highest CH4 turnover rate (155 mol s−1 mol−1) and CO selectivity (80%) at a CH4/O2 ratio 2.5. CH4 conversion and CO production were constant after 50 reaction-regeneration cycles that dosed the catalyst for 25 min with methane/air followed by an equal time in air at the same reaction temperature.",

keywords = "CPOX, FeCrAl, Gauze, Natural gas, Ni/CeO, Syngas",

author = "Gianluca Pauletto and Nicole Libretto and Boffito, {Daria C.} and Miller, {Jeffrey T.} and Andreas Jentys and Patience, {Gregory S.} and Lercher, {Johannes A.}",

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T1 - Ni/CeO2 promoted Ru and Pt supported on FeCrAl gauze for cycling methane catalytic partial oxidation—CPOX

AU - Pauletto, Gianluca

AU - Libretto, Nicole

AU - Boffito, Daria C.

AU - Miller, Jeffrey T.

AU - Jentys, Andreas

AU - Patience, Gregory S.

AU - Lercher, Johannes A.

PY - 2021/6/5

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N2 - Stranded natural gas is economically unattractive due to high operating and investment costs of conventional technologies necessary to bring it to market. However, milli-second reactors operating at a GHSV up to 200 000 h−1 reduce investment. The first step of a gas-to-liquids process produces syngas—a mixture of CO and H2. Here, we propose promoted Ni-based catalysts supported on FeCrAl knitted gauze to partially oxidize CH4 in air to syngas. High syngas selectivities at 1 bar, 700 °C and CH4/O2 ratios of 2.5 to 5 suggests an apparent direct reaction path to CO and H2. Ru promoted catalysts had higher turnover rates in CH4 activation compared to Ni, Ni-Pt and Ni-Pt-Ru. All catalysts containing Pt formed carbon species refractory to air regeneration at 700 °C. 2.25% Ni with 0.1% Ru had the highest CH4 turnover rate (155 mol s−1 mol−1) and CO selectivity (80%) at a CH4/O2 ratio 2.5. CH4 conversion and CO production were constant after 50 reaction-regeneration cycles that dosed the catalyst for 25 min with methane/air followed by an equal time in air at the same reaction temperature.

AB - Stranded natural gas is economically unattractive due to high operating and investment costs of conventional technologies necessary to bring it to market. However, milli-second reactors operating at a GHSV up to 200 000 h−1 reduce investment. The first step of a gas-to-liquids process produces syngas—a mixture of CO and H2. Here, we propose promoted Ni-based catalysts supported on FeCrAl knitted gauze to partially oxidize CH4 in air to syngas. High syngas selectivities at 1 bar, 700 °C and CH4/O2 ratios of 2.5 to 5 suggests an apparent direct reaction path to CO and H2. Ru promoted catalysts had higher turnover rates in CH4 activation compared to Ni, Ni-Pt and Ni-Pt-Ru. All catalysts containing Pt formed carbon species refractory to air regeneration at 700 °C. 2.25% Ni with 0.1% Ru had the highest CH4 turnover rate (155 mol s−1 mol−1) and CO selectivity (80%) at a CH4/O2 ratio 2.5. CH4 conversion and CO production were constant after 50 reaction-regeneration cycles that dosed the catalyst for 25 min with methane/air followed by an equal time in air at the same reaction temperature.

KW - CPOX

KW - FeCrAl

KW - Gauze

KW - Natural gas

KW - Ni/CeO

KW - Syngas

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Ni/CeO₂ promoted Ru and Pt supported on FeCrAl gauze for cycling methane catalytic partial oxidation—CPOX

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