Huanhao Chen, Mork Family Department of Chemical Engineering and Materials Science Viterbi School of Engineering, University of Southern California, Los Angeles, CA, Mingyuan Cao, Mork Family Department of Chemical Engineering and Materials Science Viterbi School of Engineering, University of Southern California, Los Angeles, Secgin Karagoz, Chemical & Biomolecular Engineering, UCLA, Los Angeles, CA, Vasilios Manousiouthakis, Chemical & Biomolecular Engineering Department,, University of California Los Angeles, Los Angeles, Los Angeles, CA and Theodore Tsotsis, Mork Family Department of Chemical Engineering, University of Southern California, Los Angeles, CA
Reactive separation processes, such as membrane reactors (MRs) and adsorptive reactors (ARs), have been attracting increased interest for industrial applications. Such a hybrid system combining a membrane reactor (MR) and an adsorptive reactor (AR) in tandem (with the AR following the MR, and the MR’s reject stream serving as the AR’s feed) can produce an ultra-pure H
2 product (without the need for using a post-processing step), and can deliver WGS reaction conversion exceeding equlibrium. The proposal configuration (AR following MR) provides significant flexibility in addition to high-purity hydrogen and carbon dioxide production.
The primary objective of this work is to first develop and simulate an advanced, and detailed mathematical model for the MR/AR sequence and then validate this model using experimental data obtained at the bench-scale. The MR system is composed of a reaction zone packed with catalyst and quartz pellets, and a water/hydrogen permeation zone. In the AR, both catalyst and adsorbent materials are used for simultaneous reaction and separation. The AR is a dynamically operated process. Both steady-state and dynamic experiment are carried out in a laboratory setting to capture the individual MR/AR performances. Experiments are carried out for a broad range of temperatures (up to 300 oC) pressures (up to 25 bar) relevant to realistic application conditions. The velocity, temperature and species concentration profiles in the MR reaction and permeation zones are captured by momentum/species transport models accounting for convection/reaction /diffusion/conduction mechanisms. The rigorous Maxwell-Stefan and dusty gas models are applied to describe mass diffusion fluxes. Finally, the performances of the combined system (the membrane reactor (MR) followed by an adsorptive reactor (AR) is simulated for a broad range of the operating conditions and design parameters. The simulation results are compared with the experimental findings.
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