A sorption-enhanced water-gas shift (SEWGS) system providing CO2-free synthesis gas (CO + H2) for jet fuel production from pure CO was studied. The water-gas shift (WGS) reaction was catalyzed by a commercial Cu/ZnO/Al2O3 catalyst and carried out with in-situ CO2 removal on a 20 wt% potassium-promoted hydrotalcite-derived sorbent. Catalyst activity was investigated in a fixed bed tubular reactor. Different sorbent materials and treatments were characterized by CO2 chemisorption among other analysis methods to choose a suitable sorbent. Cyclic breakthrough tests in an isothermal packed bed microchannel reactor (PBMR) were performed at significantly lower modified residence times than those reported in literature. A parameter study gave an insight into the effect of pressure, adsorption feed composition, desorption conditions, as well as reactor configuration on breakthrough delay and adsorbed amount of CO2. Special attention was paid to the steam content. The significance of water during adsorption as well as desorption confirmed the existence of different adsorption sites. Various reactor packing concepts showed that the interaction of relatively fast reaction and relatively slow adsorption kinetics plays a key role in the SEWGS process design at low residence time conditions.
Dedicated to Prof. Dr. Thomas Hirth on the occasion of his 60th birthday Synthesis gas (syngas) used for the production of synthetic fuels may contain significant amounts of CO 2 , depending on its source. For Fischer-Tropsch synthesis on cobalt, CO 2 can be considered as inert diluent. However, in the specific case of a coupled Fischer-Tropsch-hydrocracking (FT-HC) process, CO 2 could interact with the catalyst in the HC step. In this experimental study, HC product distributions obtained for FT-syngas compositions with and without CO 2 and N 2 are presented. The selected feed gas compositions result from an advanced syngas production route via plasma splitting of CO 2 . Main target product was kerosene, here being defined as C 10 -C 14 . It was found that the CO 2 presence is negligible with regard to adsorption or reaction on the HC catalyst. Further insights into possible impacts of CO 2 could be obtained from the analysis of alcohols in the aqueous phase.
A dynamically operated sorption-enhanced water–gas shift reactor is modelled to leverage its performance by means of model-based process design. This reactor shall provide CO2-free synthesis gas for e-fuel production from pure CO. The nonlinear model equations describing simultaneous adsorption and reaction are solved with three numerical approaches in MATLAB: a built-in solver for partial differential equations, a semi-discretization method in combination with an ordinary differential equation solver, and an advanced graphic implementation of the latter method in Simulink. The novel implementation in Simulink offers various advantages for dynamic simulations and is expanded to a process model with six reaction chambers. The continuous conditions in the reaction chambers and the discrete states of the valves, which enable switching between reactive adsorption and regeneration, lead to a hybrid system. Controlling the discrete states in a finite-state machine in Stateflow enables automated switching between reactive adsorption and regeneration depending on predefined conditions, such as a time span or a concentration threshold in the product gas. The established chemical reactor simulation approach features unique possibilities in terms of simulation-driven development of operating procedures for intensified reactor operation. In a base case simulation, the sorbent usage for serial operation with adjusted switching times is increased by almost 15%.
This work presents the dynamic simulation of a novel sorption-enhanced water-gas shift reactor used for synthesis gas production from pure CO in an e-fuels synthesis process. Due to the intended decentralized plant installation associated with fluctuating feed, process intensification and a compact reactor system is required. An optimized operating procedure was obtained by simulation-driven process design to maximize the sorbent loading and operate the process as efficient as possible. The process simulation is based on a simplified heterogeneous packed bed reactor model. The model accounts for simultaneous water-gas shift (WGS) reaction on a Cu-based catalyst and CO2 adsorption on a K-impregnated hydrotalcite-derived mixed oxide as well as subsequent desorption. An empirical rate expression was chosen to describe the water-gas shift reaction according to experimental data at 250°C. Breakthrough experiments were performed and used to adapt kinetic adsorption (pressure: 8 bar) and desorption (pressure: 1 bar) parameters. The experimental CO2 sorption equilibrium isotherm was fitted with the Freundlich model. The reactor model was extended to a complex hybrid system scale model for the pilot plant reactor consisting of six individually accessible reaction chambers. Cyclic operation with automatized switching time adjustment was accomplished by a finite state machine. A case study exploited the benefits of a serial process configuration of reaction chambers. It could be shown that the sorbent loading can be remarkably increased through optimized operating strategies depending on the process conditions. Hence, the development of the hybrid model marks a crucial step towards the planned pilot plant operation and control.
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