To generate hydrogen, whether as a source of energy or a raw material for a host of downstream products, the most important process used today is the steam reforming of hydrocarbons (SRH). We developed a framework for optimal operational strategy for maximising production through the use of our comprehensive mathematical model, which incorporates non-isothermal, non-isobaric steam reforming process and the side-reactions. In order to maximise reactor productivity via le Chatelier’s principle, we incorporated in situ separation of products in the reactor. The challenging separation step is mediated through the use of efficient adsorbents along with the reactor catalysts.

For our sorption-enhanced SRH reactor, we adopted the linear driving force model for the transient gas uptake into the solid adsorbents and the extended Langmuir isotherm for the adsorption equilibrium. A transient pressure equation was incorporated to account for variable pressure dynamics. The numerical solutions of the model equations for the transient cyclic process were obtained by applying an orthogonal collocation scheme within the method of lines.

Our model predictions compared well with experimental data. The integrated reactor/separator units with variable catalyst/adsorbent distributions were tested for optimal performance. The pressure reaction columns were found to behave as reactor/separators in series. The performances were investigated in terms of the effects of reactor configurations and reactor operating conditions on conversion, selectivity, hydrogen productivity, and the efficiency of CO2 and CO removal from the reaction zone. The distributions of catalyst/adsorbent beds within the reactor were