Effects of Feed Composition and Feed Impurities in the Catalytic Conversion of Syngas to Higher Alcohols over Alkali-Promoted Cobalt–Molybdenum Sulfide

Christensen, Jakob Munkholt; Jensen, Peter Arendt; Jensen, Anker Degn

doi:10.1021/ie200235e

Cited by 48 publications

(22 citation statements)

References 72 publications

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“…A liquid feeding system, described in greater detail elsewhere [19], was used to supply the methanol.…”

Section: Methodsmentioning

confidence: 99%

“…From experiments, Wantuck et al [42] reported a nonlinear Arrhenius behavior, with the rate constant increasing strongly above 600 K. However, their results have been questioned due to possible interference by thermal dissociation of CH 3 O (R19) at the higher temperatures. For this reason, Baulch et al [34] chose to disregard the data from Wantuck et al in their evaluation of k 19 . It is interesting to note that our theoretical rate constant (denoted by the solid line in Fig.…”

Section: Ab Initio Calculationsmentioning

confidence: 99%

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Experimental and Kinetic Modeling Study of Methanol Ignition and Oxidation at High Pressure

Aranda

Christensen

Alzueta

et al. 2013

Int J of Chemical Kinetics

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A detailed chemical kinetic model for oxidation of CH 3 OH at high pressure and intermediate temperatures has been developed and validated experimentally. Ab initio calculations and RRKM analysis were used to obtain rate coefficients for key reactions of CH 2 OH and CH 3 O (dissociation, isomerization, reaction with O 2 ). The experiments, involving CH 3 OH/O 2 mixtures diluted in N 2 , were carried out in a high pressure flow reactor at 600-900 K and 20-100 bar, varying the reaction stoichiometry from very lean to fuel-rich conditions. Under the conditions studied, the onset temperature for methanol oxidation was not dependent on the stoichiometry, while increasing pressure shifted the ignition temperature towards lower values. Model predictions of the present experimental results, as well as Rapid Compression Machine (RCM) data from the literature, were generally satisfactory. The governing reaction pathways have been outlined based on calculations with the kinetic model. Unlike what has been observed for unsaturated hydrocarbons, the oxidation 2 pathways for CH 3 OH under the investigated conditions were very similar to those prevailing at higher temperatures and lower pressures. At the high pressures, the modeling predictions for onset of reaction were particularly sensitive to the CH 3 OH+HO 2 ⇌CH 2 OH+H 2 O 2 reaction.

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“…A liquid feeding system, described in greater detail elsewhere [19], was used to supply the methanol.…”

Section: Methodsmentioning

confidence: 99%

Section: Ab Initio Calculationsmentioning

confidence: 99%

Experimental and Kinetic Modeling Study of Methanol Ignition and Oxidation at High Pressure

Aranda

Christensen

Alzueta

et al. 2013

Int J of Chemical Kinetics

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“…22,23 Fig. 4 shows that the ratio of H 2 /CO rose rapidly when the oxygen concentration was increased.…”

Section: -7mentioning

confidence: 97%

Experimental research on oxygen-enriched gasification of straw in an entrained-flow gasifier

Yang

et al. 2013

Journal of Renewable and Sustainable Energy

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Biomass (straw) gasification with oxygen-enriched air was studied in a lab-scale entrained-flow gasifier. Effects of oxygen concentration (OC), equivalence ratio (ER), and reactor temperature on the produced gas composition, gasification index and tar yield were investigated. Compared with air, oxygen-enriched air as gasifying agent was beneficial to increase the H 2 content, H 2 /CO ratio, and lower heating value (LHV) of the gas, and decrease the yield of tar contained in the flue gas. The H 2 /CO reached 1 when OC was 50%, which was an optimal value for dimethyl ether, methanol, and higher alcohol production in the process of alcohols synthesis. A reference value of OC was given approximately to 40% according to economic consideration. A reference value of ER was given around 0.25 when OC was 40%, achieved a relatively high LHV of 8.2 MJ/Nm 3 and low tar yield of 2.6 mg/g. In addition, high reaction temperature could improve both gas quality and gasification indexes significantly. The better gasification performance achieved in the paper verified that the oxygen-enriched gasification was a good option for the improvement of direct air gasification. V C 2013 AIP Publishing LLC.

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“…The performance of catalysts for CO hydrogenation was evaluated in a fixed-bed continuous-flow reactor (detailed descriptions of the experimental set-up and the experimental procedure have been provided elsewhere) [58][59][60] with an online GC-FID/TCD detection system (6890N from Agilent Technologies). A bubble flow meter was used for the determination of volumetric flow rate of the reactor effluent.…”

Section: Catalyst Activity Testingmentioning

confidence: 99%

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

Studt

Abild‐Pedersen

et al. 2012

Journal of Catalysis

Self Cite

210

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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Effects of Feed Composition and Feed Impurities in the Catalytic Conversion of Syngas to Higher Alcohols over Alkali-Promoted Cobalt–Molybdenum Sulfide

Cited by 48 publications

References 72 publications

Experimental and Kinetic Modeling Study of Methanol Ignition and Oxidation at High Pressure

Experimental and Kinetic Modeling Study of Methanol Ignition and Oxidation at High Pressure

Experimental research on oxygen-enriched gasification of straw in an entrained-flow gasifier

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

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