Non-oxidative thermocatalytic decomposition of methane into COx free hydrogen and nanocarbon over unsupported porous NiO and Fe2O3 catalysts

Manoj Pudukudy, Abudukeremu Kadier, Zahira Yaakob, Mohd Sobri Takriff

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Abstract

The non-oxidative thermal decomposition of methane is one of the most promising routes for the direct production of COx free hydrogen and nanocarbon. In this work, unsupported porous NiO and Fe2O3 catalysts were successfully synthesized by a facile precipitation method using ammonium carbonate as the precipitant and were used for the thermocatalytic decomposition of undiluted methane. The prepared catalysts were characterized for their crystalline, structural and textural properties. The pseudo spherical metal oxide nanoparticles with the size of 10–30 nm were highly inter-aggregated to provide a porous texture to the catalysts. A well packed particle arrangement was observed for the unsupported Fe2O3 catalyst whereas a loose aggregation was observed for the NiO clusters. The catalysts were found to be highly active and stable for the decomposition of methane at various reaction temperatures of 600 °C, 700 °C and 800 °C. A maximum hydrogen yield of 66% and 53% was observed for the NiO and Fe2O3 catalysts respectively for an undiluted methane feed of 150 ml/min at 800 °C. At the end of 360 min of time on stream, the hydrogen yield was measured to be 49% and 46% respectively without deactivation. Moreover, a high catalytic stability was observed for the iron catalyst due to its high carbon diffusion coefficient compared to the nickel catalyst. Bulk deposition of metal encapsulated carbon nanochunks and multilayer graphene sheets were observed over the Ni and Fe catalysts respectively. The structural, crystalline and morphological characterization of the metal dependent nanocarbon were performed by using X-ray diffraction, scanning and transmission electron microscopy, temperature programmed oxidation and Raman analysis. High oxidation stability, crystallinity and graphitization degree was observed for the metal encapsulated carbon nanochunks than the multilayer graphene sheets.

Original languageEnglish
Pages (from-to)18509-18521
Number of pages13
JournalInternational Journal of Hydrogen Energy
Volume41
Issue number41
DOIs
Publication statusPublished - 2 Nov 2016

Fingerprint

Methane
methane
Decomposition
decomposition
catalysts
Hydrogen
Catalysts
hydrogen
Metals
Graphene
Carbon
carbon
graphene
Multilayers
metals
Crystalline materials
Oxidation
oxidation
Graphitization
graphitization

Keywords

  • Graphene sheets
  • Metal encapsulated carbon nanochunks
  • Methane cracking
  • Precipitation
  • Template free synthesis
  • Unsupported catalysts

ASJC Scopus subject areas

  • Renewable Energy, Sustainability and the Environment
  • Fuel Technology
  • Condensed Matter Physics
  • Energy Engineering and Power Technology

Cite this

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title = "Non-oxidative thermocatalytic decomposition of methane into COx free hydrogen and nanocarbon over unsupported porous NiO and Fe2O3 catalysts",
abstract = "The non-oxidative thermal decomposition of methane is one of the most promising routes for the direct production of COx free hydrogen and nanocarbon. In this work, unsupported porous NiO and Fe2O3 catalysts were successfully synthesized by a facile precipitation method using ammonium carbonate as the precipitant and were used for the thermocatalytic decomposition of undiluted methane. The prepared catalysts were characterized for their crystalline, structural and textural properties. The pseudo spherical metal oxide nanoparticles with the size of 10–30 nm were highly inter-aggregated to provide a porous texture to the catalysts. A well packed particle arrangement was observed for the unsupported Fe2O3 catalyst whereas a loose aggregation was observed for the NiO clusters. The catalysts were found to be highly active and stable for the decomposition of methane at various reaction temperatures of 600 °C, 700 °C and 800 °C. A maximum hydrogen yield of 66{\%} and 53{\%} was observed for the NiO and Fe2O3 catalysts respectively for an undiluted methane feed of 150 ml/min at 800 °C. At the end of 360 min of time on stream, the hydrogen yield was measured to be 49{\%} and 46{\%} respectively without deactivation. Moreover, a high catalytic stability was observed for the iron catalyst due to its high carbon diffusion coefficient compared to the nickel catalyst. Bulk deposition of metal encapsulated carbon nanochunks and multilayer graphene sheets were observed over the Ni and Fe catalysts respectively. The structural, crystalline and morphological characterization of the metal dependent nanocarbon were performed by using X-ray diffraction, scanning and transmission electron microscopy, temperature programmed oxidation and Raman analysis. High oxidation stability, crystallinity and graphitization degree was observed for the metal encapsulated carbon nanochunks than the multilayer graphene sheets.",
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T1 - Non-oxidative thermocatalytic decomposition of methane into COx free hydrogen and nanocarbon over unsupported porous NiO and Fe2O3 catalysts

AU - Pudukudy, Manoj

AU - Kadier, Abudukeremu

AU - Yaakob, Zahira

AU - Takriff, Mohd Sobri

PY - 2016/11/2

Y1 - 2016/11/2

N2 - The non-oxidative thermal decomposition of methane is one of the most promising routes for the direct production of COx free hydrogen and nanocarbon. In this work, unsupported porous NiO and Fe2O3 catalysts were successfully synthesized by a facile precipitation method using ammonium carbonate as the precipitant and were used for the thermocatalytic decomposition of undiluted methane. The prepared catalysts were characterized for their crystalline, structural and textural properties. The pseudo spherical metal oxide nanoparticles with the size of 10–30 nm were highly inter-aggregated to provide a porous texture to the catalysts. A well packed particle arrangement was observed for the unsupported Fe2O3 catalyst whereas a loose aggregation was observed for the NiO clusters. The catalysts were found to be highly active and stable for the decomposition of methane at various reaction temperatures of 600 °C, 700 °C and 800 °C. A maximum hydrogen yield of 66% and 53% was observed for the NiO and Fe2O3 catalysts respectively for an undiluted methane feed of 150 ml/min at 800 °C. At the end of 360 min of time on stream, the hydrogen yield was measured to be 49% and 46% respectively without deactivation. Moreover, a high catalytic stability was observed for the iron catalyst due to its high carbon diffusion coefficient compared to the nickel catalyst. Bulk deposition of metal encapsulated carbon nanochunks and multilayer graphene sheets were observed over the Ni and Fe catalysts respectively. The structural, crystalline and morphological characterization of the metal dependent nanocarbon were performed by using X-ray diffraction, scanning and transmission electron microscopy, temperature programmed oxidation and Raman analysis. High oxidation stability, crystallinity and graphitization degree was observed for the metal encapsulated carbon nanochunks than the multilayer graphene sheets.

AB - The non-oxidative thermal decomposition of methane is one of the most promising routes for the direct production of COx free hydrogen and nanocarbon. In this work, unsupported porous NiO and Fe2O3 catalysts were successfully synthesized by a facile precipitation method using ammonium carbonate as the precipitant and were used for the thermocatalytic decomposition of undiluted methane. The prepared catalysts were characterized for their crystalline, structural and textural properties. The pseudo spherical metal oxide nanoparticles with the size of 10–30 nm were highly inter-aggregated to provide a porous texture to the catalysts. A well packed particle arrangement was observed for the unsupported Fe2O3 catalyst whereas a loose aggregation was observed for the NiO clusters. The catalysts were found to be highly active and stable for the decomposition of methane at various reaction temperatures of 600 °C, 700 °C and 800 °C. A maximum hydrogen yield of 66% and 53% was observed for the NiO and Fe2O3 catalysts respectively for an undiluted methane feed of 150 ml/min at 800 °C. At the end of 360 min of time on stream, the hydrogen yield was measured to be 49% and 46% respectively without deactivation. Moreover, a high catalytic stability was observed for the iron catalyst due to its high carbon diffusion coefficient compared to the nickel catalyst. Bulk deposition of metal encapsulated carbon nanochunks and multilayer graphene sheets were observed over the Ni and Fe catalysts respectively. The structural, crystalline and morphological characterization of the metal dependent nanocarbon were performed by using X-ray diffraction, scanning and transmission electron microscopy, temperature programmed oxidation and Raman analysis. High oxidation stability, crystallinity and graphitization degree was observed for the metal encapsulated carbon nanochunks than the multilayer graphene sheets.

KW - Graphene sheets

KW - Metal encapsulated carbon nanochunks

KW - Methane cracking

KW - Precipitation

KW - Template free synthesis

KW - Unsupported catalysts

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DO - 10.1016/j.ijhydene.2016.08.160

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JO - International Journal of Hydrogen Energy

JF - International Journal of Hydrogen Energy

SN - 0360-3199

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