CO2 removal from gas mixtures at high temperature using membrane technology : Application to Steam Methane Reforming

Details

Supervisors

De Wilde, Juray ; Luis Alconero, Patricia

Faculty

Ecole polytechnique de Louvain

Degree label

Master [120] : ingénieur civil en chimie et science des matériaux, à finalité spécialisée

Abstract

enSteam Methane Reforming (SMR) remains the primary industrial process for hydrogen production, yet it is heavily constrained by thermodynamic equilibrium limits and significant greenhouse gas emissions. This thesis investigates the intensification of the SMR process through the integration of a CO2-permselective membrane reactor, operating simultaneously as a reaction and separation unit. The research is conducted through a dual approach combining rigorous numerical optimization and step-by-step experimental material development. First, a 1D mathematical model of a dual-tube membrane reactor was developed in MATLAB. To identify the optimal operating window, a multi-objective Pareto optimization was performed using the gamultiobj genetic algorithm. The optimization targeted the maximization of both methane conversion and CO2 separation efficiency while managing thermal and mechanical energy costs. The resulting optimal "sweet spot" configuration achieved a methane conversion exceeding 94% alongside a separation efficiency of over 53%. When benchmarked against a conventional single-tube baseline model operating under identical conditions, the membrane reactor demonstrated a definitive thermodynamic superiority, proving that continuous in-situ CO2 extraction is a driver for enhanced hydrogen yield. In parallel, an iterative experimental methodology was undertaken to manufacture the physical dual-phase ceramic membrane. Manufacturing protocols were developed for pure alumina structural supports, alumina supports coated with a Samarium-Doped Ceria (SDC) active layer, and 8-YSZ membranes. The layer integrity, adherence, and microstructure were characterized through visual inspection and Scanning Electron Microscopy (SEM) analysis of resin-embedded cross-sections. Future work will focus on the continuous optimization of the casting protocols, the quantification of the membrane's gas diffusivity, the execution of extensive thermal cycling to assess its long-term thermomechanical resistance under realistic reforming conditions and scale-up of the manufacturing process and pilot plant testing.