Studies have been carried out between 230 and 270°C and 1.97 and 2.93 MPa total pressure on the synthesis of methanol over an industrial catalyst of the copper‐zinc oxide‐alumina type using a gradientless reactor. Two modes of forced feed composition cycling were explored: periodic variations of the mole fraction of H2 and CO and periodic variation of the CO2 content. The latter mode substantially improved methanol production and suppressed the parasitic formation of methane, while the former mode had just the opposite effect. Measurements of methanol, methane and CO during a cycle as well as separate observations of the response to step‐changes in concentration indicated substantial storage of CO on the catalyst surface. Rapid response of methane to the CO2 content suggests over‐reduced areas of the catalyst surface are responsible for methane formation and that these regions are readily oxidized. CO2 or H2O associated with methane formation appear to relate to the dynamics of methanol formation.
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