Methane decomposition into COx free hydrogen and multiwalled carbon nanotubes over ceria, zirconia and lanthana supported nickel catalysts prepared via a facile solid state citrate fusion method

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Abstract

Methane decomposition is the most effective route for the simultaneous production of COx-free hydrogen and nanocarbon. In this work, a set of porous ceria, zirconia and lanthana supported nickel catalysts were successfully synthesized via a facile solid state citrate fusion method and used for the thermocatalytic decomposition of undiluted methane for the first time. The catalysts were completely characterized for their crystalline, structural, textural and reduction properties and correlated to their catalytic performance. The active phase of fresh catalysts was found to be NiO in the CeO2 and ZrO2 supported catalysts whereas the formation of lanthanum nickel oxide solid solution was observed in the Ni/La2O3 catalyst. Various attractive porous morphologies of the fresh catalysts were confirmed by scanning electron microscopic studies. All of the catalysts exhibited high catalytic activity and stability for methane decomposition. The yield of hydrogen and carbon increased significantly with increasing the reaction temperature from 600 °C to 700 °C. A maximum initial hydrogen yield of 62%, 61% and 58% and a final carbon yield of 1360 wt%, 1159 wt% and 1576 wt% was achieved over ceria, zirconia and lanthana supported catalysts respectively, at 700 °C. The surface area of the catalysts could not have any significant effect on the catalytic efficiency and it was fully depended on the metal support interaction. The Ni/La2O3 catalyst showed high catalytic stability than ceria and zirconia supported catalysts due to the enhanced surface dispersion of finely crystallized Ni nanoparticles on the lanthana matrix aroused by the reduction of lanthanum nickel oxide. Moreover, bulk deposition of highly uniform multiwalled carbon nanotubes with high graphitization degree (ID/IG = 0.95) with different diameters depending on the Ni crystalline size was observed over the catalysts.

Original languageEnglish
Pages (from-to)302-315
Number of pages14
JournalEnergy Conversion and Management
Volume126
DOIs
Publication statusPublished - 15 Oct 2016

Fingerprint

Multiwalled carbon nanotubes (MWCN)
Cerium compounds
Lanthanum
Zirconia
Methane
Fusion reactions
Nickel
Decomposition
Hydrogen
Catalysts
Catalyst supports
Lanthanum oxides
Nickel oxide
Crystalline materials
Graphitization
Carbon
Solid solutions
Catalyst activity
Nanoparticles
Scanning

Keywords

  • Hydrogen
  • Methane cracking
  • Multiwalled carbon nanotubes
  • Nickel
  • Rare earth supports
  • Solid state citrate fusion

ASJC Scopus subject areas

  • Renewable Energy, Sustainability and the Environment
  • Nuclear Energy and Engineering
  • Fuel Technology
  • Energy Engineering and Power Technology

Cite this

@article{06c7aaaa69d34f438193c4d5d80fe9ec,
title = "Methane decomposition into COx free hydrogen and multiwalled carbon nanotubes over ceria, zirconia and lanthana supported nickel catalysts prepared via a facile solid state citrate fusion method",
abstract = "Methane decomposition is the most effective route for the simultaneous production of COx-free hydrogen and nanocarbon. In this work, a set of porous ceria, zirconia and lanthana supported nickel catalysts were successfully synthesized via a facile solid state citrate fusion method and used for the thermocatalytic decomposition of undiluted methane for the first time. The catalysts were completely characterized for their crystalline, structural, textural and reduction properties and correlated to their catalytic performance. The active phase of fresh catalysts was found to be NiO in the CeO2 and ZrO2 supported catalysts whereas the formation of lanthanum nickel oxide solid solution was observed in the Ni/La2O3 catalyst. Various attractive porous morphologies of the fresh catalysts were confirmed by scanning electron microscopic studies. All of the catalysts exhibited high catalytic activity and stability for methane decomposition. The yield of hydrogen and carbon increased significantly with increasing the reaction temperature from 600 °C to 700 °C. A maximum initial hydrogen yield of 62{\%}, 61{\%} and 58{\%} and a final carbon yield of 1360 wt{\%}, 1159 wt{\%} and 1576 wt{\%} was achieved over ceria, zirconia and lanthana supported catalysts respectively, at 700 °C. The surface area of the catalysts could not have any significant effect on the catalytic efficiency and it was fully depended on the metal support interaction. The Ni/La2O3 catalyst showed high catalytic stability than ceria and zirconia supported catalysts due to the enhanced surface dispersion of finely crystallized Ni nanoparticles on the lanthana matrix aroused by the reduction of lanthanum nickel oxide. Moreover, bulk deposition of highly uniform multiwalled carbon nanotubes with high graphitization degree (ID/IG = 0.95) with different diameters depending on the Ni crystalline size was observed over the catalysts.",
keywords = "Hydrogen, Methane cracking, Multiwalled carbon nanotubes, Nickel, Rare earth supports, Solid state citrate fusion",
author = "Manoj Pudukudy and Zahira Yaakob and Takriff, {Mohd Sobri}",
year = "2016",
month = "10",
day = "15",
doi = "10.1016/j.enconman.2016.08.006",
language = "English",
volume = "126",
pages = "302--315",
journal = "Energy Conversion and Management",
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T1 - Methane decomposition into COx free hydrogen and multiwalled carbon nanotubes over ceria, zirconia and lanthana supported nickel catalysts prepared via a facile solid state citrate fusion method

AU - Pudukudy, Manoj

AU - Yaakob, Zahira

AU - Takriff, Mohd Sobri

PY - 2016/10/15

Y1 - 2016/10/15

N2 - Methane decomposition is the most effective route for the simultaneous production of COx-free hydrogen and nanocarbon. In this work, a set of porous ceria, zirconia and lanthana supported nickel catalysts were successfully synthesized via a facile solid state citrate fusion method and used for the thermocatalytic decomposition of undiluted methane for the first time. The catalysts were completely characterized for their crystalline, structural, textural and reduction properties and correlated to their catalytic performance. The active phase of fresh catalysts was found to be NiO in the CeO2 and ZrO2 supported catalysts whereas the formation of lanthanum nickel oxide solid solution was observed in the Ni/La2O3 catalyst. Various attractive porous morphologies of the fresh catalysts were confirmed by scanning electron microscopic studies. All of the catalysts exhibited high catalytic activity and stability for methane decomposition. The yield of hydrogen and carbon increased significantly with increasing the reaction temperature from 600 °C to 700 °C. A maximum initial hydrogen yield of 62%, 61% and 58% and a final carbon yield of 1360 wt%, 1159 wt% and 1576 wt% was achieved over ceria, zirconia and lanthana supported catalysts respectively, at 700 °C. The surface area of the catalysts could not have any significant effect on the catalytic efficiency and it was fully depended on the metal support interaction. The Ni/La2O3 catalyst showed high catalytic stability than ceria and zirconia supported catalysts due to the enhanced surface dispersion of finely crystallized Ni nanoparticles on the lanthana matrix aroused by the reduction of lanthanum nickel oxide. Moreover, bulk deposition of highly uniform multiwalled carbon nanotubes with high graphitization degree (ID/IG = 0.95) with different diameters depending on the Ni crystalline size was observed over the catalysts.

AB - Methane decomposition is the most effective route for the simultaneous production of COx-free hydrogen and nanocarbon. In this work, a set of porous ceria, zirconia and lanthana supported nickel catalysts were successfully synthesized via a facile solid state citrate fusion method and used for the thermocatalytic decomposition of undiluted methane for the first time. The catalysts were completely characterized for their crystalline, structural, textural and reduction properties and correlated to their catalytic performance. The active phase of fresh catalysts was found to be NiO in the CeO2 and ZrO2 supported catalysts whereas the formation of lanthanum nickel oxide solid solution was observed in the Ni/La2O3 catalyst. Various attractive porous morphologies of the fresh catalysts were confirmed by scanning electron microscopic studies. All of the catalysts exhibited high catalytic activity and stability for methane decomposition. The yield of hydrogen and carbon increased significantly with increasing the reaction temperature from 600 °C to 700 °C. A maximum initial hydrogen yield of 62%, 61% and 58% and a final carbon yield of 1360 wt%, 1159 wt% and 1576 wt% was achieved over ceria, zirconia and lanthana supported catalysts respectively, at 700 °C. The surface area of the catalysts could not have any significant effect on the catalytic efficiency and it was fully depended on the metal support interaction. The Ni/La2O3 catalyst showed high catalytic stability than ceria and zirconia supported catalysts due to the enhanced surface dispersion of finely crystallized Ni nanoparticles on the lanthana matrix aroused by the reduction of lanthanum nickel oxide. Moreover, bulk deposition of highly uniform multiwalled carbon nanotubes with high graphitization degree (ID/IG = 0.95) with different diameters depending on the Ni crystalline size was observed over the catalysts.

KW - Hydrogen

KW - Methane cracking

KW - Multiwalled carbon nanotubes

KW - Nickel

KW - Rare earth supports

KW - Solid state citrate fusion

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