Influence of forced feed composition cycling on the rate of ammonia synthesis over an industrial iron catalyst part I — Effect of cycling parameters and mean composition

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Abstract
Studies have been carried out at 2.38 MPa total pressure and at 360 and 400°C of the synthesis of ammonia over a triply‐promoted iron catalyst (United Catalysts Inc.). Runs were carried out using a gradientless reactor in steady‐state and periodic modes, the latter employing forced composition cycling. The catalyst had a particle diameter of 0.30 mm; the resulting reaction rates were free from transport intrusions. The range of mean compositions for steady‐state measurements was from 0.1 to 0.9 mole fraction of hydrogen and for periodic operation from 0.5 to 0.9. The cycle‐split ratio (used to describe non‐uniform cycling) varied from 0.2 to 0.85. Effects of cycle period, mean composition, cycle‐split, and temperature were investigated. Instantaneous rate variations within the cycle are reported.Results showed that the cycling mode of operation results in an improvement in the time‐average rate of ammonia formation of up to 30%, depending upon the choice of operating parameters. Some implications for the mechanism of ammonia synthesis under periodic operation are presented.