Mechanism of methanol synthesis from CO2/CO/H2 mixtures over copper/zinc oxide/alumina catalysts: use of14C-labelled reactants

Chinchen, G.C.; Denny, P. J.; Parker, David G.; Spencer, Michael S.; Whan, David A.

doi:10.1016/s0166-9834(00)84123-8

Cited by 483 publications

(180 citation statements)

References 10 publications

Supporting

Mentioning

168

Contrasting

Order By: Relevance

“…As reported by Klier [1] and Chinchen et al [37], the presence of a small amount of CO, in the synthesis gas used appears to be beneficial to the rate of synthesis of methanol. Fink [35] has shown (see above) that CO, decreased the rate of formation of alcohols higher than methanol over a Cu/ZnO catalyst, and Tronconi et al [38] reported the same behaviour using a Zn-Cr-K-oxide catalyst.…”

Section: The Influence Of Process Variables On the Catalyst Selectivitymentioning

confidence: 66%

The synthesis of higher alcohols using modified Cu/ZnO/Al2O3 catalysts

1992

View full text Add to dashboard Cite

This paper gives a review of research work in the synthesis of higher alcohols over catalysts based on Cu/ZnO/Al,O,, emphasizing three main topics: (i) the effect on selectivity of the addition of several compounds to this catalyst, (ii) the effect on selectivity of the reaction conditions used, and (iii) the reaction network leading to the different products found. Although the use of aLkali compounds has been studied most extensively, other corn~un~, for example those containing manganese, also appear to be promising additives. The process conditions are rather critical and this may cause some practical difficulties in industrial plants. An extended aldol condensation mechanism is proposed which can explain the product distribution found.

show abstract

Section: The Influence Of Process Variables On the Catalyst Selectivitymentioning

confidence: 66%

The synthesis of higher alcohols using modified Cu/ZnO/Al2O3 catalysts

1992

View full text Add to dashboard Cite

show abstract

“…While CO was assumed to be the main carbon source in the early years, [6] isotope labeling experiments clearly showed that CO 2 is preferentially hydrogenated to methanol. [1,7] CO can then react with water to form CO 2 via the water-gas-shift reaction, which is easily facilitated on Cu surfaces. Theoretically, however, it is generally found using semi-local density functional theory calculations that the hydrogenation of CO 2 involves intermediates and reaction barriers that are higher in free energy when compared to CO hydrogenation.…”

Section: Main Textmentioning

confidence: 99%

“…This result is at odds with the experimental evidence suggesting that CO 2 is the major source of carbon in methanol over Cu based catalysts. [15,16] The results using the BEEF-vdW functional (red line in figure 1) are quite different. Since this functional accounts for the dispersion forces of adsorbed species, one might expect a stabilization for larger intermediates, e.g.…”

Section: Main Textmentioning

confidence: 99%

CO and CO2 Hydrogenation to Methanol Calculated Using the BEEF-vdW Functional

et al. 2012

View full text Add to dashboard Cite

Hydrogenation of CO and CO 2 to methanol on a stepped Copper surface has been calculated using the BEEF-vdW functional and is compared to values derived with RPBE. It is found that the inclusion of vdW forces in the BEEF-vdW functional yields a better description of CO 2 hydrogenation as compared to RPBE. These differences are significant for a qualitative description of the overall methanol synthesis kinetics and it is suggested that the selectivity with respect to CO and CO 2 is only described correctly with BEEF-vdW.

show abstract

“…Methanol is currently produced from synthesis gas (CO/CO 2 /H 2 ) using a ternary Cu-Zn-Al oxide catalyst at 50±100 bar and 473±523 K [2]. Methanol synthesis from CO 2 /H 2 feed is closely related to the fact that kinetic experiments, using isotope-labelled carbon oxides [3,4] and spectroscopic experiments [5], have demonstrated that under industrial conditions methanol is produced by hydrogenation of CO 2 , with CO merely providing a source of CO 2 and acting as a reducing agent by scavenging surface oxygen. Nevertheless, the ternary catalyst that is active for CO-rich feed-stock is not so active for the CO 2 -rich sources [6,7].…”

Section: Introductionmentioning

confidence: 99%

Untitled

2002

View full text Add to dashboard Cite

Effect of Pd on Cu-Zn catalysts for the hydrogenation of CO2 to methanol López Granados, M.; Melián-Cabrera, I.; Fierro, J.L.G. Take-down policy If you believe that this document breaches copyright please contact us providing details, and we will remove access to the work immediately and investigate your claim.Downloaded from the University of Groningen/UMCG research database (Pure): http://www.rug.nl/research/portal. For technical reasons the number of authors shown on this cover page is limited to 10 maximum. A palladium±copper±zinc catalyst (PdO : CuO : ZnO 2 : 28 : 70), prepared by sequential precipitation of the respective cations, was tested in the hydrogenation of CO 2 at high pressure (conditions: 60 bar, CO 2 : H 2 1 : 3 (molar), WaF 0X0675 kg h/m 3 , 453±513 K). The methanol yield was improved on using this Pd-containing catalyst at all temperatures with respect to the reference copper±zinc catalyst (CuO : ZnO 30 : 70). This improvement was not due to an additional e ect in which palladium was acting as an independent catalytic site but was caused by a synergetic e ect of Pd on the active Cu sites. This e ect was explained in terms of hydrogen spillover and an increased stability against CO 2 oxidation of the surface copper. Therefore, the present contribution not only supports previous literature ®ndings concerning the hydrogen spillover mechanism but also resulted in a complementary view regarding the role of palladium in Pd-modi®ed CuO-ZnO-based catalysts.

show abstract

Mechanism of methanol synthesis from CO2/CO/H2 mixtures over copper/zinc oxide/alumina catalysts: use of14C-labelled reactants

Cited by 483 publications

References 10 publications

The synthesis of higher alcohols using modified Cu/ZnO/Al2O3 catalysts

The synthesis of higher alcohols using modified Cu/ZnO/Al2O3 catalysts

CO and CO2 Hydrogenation to Methanol Calculated Using the BEEF-vdW Functional

Untitled

Contact Info

Product

Resources

About