Owing to the massive expansion and intermittent nature of renewable power, green hydrogen production, storage, and transportation technologies with improved economic returns need to be developed. Moreover, the slowness of the dehydrogenation reaction is a primary barrier to the commercialization of liquid organic hydrogen carrier (LOHC) technology. The present study focused on increasing the speed of dehydrogenation, resulting in the proposal of a triple-loop dehydrogenation system comprising reaction, heating, and chilling loops. The reactor has a rotating cage containing a packed bed of catalyst pellets, which is designed to enhance both heat and mass transfer by helping to detach precipitated hydrogen bubbles from the catalyst surface. In addition, the centrifugal force aids in isolating the gas phase from the LOHC liquid. A dehydrogenation experiment was conducted using the reaction and chilling loops, which revealed that the average hydrogen production rate during the first hour was 52.6 LPM (liter per minute) from 26.3 L of perhydro-dibenzyl-toluene with 1.5 kg of 0.5 wt% Pt/Al2O3 catalyst. This was approximately 48% more than the value predicted with the reaction kinetics measured with a small-scale plug flow dehydrogenation reactor with less than 1.0 g of 5.0 wt% Pt/Al2O3 catalyst. The concept, construction methods, and results of the preliminary gas infiltration, flow visualization, and reactor pumping experiments are also described in this paper.
Hydrogen for building fuel cells is primarily produced by natural-gas steam-reforming reactions. Pipeline-transported natural gas in Europe and North America used to contain about 1% to 5% N2, which reacts with H2 in steam-reforming reactions to form NH3. In the case of Ru, one of the catalysts used in natural-gas steam-reforming reactions, the activity of the NH3-formation reaction is higher than that of Ni and Rh catalysts. Reforming gas containing NH3 is known to poison Pt catalysts in Polymer Electrolyte Membrane Fuel Cells (PEMFCs) and also poison catalysts in preferential oxidation (PROX). In this study, Langmuir–Hinshelwood-based models of the NH3-formation reaction considering H2 and CO were proposed and compared with a simplified form of the Temkin–Pyzhev model for NH3-formation rate. The kinetic parameters of each model were optimized by performing multi-objective function optimization on the experimental results using a tube-type reactor and the numerical results of a plug-flow one-dimension simple SR (steam-reforming) reactor.