Production of higher alcohols from synthesis gas on nickel oxide-based catalysts

Uchiyama, S.; Obayashi, Yasuo; Shibata, Masatoshi; Uchiyama, Tsutomu; Kawata, Noboru; Konishi, Tatsuo

doi:10.1039/c39850001071

Cited by 16 publications

(9 citation statements)

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“…Most catalysts produce a mixture of methanol, methane, hydrocarbons and higher alcohols [38][39][40][41][42]. Activity in methane production is not surprising, since both the AB step (CuNi step) of CuNi 3 and the AA and AB steps of Ni 3 Cu are calculated to have DE C and DE O that are within the region exhibiting high selectivity towards methane.…”

Section: Resultsmentioning

confidence: 95%

CO hydrogenation to methanol on Cu–Ni catalysts: Theory and experiment

Studt

Abild‐Pedersen

et al. 2012

Journal of Catalysis

203

161

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a b s t r a c tWe present density functional theory (DFT) calculations for CO hydrogenation on different transition metal surfaces. Based on the calculations, trends are established over the different monometallic surfaces, and scaling relations of adsorbates and transition states that link their energies to only two descriptors, the carbon oxygen binding energies, are constructed. A micro-kinetic model of CO hydrogenation is developed and a volcano-shaped relation based on the two descriptors is obtained for methanol synthesis. A large number of bimetallic alloys with respect to the two descriptors are screened, and CuNi alloys of different surface composition are identified as potential candidates. These alloys, proposed by the theoretical predictions, are prepared using an incipient wetness impregnation method and tested in a highpressure fixed-bed reactor at 100 bar and 250-300°C. The activity based on surface area of the active material is comparable to that of the industrially used Cu/ZnO/Al 2 O 3 catalyst. We employ a range of characterization tools such as inductively coupled plasma optical emission spectroscopy (ICP-OES) analysis, in situ X-ray diffraction (XRD) and in situ transmission electron microscope (TEM) to identify the structure of the catalysts.

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Section: Resultsmentioning

confidence: 95%

CO hydrogenation to methanol on Cu–Ni catalysts: Theory and experiment

Studt

Abild‐Pedersen

et al. 2012

Journal of Catalysis

203

161

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“…It is interesting to note that the support effect on ethanol and acetaldehyde selectivity on Rh catalysts has also been observed on the co-precipitated Ni catalysts, as shown in figure 4. Rh supported on ZnO and Ni co-precipitated with Zn precursors have been shown to have excellent selectivity toward methanol; both Rh on TiO 2 and Ni co-precipitated with Ni nitrate exhibit high C 2 oxygenate selectivity [47].…”

Section: + Oxygenate Synthesismentioning

confidence: 99%

Mechanism of C2+ oxygenate synthesis on Rh catalysts

2005

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“…[6][7][8] Catalytic properties of bimetallic nanomaterials often differ completely from the constituent elements because of the modification of the surface electronic structure in combination with modified surface morphology. [9] Bimetallic Cu and Ni nanomaterials are of interest in heterogeneous catalysis for a number of reactions, these include methanation, [10] higher alcohol synthesis, [11][12][13] dehydrogena-tion, [14,15] methanol synthesis, [16][17][18][19][20][21] steam reforming, [22][23][24][25] and water-gas shift. [26,27] The structure of Cu-Ni catalysts has been the topic of numerous studies.…”

Section: Introductionmentioning

confidence: 99%

“…[26,27] The structure of Cu-Ni catalysts has been the topic of numerous studies. These catalysts have been prepared by using different preparation methods such as: impregnation, [18,25] coprecipitation, [28] microemulsion, [29] and sol-gel methods, [30] and have been supported on different high surface area materials such as SiO 2 , [18,25,31,32] Al 2 O 3 , [28,33,34] ZnO, [17] TiO 2 , [11,12,35] ZrO 2 , [36,37] CeO 2 , [38] zeolite, [33] and carbon nanotubes. [39] Moreover, the selectivity and/or the activity is reported to change significantly upon variation in the Cu/Ni ratio for reactions such as hydrocarbon hydrogenolysis, [14] steam reforming, [25] CO 2 hydrogenation, [40,41] CO hydrogenation, [17] and water-gas shift.…”

Section: Introductionmentioning

confidence: 99%

In Situ Observation of Cu–Ni Alloy Nanoparticle Formation by X‐Ray Diffraction, X‐Ray Absorption Spectroscopy, and Transmission Electron Microscopy: Influence of Cu/Ni Ratio

Duchstein

Chiarello

et al. 2013

ChemCatChem

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Silica‐supported, bimetallic Cu–Ni nanomaterials were prepared with different ratios of Cu to Ni by incipient wetness impregnation without a specific calcination step before reduction. Different in situ characterization techniques, in particular transmission electron microscopy (TEM), X‐ray diffraction (XRD), and X‐ray absorption spectroscopy (XAS), were applied to follow the reduction and alloying process of Cu–Ni nanoparticles on silica. In situ reduction of Cu–Ni samples with structural characterization by combined synchrotron XRD and XAS reveals a strong interaction between Cu and Ni species, which results in improved reducibility of the Ni species compared with monometallic Ni. At high Ni concentrations silica‐supported Cu–Ni alloys form a homogeneous solid solution of Cu and Ni, whereas at lower Ni contents Cu and Ni are partly segregated and form metallic Cu and Cu–Ni alloy phases. Under the same reduction conditions, the particle sizes of reduced Cu–Ni alloys decrease with increasing Ni content. Estimates of the metal surface area from sulfur chemisorption and from the XRD particle size generally agree well on the trend across the composition range, but show some disparity in terms of the absolute magnitude of the metal area. This work provides practical synthesis guidelines towards preparation of Cu–Ni alloy nanomaterials with different Cu/Ni ratios, and insight into the application of different in situ techniques for characterization of the alloy formation.

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Production of higher alcohols from synthesis gas on nickel oxide-based catalysts

Cited by 16 publications

References 0 publications

CO hydrogenation to methanol on Cu–Ni catalysts: Theory and experiment

CO hydrogenation to methanol on Cu–Ni catalysts: Theory and experiment

Mechanism of C2+ oxygenate synthesis on Rh catalysts

In Situ Observation of Cu–Ni Alloy Nanoparticle Formation by X‐Ray Diffraction, X‐Ray Absorption Spectroscopy, and Transmission Electron Microscopy: Influence of Cu/Ni Ratio

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