(426g) Investigation of Thermodynamics and Kinetics of Glycerol Aqueous Phase Reforming Via Multi-Scale Simulations

Aqueous phase reforming (APR) is a rising method to convert glycerol, which is abundant in biomass waste streams, to H₂, which is essential to a successful biorefinery. One of the major obstacles is the low H₂ yields. Improving H₂ yields requires a better understanding of the reaction mechanism, which will enable tuning of the catalyst and operating conditions to optimize activity and selectivity to H₂. This knowledge gap is caused by the large reaction network and the aqueous-phase reaction environment. In this work, we use a multil-scale simulation technique employing a combination of classical molecular dynamics and density functional theory to assess the thermodynamic, kinetic, and mechanistic influences of the liquid environment on the surface chemistry for catalytic glycerol reforming. We derive scaling relations to reduce the computational effort and additionally show how the liquid environment influences correlations between surface energetics. We input calculated energetics to a microkinetic model, which we use to compare with experimental results from the literature. Our simulated product distributions are in excellent agreement with these experimental results.