Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases p. 2193 - 2212 (1987)
Update date:2022-08-17
Topics:
Chinchen, Godfrey C.
Spencer, Michael S.
Waugh, Kenneth C.
Whan, David A.
The surfaces of the copper metal crystallites of working Cu/ZuO/Al2O3 and other copper catalysts are partially oxidised in reaction mixtures for methanol synthesis and the water-gas shift reaction.Work with unsupported polycrystalline copper has confirmed earlier results that copper metal is the active phase in supported copper catalysts.The coverage of adsorbed oxygen, O(a), up to half-monolayer, was determined by reaction with N2O and it was found to be controlled by the overall reaction CO2(g) = CO(g) + O(a).The free energy of formationn of O(a) was calculated to be -240 kJ mol-1 at 513 K.The induction period found in methanol synthesis from CO-CO2-H2 mixtures is consistent with the calculated rate of formation of O(a).The role of O(a) in the methanol synthesis and water-gas shift reactions is both as promoter and reaction intermediate.The dissociative chemisorption of hydrogen on copper is promoted by O(a) but this is not nesessary for the reactions.Experiments with unsupported polycrystalline copper have shown that O(a) both increases the extent of physisorption of CO2 and creates new chemisorbed states of CO2, with desorption energies of 109, 113 and 125 kJ mol-1.O(a) is also essential for the dissociative chemisorption of water on copper.A regenerative mechanism for the water-gas shift reaction on copper
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