In situ IR study for elucidating reaction mechanism of toluene steam reforming over Ni/La0.7Sr0.3AlO3−δ catalyst

Mukai, Daiki; Murai, Yuki; Higo, Takuma; Tochiya, Satoshi; Hashimoto, Takashi; Sugiura, Yukihiro; Sekine, Yasushi

doi:10.1016/j.apcata.2013.06.052

Cited by 44 publications

(30 citation statements)

References 47 publications

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“…Peaks for methylcyclohexane were observed at 1564 cm -1 and 1347 cm -1 , similar to the case of n-heptane. However, peaks for toluene 24) were observed at 1594, 1546, and 1401 cm -1 , in contrast to the other catalysts. These differences in the spectra indicate different conditions for the reaction intermediate and variations in the apparent activation energies, as described in section 3.…”

Section: Apparent Activation Energy and Latticementioning

confidence: 62%

“…The desorption peaks on Sr/LAO (i.e. Sr 2 was not incorporated but supported on LAO) appeared at 1509 cm -1 and 1393 cm -1 , which were different to the peaks for toluene on LAO 24) . Therefore, the peaks observed for Sr/LAO adsorption are attributable to the adsorption of toluene on Sr 2 sites.…”

Section: Adsorption Sites On Lsao Supportmentioning

confidence: 96%

“…4) at 1573, 1466, and 1406 cm -1 . The peak at 1466 cm -1 is assigned to the C _ C vibration, and 1406 cm -1 to the COO asymmetric stretching vibration 24) . In addition, adsorption peaks were observed for methylcyclohexane TPD at 1516, 1469, and 1396 cm -1 , and for toluene at 1478 cm -1 and 1400 cm -1 .…”

Section: Apparent Activation Energy and Latticementioning

confidence: 99%

“…The adsorption peaks disappeared at 573 K for n-heptane and methylcyclohexane (Fig. 5), and at 773 K for toluene on Ni/ LAO catalyst 24) . The reactants did not strongly adsorb onto the catalyst, or rapidly desorbed because no peak change was detected from low temperatures to high temperatures on Ni/α-Al2O3 (Fig.…”

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confidence: 99%

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Effect of Hydrocarbon Structure on Steam Reforming over Ni/perovskite Catalyst

Higo

Hashimoto

Mukai

et al. 2015

J. Jpn. Petrol. Inst.

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Ni/perovskite-type oxide catalyst (Ni/La0.7Sr0.3AlO2.85: LSAO) shows high catalytic activity and low carbon formation during the steam reforming of aromatic hydrocarbons because of the high mobility of lattice oxygen in the support. The reaction mechanisms of the catalyst were investigated by characterizations and catalytic activity tests for steam reforming of various hydrocarbons including toluene, methylcyclohexane, and n-heptane. The catalytic performance was affected by the reactant structure, as revealed by Arrhenius plots and FT-IR analyses. Adsorption state and stability of reaction intermediates were very important factors in the catalytic activity for steam reforming.

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Section: Apparent Activation Energy and Latticementioning

confidence: 62%

Section: Adsorption Sites On Lsao Supportmentioning

confidence: 96%

Section: Apparent Activation Energy and Latticementioning

confidence: 99%

mentioning

confidence: 99%

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Effect of Hydrocarbon Structure on Steam Reforming over Ni/perovskite Catalyst

Higo

Hashimoto

Mukai

et al. 2015

J. Jpn. Petrol. Inst.

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“…However, due to the complexity of tar composition, different model molecules representatives of tar have been used in the studies such as benzene, toluene, naphthalene and methylnaphthalene. Nickel-based catalysts have been extensively investigated for the steam reforming (SR) of toluene due to the high activity of Ni for C-C bond breaking and its low cost [3][4][5][6][7][8][9][10][11][12][13][14][15][16][17]. However, nickel catalysts undergo significant deactivation during steam reforming of toluene, mainly attributed to carbon deposition.…”

Section: Introductionmentioning

confidence: 99%

Steam Reforming of Toluene Over Pt/Ce x Zr1−x O2/Al2O3 Catalysts

et al. 2015

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Steam reforming of toluene was investigated over Pt/Ce x Zr 1-x O 2 /Al 2 O 3 catalysts with different ceria and zirconia content (x = 0.25, 0.50, 0.75, and 1.00). Toluene was used as model molecule representative of tar produced in biomass gasification. The main reactions over Pt/Ce x Zr 1-x O 2 /Al 2 O 3 catalysts are the steam reforming of toluene and the water-gas shift. The dealkylation of toluene to benzene and methane takes place only at the beginning of the reaction. Toluene conversion significantly decreases during the reaction for all catalysts excepted for Pt/CeO 2 /Al 2 O 3 catalyst. Catalyst deactivation was attributed to carbon deposition as revealed by Raman spectroscopy. A clear relationship is observed between the acidity of the catalyst and the amount of carbon formed over Pt/Ce x Zr 1-x O 2 /Al 2 O 3 catalysts. Decreasing the Ce/Zr ratio increased the density of acid sites as well as the amount of carbon formed. This result suggests that the main route for carbon deposition proceeds by the oligomerization of toluene molecule on the acid sites of the support. Pt/CeO 2 /Al 2 O 3 catalyst was quite stable during steam reforming of toluene without carbon deposition. For this catalyst, ceria covered the acid sites of alumina and did not introduce significant Lewis acid sites.

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Mechanism and kinetic modeling for steam reforming of toluene on La_0.8Sr_0.2Ni_0.8Fe_0.2O₃ catalyst

Oemar

Hidajat

et al. 2014

AIChE Journal

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Reaction mechanism for steam reforming of toluene is proposed for La0.8Sr0.2Ni0.8Fe0.2O3 perovskite catalyst. The proposed mechanism was derived from various characterization results such as temperature‐programmed desorption (TPD) and temperature‐programmed surface reaction (TPSR) water, TPSR toluene, TPD O2 and in situ DRIFT of toluene decomposition, and steam reforming of toluene. Five kinetic models were developed based on the proposed dual‐site reaction mechanism using Langmuir–Hinshelwood approach. Subsequently, the parameters of the kinetic models were estimated by nonlinear least square regression. A good agreement was obtained between experimental and model predicted results for the rate determining step based on reaction between adsorbed aldehyde and adsorbed oxygen. The adsorbed aldehyde species is produced from the reaction between adsorbed C2H2 or CH2 and adsorbed oxygen while the adsorbed oxygen species can come from the oxygen from water activation, lattice oxygen species, and/or the redox property of some metals such as Fe. This shows that the adsorbed oxygen species plays important role in this reaction. © 2014 American Institute of Chemical Engineers AIChE J 60: 4190–4198, 2014

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In situ IR study for elucidating reaction mechanism of toluene steam reforming over Ni/La0.7Sr0.3AlO3−δ catalyst

Cited by 44 publications

References 47 publications

Effect of Hydrocarbon Structure on Steam Reforming over Ni/perovskite Catalyst

Effect of Hydrocarbon Structure on Steam Reforming over Ni/perovskite Catalyst

Steam Reforming of Toluene Over Pt/Ce x Zr1−x O2/Al2O3 Catalysts

Mechanism and kinetic modeling for steam reforming of toluene on La_0.8Sr_0.2Ni_0.8Fe_0.2O₃ catalyst

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In situ IR study for elucidating reaction mechanism of toluene steam reforming over Ni/La0.7Sr0.3AlO3−δ catalyst

Cited by 44 publications

References 47 publications

Effect of Hydrocarbon Structure on Steam Reforming over Ni/perovskite Catalyst

Effect of Hydrocarbon Structure on Steam Reforming over Ni/perovskite Catalyst

Steam Reforming of Toluene Over Pt/Ce x Zr1−x O2/Al2O3 Catalysts

Mechanism and kinetic modeling for steam reforming of toluene on La0.8Sr0.2Ni0.8Fe0.2O3 catalyst

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Mechanism and kinetic modeling for steam reforming of toluene on La_0.8Sr_0.2Ni_0.8Fe_0.2O₃ catalyst