Self-diffusion of carbon dioxide in samaria/alumina aerogel catalyst using high field NMR diffusometry

Pulsed field gradient (PFG) NMR was used to investigate the self-diffusion of carbon dioxide in alumina stabilized samaria aerogel catalyst, a promising porous catalyst for gas-phase reactions featuring high porosity and high surface area. For diffusion studies, the catalyst was prepared in two sample packing types, macroscopic monoliths (i.e., macroscopic cylindrical particles) and powder beds with particle sizes around 200 μm that are considered for catalytic applications. Studies of diffusion in these samples revealed how macroscopic packing influences the catalyst transport properties. Application of a high magnetic field of 17.6 T in the reported PFG NMR studies enabled diffusion measurements for relatively low carbon dioxide densities in the catalyst samples corresponding to a gas loading pressure of around 0.1 atm. As a result, it was possible to perform diffusion measurements for a large range of carbon dioxide loading pressures between 0.1 and 10 atm. The measured carbon dioxide diffusivities in the beds of catalyst particles are interpreted in the context of a simple diffusion-mediated exchange model previously used for zeolites and other porous materials.