Development of reaction-diffusion DFT and its application to catalytic oxidation of NO in porous materials

The reaction-diffusion (RD) process is an important and complex subject that involves nonequilibrium modeling and multiscale calculations and may be applied to multiple fields. State-of-art theories are computationally too expensive for real-world applications. We propose a novel classical density functional theory (CDFT) for RD modeling by combining ordinary time-dependent density functional theory (TDDFT) and reaction kinetic models to examine the multiscale RD process. The theory is applied to NO oxidation in porous materials. The uptake, flux, and density profiles are examined, to reveal that the shape of the pore could influence the selectivity of adsorption between the reactant and product, which further leads to variations in the catalytic efficiency. It is noted that open pores are more favorable for catalytic reactions. The importance of adsorption is examined in the presence as well as the absence of pore-gas attraction. Without attraction, the catalytic efficiency is decreased by three orders of magnitude.