Storage models for ammonia synthesis over iron catalyst under periodic operation

Abstract Two models of possible nitrogen storage mechanisms in an iron catalyst during cycling of ammonia synthesis are examined. A surface storage model assumes two kinds of nitrogen adsorption sites on the catalyst surface. It is also assumed that chemical reaction can take place during the surface diffusion of nitrogen atoms between these sites. A bulk dissolution model also assumes dual nitrogen sites. With a well-mixed gas phase, it is shown that the surface storage model and bulk dissolution model can predict enhancement of the time-average production rate of ammonia over the optimal steady-state rate as well as resonance behaviour.

[1]  C. Takoudis,et al.  PERIODIC OPERATION OF CHEMICAL REACTOR SYSTEMS: ARE GLOBAL IMPROVEMENTS ATTAINABLE? , 1986 .

[2]  L. Chiao,et al.  A kinetic study of ammonia synthesis: modeling high-pressure steady-state and forced-cycling behavior , 1989 .

[3]  P. L. Silveston,et al.  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 , 1983 .

[4]  J. Dennis,et al.  Derivative free analogues of the Levenberg-Marquardt and Gauss algorithms for nonlinear least squares approximation , 1971 .

[5]  Albert Renken Unsteady-State Operation of Continuous Reactors , 1982 .

[6]  P. L. Silveston,et al.  Evidence for bulk-phase nitrogen dissolution in iron in catalytic ammonia synthesis† , 1982 .

[7]  P. L. Silveston,et al.  Adsorption/desorption models: How useful for predicting reaction rates under cyclic operation , 1983 .

[8]  P. L. Silveston,et al.  Modelling of non-stationary ammonia synthesis kinetics over an iron catalyst. II: Modelling results of forced feed composition in periodic operation and for step-changes , 1985 .

[9]  M. Boudart Kinetics and Mechanism of Ammonia Synthesis , 1981 .

[10]  Y. Matros,et al.  Unsteady-State Performance of Heterogeneous Catalytic Reactions , 1983 .

[11]  L. Chiao,et al.  CONCENTRATION FORCING IN AMMONIA SYNTHESIS: PLUG-FLOW EXPERIMENTS AT HIGH TEMPERATURE AND PRESSURE , 1987 .

[12]  P. L. Silveston,et al.  Modelling of non‐stationary ammonia synthesis kinetics over an iron catalyst: I. Deriving a model and estimating parameters from transient response data , 1985 .