One-pot sol-gel synthesis of Ni/TiO2 catalysts for methane decomposition into COx free hydrogen and multiwalled carbon nanotubes

Manoj Pudukudy, Zahira Yaakob, Abudukeremu Kadier, Mohd Sobri Takriff, Nik Suhaimi Mat Hassan

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11 Citations (Scopus)

Abstract

A series of mesoporous Ni/TiO2 catalysts with different loadings of nickel from 10 to 50 wt% was successfully prepared via a facile one-pot sol-gel route; characterized for its structural, textural and redox properties; and tested for the non-oxidative thermocatalytic decomposition of undiluted methane for the first time. The characterization results reveal the presence of both NiO and NiTiO3 and metallic nickel as active metal phase in the fresh and reduced catalysts, respectively. Spherical catalyst particles were found to be highly inter-aggregated and to provide a porous texture to the catalyst. All of the prepared catalysts exhibited high catalytic activity and stability for methane decomposition. It is due to the fine dispersion of active nickel nanoparticles on the surface of the TiO2 support with proper metal-support interaction. Moreover, with increasing nickel loading and reaction temperature, the yields of hydrogen and nanocarbon were found to be significantly increased. A maximum hydrogen yield of 56% and a final carbon yield of 1544% were obtained for the 50% Ni/TiO2 catalyst at 700 °C with an undiluted methane feed of 150 ml/min for 360 min of time on stream. The catalyst showed high catalyst stability, for a period of 960 min of time on stream and ∼24% hydrogen yield was observed at the end of long-term run using the 50% Ni/TiO2 catalyst. Moreover, irrespective of the nickel loading involved, bulk amount of multiwalled carbon nanotubes were deposited on the surface of the catalyst. XRD and Raman analyses of the spent catalysts showed that the crystallinity of nanocarbon increased with increasing nickel loadings, whereas the graphitization degree remained unaffected, with an ID/IG value of 0.88.

Original languageEnglish
JournalInternational Journal of Hydrogen Energy
DOIs
Publication statusAccepted/In press - 10 Mar 2017

Fingerprint

Multiwalled carbon nanotubes (MWCN)
Sol-gels
Methane
methane
carbon nanotubes
gels
Decomposition
decomposition
catalysts
Hydrogen
Catalysts
hydrogen
synthesis
Nickel
nickel
Graphitization
graphitization
Metals
metals
catalytic activity

Keywords

  • Catalytic conversion
  • Graphitization degree
  • Hydrogen
  • Multiwalled carbon nanotubes
  • Sol-gel method
  • Titania supported nickel

ASJC Scopus subject areas

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

Cite this

@article{749825bd0d8b4e69b584f7f9bc28db22,
title = "One-pot sol-gel synthesis of Ni/TiO2 catalysts for methane decomposition into COx free hydrogen and multiwalled carbon nanotubes",
abstract = "A series of mesoporous Ni/TiO2 catalysts with different loadings of nickel from 10 to 50 wt{\%} was successfully prepared via a facile one-pot sol-gel route; characterized for its structural, textural and redox properties; and tested for the non-oxidative thermocatalytic decomposition of undiluted methane for the first time. The characterization results reveal the presence of both NiO and NiTiO3 and metallic nickel as active metal phase in the fresh and reduced catalysts, respectively. Spherical catalyst particles were found to be highly inter-aggregated and to provide a porous texture to the catalyst. All of the prepared catalysts exhibited high catalytic activity and stability for methane decomposition. It is due to the fine dispersion of active nickel nanoparticles on the surface of the TiO2 support with proper metal-support interaction. Moreover, with increasing nickel loading and reaction temperature, the yields of hydrogen and nanocarbon were found to be significantly increased. A maximum hydrogen yield of 56{\%} and a final carbon yield of 1544{\%} were obtained for the 50{\%} Ni/TiO2 catalyst at 700 °C with an undiluted methane feed of 150 ml/min for 360 min of time on stream. The catalyst showed high catalyst stability, for a period of 960 min of time on stream and ∼24{\%} hydrogen yield was observed at the end of long-term run using the 50{\%} Ni/TiO2 catalyst. Moreover, irrespective of the nickel loading involved, bulk amount of multiwalled carbon nanotubes were deposited on the surface of the catalyst. XRD and Raman analyses of the spent catalysts showed that the crystallinity of nanocarbon increased with increasing nickel loadings, whereas the graphitization degree remained unaffected, with an ID/IG value of 0.88.",
keywords = "Catalytic conversion, Graphitization degree, Hydrogen, Multiwalled carbon nanotubes, Sol-gel method, Titania supported nickel",
author = "Manoj Pudukudy and Zahira Yaakob and Abudukeremu Kadier and Takriff, {Mohd Sobri} and Hassan, {Nik Suhaimi Mat}",
year = "2017",
month = "3",
day = "10",
doi = "10.1016/j.ijhydene.2017.04.223",
language = "English",
journal = "International Journal of Hydrogen Energy",
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TY - JOUR

T1 - One-pot sol-gel synthesis of Ni/TiO2 catalysts for methane decomposition into COx free hydrogen and multiwalled carbon nanotubes

AU - Pudukudy, Manoj

AU - Yaakob, Zahira

AU - Kadier, Abudukeremu

AU - Takriff, Mohd Sobri

AU - Hassan, Nik Suhaimi Mat

PY - 2017/3/10

Y1 - 2017/3/10

N2 - A series of mesoporous Ni/TiO2 catalysts with different loadings of nickel from 10 to 50 wt% was successfully prepared via a facile one-pot sol-gel route; characterized for its structural, textural and redox properties; and tested for the non-oxidative thermocatalytic decomposition of undiluted methane for the first time. The characterization results reveal the presence of both NiO and NiTiO3 and metallic nickel as active metal phase in the fresh and reduced catalysts, respectively. Spherical catalyst particles were found to be highly inter-aggregated and to provide a porous texture to the catalyst. All of the prepared catalysts exhibited high catalytic activity and stability for methane decomposition. It is due to the fine dispersion of active nickel nanoparticles on the surface of the TiO2 support with proper metal-support interaction. Moreover, with increasing nickel loading and reaction temperature, the yields of hydrogen and nanocarbon were found to be significantly increased. A maximum hydrogen yield of 56% and a final carbon yield of 1544% were obtained for the 50% Ni/TiO2 catalyst at 700 °C with an undiluted methane feed of 150 ml/min for 360 min of time on stream. The catalyst showed high catalyst stability, for a period of 960 min of time on stream and ∼24% hydrogen yield was observed at the end of long-term run using the 50% Ni/TiO2 catalyst. Moreover, irrespective of the nickel loading involved, bulk amount of multiwalled carbon nanotubes were deposited on the surface of the catalyst. XRD and Raman analyses of the spent catalysts showed that the crystallinity of nanocarbon increased with increasing nickel loadings, whereas the graphitization degree remained unaffected, with an ID/IG value of 0.88.

AB - A series of mesoporous Ni/TiO2 catalysts with different loadings of nickel from 10 to 50 wt% was successfully prepared via a facile one-pot sol-gel route; characterized for its structural, textural and redox properties; and tested for the non-oxidative thermocatalytic decomposition of undiluted methane for the first time. The characterization results reveal the presence of both NiO and NiTiO3 and metallic nickel as active metal phase in the fresh and reduced catalysts, respectively. Spherical catalyst particles were found to be highly inter-aggregated and to provide a porous texture to the catalyst. All of the prepared catalysts exhibited high catalytic activity and stability for methane decomposition. It is due to the fine dispersion of active nickel nanoparticles on the surface of the TiO2 support with proper metal-support interaction. Moreover, with increasing nickel loading and reaction temperature, the yields of hydrogen and nanocarbon were found to be significantly increased. A maximum hydrogen yield of 56% and a final carbon yield of 1544% were obtained for the 50% Ni/TiO2 catalyst at 700 °C with an undiluted methane feed of 150 ml/min for 360 min of time on stream. The catalyst showed high catalyst stability, for a period of 960 min of time on stream and ∼24% hydrogen yield was observed at the end of long-term run using the 50% Ni/TiO2 catalyst. Moreover, irrespective of the nickel loading involved, bulk amount of multiwalled carbon nanotubes were deposited on the surface of the catalyst. XRD and Raman analyses of the spent catalysts showed that the crystallinity of nanocarbon increased with increasing nickel loadings, whereas the graphitization degree remained unaffected, with an ID/IG value of 0.88.

KW - Catalytic conversion

KW - Graphitization degree

KW - Hydrogen

KW - Multiwalled carbon nanotubes

KW - Sol-gel method

KW - Titania supported nickel

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U2 - 10.1016/j.ijhydene.2017.04.223

DO - 10.1016/j.ijhydene.2017.04.223

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JO - International Journal of Hydrogen Energy

JF - International Journal of Hydrogen Energy

SN - 0360-3199

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