Oxidative coupling of methane using non-stoichiometric lead hydroxyapatite catalyst mixtures

Jai Hyun Park; Dae Won Lee; Sung Woo Im; Yong Hee Lee; Dong Jin Suh; Ki Won Jun; Kwan Young Lee

doi:10.1016/j.fuel.2011.08.056

Oxidative coupling of methane using non-stoichiometric lead hydroxyapatite catalyst mixtures

Jai Hyun Park, Dae Won Lee, Sung Woo Im, Yong Hee Lee, Dong Jin Suh, Ki Won Jun, Kwan Young Lee

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

29 Citations (Scopus)

Abstract

Lead hydroxyapatite (Pb _xCa _10-x(PO ₄) ₆(OH) ₂, 0 < x ≤ 10) is one of the most active catalysts for oxidative coupling of methane (OCM) to produce ethane and ethylene from natural gas (methane). In this study, we investigated how the OCM activity of a precipitated lead hydroxyapatite is associated with its mixture and non-stoichiometric properties. Lead hydroxyapatite was prepared through aqueous precipitation in the presence of chlorine anions and calcination under helium background at 1073 K, which resulted in a mixture of non-stoichiometric lead hydroxyapatites, each having a different cationic composition (Pb _xCa _10-x). The mixture could be diversified by extracting the chlorines thermally from the chloro-hydroxyapatites of various chlorine contents. The formation of an apatite structure was confirmed through Fourier transform infrared (FT-IR) spectroscopy, X-ray diffraction (XRD), X-ray fluorescence (XRF) and inductively coupled plasma (ICP) analyses. The non-stoichiometric characters of the prepared hydroxyapatites were analyzed through Raman/FT-Raman spectroscopy. The C ₂ selectivities of the prepared catalysts were evaluated at 1048 K with a fixed CH ₄ conversion of 35%. Among the tested catalysts, lead hydroxyapatite, which was obtained by removing chlorines from Pb ₂Ca ₈(PO ₄) ₆(OH) _0.5Cl _1.5, showed a C ₂ selectivity of 62%, and achieved a C ₂ yield of 22% at 1048 K. The OCM activity of the catalyst was mainly associated with its surface basicity, which was investigated using CO ₂-temperature-programmed desorption (TPD) and X-ray photoelectron spectroscopy (XPS) analyses.

Original language	English
Pages (from-to)	433-439
Number of pages	7
Journal	Fuel
Volume	94
DOIs	https://doi.org/10.1016/j.fuel.2011.08.056
Publication status	Published - 2012 Apr

Bibliographical note

Funding Information:
The authors would like to acknowledge funding from the Korea Ministry of Knowledge and Economy through “Project of next-generation novel technology development” of KEIT. Dr. Dae-Won Lee was supported by a Korea University Grant.

Keywords

Ethylene
Lead hydroxyapatite
Natural gas
Oxidative coupling of methane
Partial oxidation

ASJC Scopus subject areas

General Chemical Engineering
Fuel Technology
Energy Engineering and Power Technology
Organic Chemistry

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10.1016/j.fuel.2011.08.056

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title = "Oxidative coupling of methane using non-stoichiometric lead hydroxyapatite catalyst mixtures",

abstract = "Lead hydroxyapatite (Pb xCa 10-x(PO 4) 6(OH) 2, 0 < x ≤ 10) is one of the most active catalysts for oxidative coupling of methane (OCM) to produce ethane and ethylene from natural gas (methane). In this study, we investigated how the OCM activity of a precipitated lead hydroxyapatite is associated with its mixture and non-stoichiometric properties. Lead hydroxyapatite was prepared through aqueous precipitation in the presence of chlorine anions and calcination under helium background at 1073 K, which resulted in a mixture of non-stoichiometric lead hydroxyapatites, each having a different cationic composition (Pb xCa 10-x). The mixture could be diversified by extracting the chlorines thermally from the chloro-hydroxyapatites of various chlorine contents. The formation of an apatite structure was confirmed through Fourier transform infrared (FT-IR) spectroscopy, X-ray diffraction (XRD), X-ray fluorescence (XRF) and inductively coupled plasma (ICP) analyses. The non-stoichiometric characters of the prepared hydroxyapatites were analyzed through Raman/FT-Raman spectroscopy. The C 2 selectivities of the prepared catalysts were evaluated at 1048 K with a fixed CH 4 conversion of 35%. Among the tested catalysts, lead hydroxyapatite, which was obtained by removing chlorines from Pb 2Ca 8(PO 4) 6(OH) 0.5Cl 1.5, showed a C 2 selectivity of 62%, and achieved a C 2 yield of 22% at 1048 K. The OCM activity of the catalyst was mainly associated with its surface basicity, which was investigated using CO 2-temperature-programmed desorption (TPD) and X-ray photoelectron spectroscopy (XPS) analyses.",

keywords = "Ethylene, Lead hydroxyapatite, Natural gas, Oxidative coupling of methane, Partial oxidation",

author = "Park, {Jai Hyun} and Lee, {Dae Won} and Im, {Sung Woo} and Lee, {Yong Hee} and Suh, {Dong Jin} and Jun, {Ki Won} and Lee, {Kwan Young}",

note = "Funding Information: The authors would like to acknowledge funding from the Korea Ministry of Knowledge and Economy through “Project of next-generation novel technology development” of KEIT. Dr. Dae-Won Lee was supported by a Korea University Grant. ",

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doi = "10.1016/j.fuel.2011.08.056",

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T1 - Oxidative coupling of methane using non-stoichiometric lead hydroxyapatite catalyst mixtures

AU - Park, Jai Hyun

AU - Lee, Dae Won

AU - Im, Sung Woo

AU - Lee, Yong Hee

AU - Suh, Dong Jin

AU - Jun, Ki Won

AU - Lee, Kwan Young

N1 - Funding Information: The authors would like to acknowledge funding from the Korea Ministry of Knowledge and Economy through “Project of next-generation novel technology development” of KEIT. Dr. Dae-Won Lee was supported by a Korea University Grant.

PY - 2012/4

Y1 - 2012/4

N2 - Lead hydroxyapatite (Pb xCa 10-x(PO 4) 6(OH) 2, 0 < x ≤ 10) is one of the most active catalysts for oxidative coupling of methane (OCM) to produce ethane and ethylene from natural gas (methane). In this study, we investigated how the OCM activity of a precipitated lead hydroxyapatite is associated with its mixture and non-stoichiometric properties. Lead hydroxyapatite was prepared through aqueous precipitation in the presence of chlorine anions and calcination under helium background at 1073 K, which resulted in a mixture of non-stoichiometric lead hydroxyapatites, each having a different cationic composition (Pb xCa 10-x). The mixture could be diversified by extracting the chlorines thermally from the chloro-hydroxyapatites of various chlorine contents. The formation of an apatite structure was confirmed through Fourier transform infrared (FT-IR) spectroscopy, X-ray diffraction (XRD), X-ray fluorescence (XRF) and inductively coupled plasma (ICP) analyses. The non-stoichiometric characters of the prepared hydroxyapatites were analyzed through Raman/FT-Raman spectroscopy. The C 2 selectivities of the prepared catalysts were evaluated at 1048 K with a fixed CH 4 conversion of 35%. Among the tested catalysts, lead hydroxyapatite, which was obtained by removing chlorines from Pb 2Ca 8(PO 4) 6(OH) 0.5Cl 1.5, showed a C 2 selectivity of 62%, and achieved a C 2 yield of 22% at 1048 K. The OCM activity of the catalyst was mainly associated with its surface basicity, which was investigated using CO 2-temperature-programmed desorption (TPD) and X-ray photoelectron spectroscopy (XPS) analyses.

AB - Lead hydroxyapatite (Pb xCa 10-x(PO 4) 6(OH) 2, 0 < x ≤ 10) is one of the most active catalysts for oxidative coupling of methane (OCM) to produce ethane and ethylene from natural gas (methane). In this study, we investigated how the OCM activity of a precipitated lead hydroxyapatite is associated with its mixture and non-stoichiometric properties. Lead hydroxyapatite was prepared through aqueous precipitation in the presence of chlorine anions and calcination under helium background at 1073 K, which resulted in a mixture of non-stoichiometric lead hydroxyapatites, each having a different cationic composition (Pb xCa 10-x). The mixture could be diversified by extracting the chlorines thermally from the chloro-hydroxyapatites of various chlorine contents. The formation of an apatite structure was confirmed through Fourier transform infrared (FT-IR) spectroscopy, X-ray diffraction (XRD), X-ray fluorescence (XRF) and inductively coupled plasma (ICP) analyses. The non-stoichiometric characters of the prepared hydroxyapatites were analyzed through Raman/FT-Raman spectroscopy. The C 2 selectivities of the prepared catalysts were evaluated at 1048 K with a fixed CH 4 conversion of 35%. Among the tested catalysts, lead hydroxyapatite, which was obtained by removing chlorines from Pb 2Ca 8(PO 4) 6(OH) 0.5Cl 1.5, showed a C 2 selectivity of 62%, and achieved a C 2 yield of 22% at 1048 K. The OCM activity of the catalyst was mainly associated with its surface basicity, which was investigated using CO 2-temperature-programmed desorption (TPD) and X-ray photoelectron spectroscopy (XPS) analyses.

KW - Ethylene

KW - Lead hydroxyapatite

KW - Natural gas

KW - Oxidative coupling of methane

KW - Partial oxidation

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DO - 10.1016/j.fuel.2011.08.056

M3 - Article

AN - SCOPUS:84856717701

SN - 0016-2361

VL - 94

SP - 433

EP - 439

JO - Fuel

JF - Fuel

ER -

Oxidative coupling of methane using non-stoichiometric lead hydroxyapatite catalyst mixtures

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

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