화학공학소재연구정보센터
Chemical Engineering Science, Vol.173, 428-442, 2017
Sorption enhanced steam methane reforming on catalyst-sorbent bifunctional particles: A CFD fluidized bed reactor model
Sorption Enhanced Steam Methane Reforming (SE-SMR) has been proposed as an efficient novel technology to increase hydrogen yield and reduce the environmental footprint in comparison to state of art H-2 production processes. Sorbent/catalyst materials characterized by stable behaviour over multiple reforming/ calcination cycles may ensure to achieve almost stationary operating conditions utilizing a dual fluidized bed system (the reformer and the sorbent regenerator) with a solid circulation loop. Bifunctional, Combined Sorbent-Catalyst Materials (CSCM) are under development to integrate endothermic catalytic reforming and heterogeneous CO2 sorption in one particle, decrease mass and heat transfer resistances and reduce the solid hold-up in the reactors. This paper deals with the numerical simulation of a pilot scale bubbling fluidized bed SE-SMR reactor by means of a Two-Dimensional Computational Fluid-Dynamic (2D CFD) approach. The hydrodynamic picture is supplemented with a comprehensive Particle Grain Model (PGM) previously developed to describe the kinetics of catalytic and sorption functions, and successfully validated with micro-reactor reactivity tests and multi-cycle thermo-gravimetric sorption tests. The effect of repeated carbonationcalcination steps (the "history" of the granular material) is included in the computation of the reactor performance by utilizing the appropriate size of the sorbent grains in the carbonation rate expression. The numerical results show quantitatively the positive influence of carbon dioxide sorption on the reforming process, at different operating conditions, specifically the enhancement of hydrogen yield and reduction of methane residual concentration in the reactor outlet stream. A preliminary validation of CFD simulations is also carried out utilizing experimental data obtained from a pilot scale bubbling fluidized bed SE-SMR reactor (total bed mass approximate to 14 kg). An estimate is provided for the inward heat flow that would be required to operate the reactor in stationary temperature conditions: it is substantially reduced by the exothermic sorption process and could be satisfied by means of the solid circulation loop connecting the SE-SMR reactor to the high temperature calciner in the whole dual fluidized bed system. (C) 2017 Elsevier Ltd. All rights reserved.