The work deals with fundamental analysis of the sorption-enhanced steam methane reforming (SE-SMR) process in which the simultaneous removal of carbon dioxide by hydrotalcite-based chemisorbent is coupled. A two-section reactor model is developed to describe the SE-SMR reactor, decoupling the complexity in process analysis. The model defines two subsequent sections in the reactor: an equilibrium conversion section (upstream) and an adsorption reforming section (downstream). The material balance relationship in the equilibrium conversion section is directly determined by thermodynamic equilibrium calculation, providing an equilibrated atmosphere to the next section. The adsorption reforming section is described using an isothermal multi-component dynamic model into which the SMR reactions and the high-temperature CO2 adsorption are embedded. The multiple requirements (including H-2 purity, H-2 productivity, CH4 conversion enhancement, and carbon oxides concentrations) are taken into account simultaneously so as to analyze and define feasible operation window for producing high-purity hydrogen with ppm-level CO impurity. The performances of the reactors with different dimensions (laboratory-scale and pilot-scale) are explored, highlighting the importance of operation parameter control to the process feasibility. (c) 2005 Elsevier Ltd. All rights reserved.