Chemisorption of methane on silica-supported nickel catalysts: A magnetic and infrared study

Kuijpers, E.G.M.; Breedijk, A.K.; Wal, W.J.J. van der; Geus, J.W.

doi:10.1016/0021-9517(81)90003-8

Cited by 36 publications

(3 citation statements)

References 5 publications

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“…Comparison of the area under the curve shows that H 2 desorbed for the 13.5Ni/Al 2 O 3 catalyst is higher compared to that of the promoted catalysts, in agreement with the results of pulse chemisorption. The existence of Ni−H has been proven by Kuijpers et al The results of H 2 -TPD revealed that the Ni−H bonds on promoted catalysts are fewer and weaker than those of 13.5Ni/Al 2 O 3 catalyst because of stronger interaction between Ni and the support for the promoted catalysts which leads to weakening of the Ni−H bond. Studies of Monteiro et al also demonstrated that the addition of CeO 2 to Pd/Al 2 O 3 catalyst would decrease H 2 uptake and diminish the H/Pd ratio.…”

Section: Resultsmentioning

confidence: 93%

Characterization and Activity of K, CeO₂, and Mn Promoted Ni/Al₂O₃Catalysts for Carbon Dioxide Reforming of Methane

Pechimuthu

Pant

Dhingra

et al. 2006

Ind. Eng. Chem. Res.

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Reforming of methane with carbon dioxide into syngas over Ni/γ-Al2O3 catalysts modified by potassium, MnO, and CeO2 was studied. The catalysts were prepared by impregnation technique and were characterized by BET surface area, pore volume, X-ray diffraction, scanning electron microscopy, transmission electron microscopy, temperature-programmed studies, and pulse chemisorption. The performance of these catalysts was evaluated by conducting the reforming reaction in a fixed-bed reactor. Results of the investigation suggested that stable Ni/Al2O3 catalysts for the carbon dioxide reforming of methane can be prepared by the addition of both potassium and CeO2 (or MnO) as promoters. The results of the various characterization techniques were used to relate the observed catalytic activity and stability to the catalyst property. The stability and lower amounts of coking on promoted catalysts were attributed to partial coverage of the surface of nickel by patches of promoters, strong metal−support interaction (TPR, H2 pulse chemisorption, H2-TPD), and their increased CO2 adsorption (CO2-TPD). For the stable 13.5Ni−2K/10CeO2−Al2O3 catalyst, the effect of reaction temperature and contact time on conversion and product yield was studied. It was found that the conversion and product yield increased with increasing reaction temperature and W/F CH 4 ,0 and reached equilibrium at W/F CH 4 ,0 = 1.7 kg-cat·h/kgmethane. The mechanism of the CH4/CO2 reaction has been proposed, based on which a kinetic model was developed to estimate the kinetic parameters. The estimated kinetic parameters predicted the product yields satisfactorily. CH4 activation to form CH x and CH x O decomposition are suggested to be the rate-determining steps of the CH4/CO2 reaction over the 13.5Ni−2K/10CeO2−Al2O3 catalyst. The activation energy for methane adsorption and dissociation (E k 1L ), CH x O decomposition (E k 7L ), and reverse water gas shift reaction (E k r ) were estimated to be 113.8 ± 5.5, 119.3 ± 4.7, and 155.3 ± 7.0 kJ/mol, respectively.

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Section: Resultsmentioning

confidence: 93%

Characterization and Activity of K, CeO₂, and Mn Promoted Ni/Al₂O₃Catalysts for Carbon Dioxide Reforming of Methane

Pechimuthu

Pant

Dhingra

et al. 2006

Ind. Eng. Chem. Res.

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“…It is known that CH 4 only weakly adsorbs on La 2 O 3 39,40 while it easily cracks on metallic Ni at high temperatures. − Thus, it may be anticipated that, with or without the assistance of CO 2 , CH 4 activation (breaking of the C−H bond) favorably occurs on the Ni crystallites, even though the nature of Ni in the working catalyst may be somewhat different from that of metallic Ni. On the other hand, it is known that CO 2 is preferentially adsorbed on La 2 O 3 in the form of La 2 O 2 CO 3 . , The present FTIR results also confirm the formation of La 2 O 2 CO 3 on the Ni/La 2 O 3 catalyst.…”

Section: Discussionmentioning

confidence: 99%

Comparative Study of Carbon Dioxide Reforming of Methane to Synthesis Gas over Ni/La₂O₃and Conventional Nickel-Based Catalysts

et al. 1996

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Carbon dioxide reforming of methane to synthesis gas was studied by employing a Ni/La2O3 catalyst as well as conventional nickel-based catalysts, i.e., Ni/γ-Al2O3, Ni/CaO/γ-Al2O3, and Ni/CaO. It is observed that, in contrast to conventional nickel-based catalysts, which exhibit continuous deactivation with time on stream, the rate of reaction over the Ni/La2O3 catalyst increases during the initial 2−5 h and then tends to be essentially invariable with time on stream. X-ray photoelectron spectroscopy (XPS) studies show that the surface carbon on spent Ni/Al2O3 catalyst is dominated by −C−C− species that eventually block the entire Ni surface, leading to total loss of activity. The surface carbon on the working Ni/La2O3 catalyst is found to consist of −C−C− species and a large amount of oxidized carbon. Both XPS and secondary ion mass spectrometry results reveal that a large fraction of surface Ni on the working Ni/La2O3 catalyst is not shielded by carbon deposition. FTIR studies reveal that the enhancement of the rate of reaction over the Ni/La2O3 catalyst during the initial 2−5 h of reaction correlates well with increasing concentrations of La2O2CO3 and formate species on the support, suggesting that these species may participate in the surface chemistry to produce synthesis gas. It is proposed that the interaction between nickel and lanthanum species creates a new type of synergetic sites at the Ni−La2O3 interfacial area, which offer active and stable performance of carbon dioxide reforming of methane to synthesis gas over the stated catalyst.

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“…Both CH 4 and CO 2 gases were introduced after reduction under H 2 gas. CH 4 was adsorbed on the Ni active sites and dissociated to form adsorbed hydrogen and carbon atoms [41,42]:…”

Section: 9mentioning

confidence: 99%

CO2 dry-reforming of methane over La0.8Sr0.2Ni0.8M0.2O3 perovskite (M = Bi, Co, Cr, Cu, Fe): Roles of lattice oxygen on C–H activation and carbon suppression

Sutthiumporn

Maneerung

Kathiraser

et al. 2012

International Journal of Hydrogen Energy

267

115

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Chemisorption of methane on silica-supported nickel catalysts: A magnetic and infrared study

Cited by 36 publications

References 5 publications

Characterization and Activity of K, CeO₂, and Mn Promoted Ni/Al₂O₃Catalysts for Carbon Dioxide Reforming of Methane

Characterization and Activity of K, CeO₂, and Mn Promoted Ni/Al₂O₃Catalysts for Carbon Dioxide Reforming of Methane

Comparative Study of Carbon Dioxide Reforming of Methane to Synthesis Gas over Ni/La₂O₃and Conventional Nickel-Based Catalysts

CO2 dry-reforming of methane over La0.8Sr0.2Ni0.8M0.2O3 perovskite (M = Bi, Co, Cr, Cu, Fe): Roles of lattice oxygen on C–H activation and carbon suppression

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Chemisorption of methane on silica-supported nickel catalysts: A magnetic and infrared study

Cited by 36 publications

References 5 publications

Characterization and Activity of K, CeO2, and Mn Promoted Ni/Al2O3Catalysts for Carbon Dioxide Reforming of Methane

Characterization and Activity of K, CeO2, and Mn Promoted Ni/Al2O3Catalysts for Carbon Dioxide Reforming of Methane

Comparative Study of Carbon Dioxide Reforming of Methane to Synthesis Gas over Ni/La2O3and Conventional Nickel-Based Catalysts

CO2 dry-reforming of methane over La0.8Sr0.2Ni0.8M0.2O3 perovskite (M = Bi, Co, Cr, Cu, Fe): Roles of lattice oxygen on C–H activation and carbon suppression

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Characterization and Activity of K, CeO₂, and Mn Promoted Ni/Al₂O₃Catalysts for Carbon Dioxide Reforming of Methane

Characterization and Activity of K, CeO₂, and Mn Promoted Ni/Al₂O₃Catalysts for Carbon Dioxide Reforming of Methane

Comparative Study of Carbon Dioxide Reforming of Methane to Synthesis Gas over Ni/La₂O₃and Conventional Nickel-Based Catalysts