Abstract
In situ FT-IR spectroscopy allows the methanol synthesis reaction to be investigated under actual industrial conditions of 503 K and 10 MPa. On Cu/SiO2 catalyst formate species were initially formed which were subsequently hydrogenated to methanol. During the reaction a steady state concentration of formate species persisted on the copper. Additionally, a small quantity of gaseous methane was produced. In contrast, the reaction of CO2 and H2 on ZnO/SiO2 catalyst only resulted in the formation of zinc formate species: no methanol was detected. The interaction of CO2 and H2 with Cu/ZnO/SiO2 catalyst gave formate species on both copper and zinc oxide. Methanol was again formed by the hydrogenation of copper formate species. Steady-state concentrations of copper formate existed under actual industrial reaction conditions, and copper formate is the pivotal intermediate for methanol synthesis. Collation of these results with previous data on copper-based methanol synthesis catalysts allowed the formulation of a reaction mechanism.
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References
K. Klier, Adv. Catal. 31 (1982) 243.
J.C.J. Bart and R.P.A. Sneeden, Catal. Today 2 (1987) 1.
G.C. Chinchen, K.C. Waugh and D.A. Whan, Appl. Catal. 25 (1986) 101.
W.X. Pan, R. Cao, D.L. Roberts and G.L. Griffin, J. Catal. 114 (1988) 440.
R. Burch, S.E. Golunski and M.S. Spencer, Catal. Lett. 5 (1990) 55.
G.J.J. Bartley and R. Burch, Appl. Catal. 43 (1988) 141.
R. Burch, R.J. Chappell and S.E. Golunski, J. Chem. Soc. Faraday Trans. I 85 (1989) 3569.
R. Burch, S.E. Golunski and M.S. Spencer, J. Chem. Soc. Faraday Trans. 86 (1990) 2683.
G.C. Chinchen, P.J. Denny, D.G. Parker, G.D. Short, M.S. Spencer, K.C. Waugh and D.A. Whan, Prepr. Am. Chem. Soc. Div. Fuel Chem. 29 (1984) 178.
G.C. Chinchen, P.J. Denny, D.G. Parker and M.S. Spencer, Appl. Catal. 30 (1987) 333.
M. Bowker, R.A. Hadden, H. Houghton, J.N.K. Hyland and K.C. Waugh, J. Catal. 109 (1988) 263.
R. Burch, S. Chalker and J. Pritchard, J. Chem. Soc. Faraday Trans. 87 (1991) 1791.
G.J. Millar, C.H. Rochester and K.C. Waugh, J. Chem. Soc. Faraday Trans., in press.
J.A. Anderson, M.W. McQuire, C.H. Rochester and T. Sweeney, Catal. Today 9 (1991) 23.
G.J. Millar, C.H. Rochester and K.C. Waugh, J. Chem. Soc. Faraday Trans. 87 (1991) 1491.
B.E. Hayden, K. Prince, D.P. Woodruff and A.M. Bradshaw, Surf. Sci. 133 (1983) 589.
R.K. Iler,The Chemistry of Silica (Wiley, New York, 1979).
G.J. Millar, C.H. Rochester and K.C. Waugh, J. Chem. Soc. Faraday Trans. 87 (1991) 2795.
M.W. McQuire, C.H. Rochester and J.A. Anderson, J. Chem. Soc. Faraday Trans. 87 (1991) 1921.
G.J. Millar, C.H. Rochester and K.C. Waugh, J. Chem. Soc. Faraday Trans. 87 (1991) 1467.
G.J. Millar, C.H. Rochester and K.C. Waugh, J. Chem. Soc. Faraday Trans. 87 (1991) 2785.
G.J. Millar, C.H. Rochester, C. Howe and K.C. Waugh, J. Mol. Phys., in press.
D.L. Roberts and G.L. Griffin, J. Catal. 95 (1985) 617.
C. Chauvin, J. Saussey, J.C. Lavalley, H. Idriss, J.P. Hindermann, A. Kiennemann, P. Chaumette and P. Courty, J. Catal. 121 (1990) 56.
A. Ueno, T. Onishi and K. Tamara, Trans. Faraday Soc. 67 (1971) 3585.
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Millar, G.J., Rochester, C.H. & Waugh, K.C. An in situ high pressure FT-IR study of CO2/H2 interactions with model ZnO/SiO2, Cu/SiO2 and Cu/ZnO/SiO2 methanol synthesis catalysts. Catal Lett 14, 289–295 (1992). https://doi.org/10.1007/BF00769666
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DOI: https://doi.org/10.1007/BF00769666