Carbon nanospheres as novel support in the nickel catalyzed gas phase hydrogenation of butyronitrile

Nieto-Márquez, Antonio; Toledano, Diana; Lazo, José C.; Romero, Amaya; Valverde, J.L.

doi:10.1016/j.apcata.2009.11.013

Cited by 11 publications

(10 citation statements)

References 40 publications

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“…1400-1600 m 2 g À1 . 36,37 It is worth saying that this value is slightly higher than that exhibited by the pristine spheres (3.6 m 2 g À1 ), as a consequence of annealing. In line with that, differential pore volume distribution of the spheres by DFT has been calculated, suggesting the presence of ultramicropores (see SI 8, ESI †).…”

Section: Resultsmentioning

confidence: 83%

“…0.80, showing a higher degree of graphitization (lower I D /I G ) than most of the other CVD carbon spheres reported to date. 10,33,37,38 Lower I D /I G ratios can be achieved in the presence of MnO 2 or Ni doping. 39,40 In any case, our results are in accordance with the graphitization trend reported by Nieto-Márquez et al: graphite 4 carbon nanotubes/nanofibers 4 carbon nanospheres 4 activated carbon.…”

Section: Resultsmentioning

confidence: 99%

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CVD synthesis of carbon spheres using NiFe-LDHs as catalytic precursors: structural, electrochemical and magnetoresistive properties

et al. 2016

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The gram-scale synthesis of carbon spheres with a diameter of ca. 740 nm has been achieved by means of a chemical vapour deposition method using NiFe-layered double hydroxides as a solid catalytic precursor. The presence of the catalyst (FeNi 3 ) allows controlling the final size distribution, resulting in a monodisperse sample. Their structural properties exhibited a high degree of graphitization according to their I D /I G ratio. In addition, their morphological features were unveiled by FIB-SEM and HRTEM, showing that they are formed by solid inner cores, and presenting labile chain-like structures due to accretion procedures. The solution and posterior sonication of the samples in toluene gave rise to the well-defined isolated spheres. The textural and electrochemical properties of the spheres have been tested showing non-mesoporous structures with a good behaviour as electrode materials for supercapacitors due to the presence of redox functionalities on their surface. Finally, magneto-transport measurements have been carried out, demonstrating semiconductor behaviour, as well as a positive magnetoresistance effect (ca. 72%) for the lowest studied temperature (2 K).

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Section: Resultsmentioning

confidence: 83%

Section: Resultsmentioning

confidence: 99%

CVD synthesis of carbon spheres using NiFe-LDHs as catalytic precursors: structural, electrochemical and magnetoresistive properties

et al. 2016

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“…This is significant given the temporal decline in activity reported in liquid 4 -7,9,54 -56 and gas phase 10,11,18,20 nitrile hydrogenation over supported Pd, 5 -7,9,55,56 Pt, 7,57 Ru, 7 and Ni. 11,19,20 Catalyst deactivation has been ascribed to metal particle agglomeration, 7,10 active site occlusion by amine product(s), 7,10,15,57,58 and catalyst coking associated with the formation of dehydrogenated surface species and carbides. 11,15,19,21 The greater levels of H 2 uptake/release exhibited by Ba -Pd/SiO 2 (Table 1) can account for the observed higher nitrile hydrogenation activity.…”

Section: Butyronitrile Hydrogenation: Thermodynamic Considerationsmentioning

confidence: 97%

“…8. Nieto-Márquez et al 11 reported a maximum rate of butyronitrile hydrogenation over (carbon nanosphere) supported Ni at comparable temperatures (463 K , T , 583 K) that they linked to reactant thermal desorption that decreased surface coverage. Reaction over Ba-Pd/SiO 2 delivered higher nitrile consumption rates with the maximum at a lower temperature (493 K).…”

Section: Butyronitrile Hydrogenation: Temperature Effectsmentioning

confidence: 99%

“…11,19,20 Catalyst deactivation has been ascribed to metal particle agglomeration, 7,10 active site occlusion by amine product(s), 7,10,15,57,58 and catalyst coking associated with the formation of dehydrogenated surface species and carbides. 11,15,19,21 The greater levels of H 2 uptake/release exhibited by Ba -Pd/SiO 2 (Table 1) can account for the observed higher nitrile hydrogenation activity. Product distribution was invariant with conversion ( Fig.…”

Section: Butyronitrile Hydrogenation: Thermodynamic Considerationsmentioning

confidence: 99%

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Production of Butylamine in the Gas Phase Hydrogenation of Butyronitrile over Pd/SiO₂ and Ba-Pd/SiO₂

Hao

Cárdenas‐Lizana

et al. 2015

Catalysis, Structure & Reactivity

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The gas phase (1 atm, 473 -563 K) hydrogenation of butyronitrile has been studied over Pd/SiO 2 and Ba -Pd/SiO 2 . Catalysts characterization involved temperature-programmed reduction (TPR), H 2 /NH 3 chemisorption/temperature programmed desorption (TPD), X-ray diffraction (XRD), and TEM measurements. The incorporation of Ba with Pd resulted in the formation of smaller metal nano-particles (7 vs 28 nm) with a resultant (seven-fold) higher H 2 chemisorption and decreased total surface acidity (from NH 3 chemisorption/TPD).Temperature-related activity maxima were observed for both catalysts and are associated with thermal desorption of the nitrile reactant. Exclusivity to the target butylamine was achieved at T $ 543 K where Ba -Pd/SiO 2 delivered higher selective hydrogenation rate (91 mol h 21 mol Pd 21) than Pd/SiO 2 (54 mol h 21 mol Pd 21 ), attributed to greater availability of surface-reactive hydrogen. Lower surface acidity served to minimize condensation to higher amines. The rate and selectivity to butylamine exceed those previously reported for gas phase operation.

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