A new unit operation is presented that utilizes a rapid feed pressure swing cycle in a bed packed with catalyst and adsorbent to effect both reaction and separation. This hybrid device combines features of a cyclic-steady-state pressure swing adsorber with those of a flowforced catalytic reactor. Feed sequences for the periodic separating reactor (PSR) are those of rapid, single-bed pressure swing adsorbers (PSA). Only the case of extremely fast reactions is considered here. A perturbed reaction-sorption equilibrium model is formulated and solved for isothermal operation for different equilibrium constants and reaction stoichiometries. The capacity and separation performance for an equilibrium-limited PSR (EPSR) can be of the same order of magnitude as PSA alone. For reactions involving a single reactant or single product, the principal component in a particular exit stream depends upon both the reaction stoichiometry and feed fraction of the process cycle. The pressure dependency of the reaction equilibrium expression is the cause of separation reversals as parameters are varied.
Forced reactant cycling of carbon monoxide-nitrogen and oxygen-nitrogen streams over Pt-SnO, in a differential reactor results in enhancements of the reaction rate of up to 9 times that of the optimal steady state. Dynamic features common to periodically forced reaction systems were experimentally observed. In addition, quasi-periodic behaviour under forced concentration cycling was also observed. Transient response experiments combined with see-through FTIR analysis confirm an underlying Langmuir-Hinshelwood-type mechanism. Spectral analysis of the quasi-periodic patterns identified at least three time constants of different orders of magnitude. The nature of the patterns also indicated a reaction mechanism which included one or more "reservoirs" of reactants and/or reaction intermediates
The novel combination of a pressure swing adsorber (PSA) with a periodic flow-forced packed-bed reactor is explored. The device provides integral component separation and reaction. Feed sequences studied for the periodic separating reactor (PSR) were those of rapid, single-bed pressure swing adsorption (RPSA). The experimental investigation employed CO oxidation over a packed bed of supported platinum catalyst and molecular sieve adsorbent. A reaction rate limited model is formulated and solved for a variety of irreversible and reversible reactions.The presence of irreversible chemical reaction is shown to greatly enhance the separation achievable by RPSA alone. For a wide range of inlet CO/O, ratios, CO, production could be increased up to two times over steady-state plug-flow reactor operation, while providing a recycle stream without phase change or extractive procedures. Selectivity and conversion improvements were predicted for multiple reaction systems. Other unusual features of operation, such as separation reversals, were also predicted and observed.
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