Nitrogen-Doped Graphene Monolith Catalysts for Oxidative Dehydrogenation of Propane

It’s of paramount importance to develop renewable nanocarbon materials to replace conventional precious metal catalysts in alkane dehydrogenation reactions. Graphene-based materials with high surface area have great potential for light alkane dehydrogenation. However, the powder-like state of the graphene-based materials seriously limits their potential industrial applications. In the present work, a new synthetic route is designed to fabricate nitrogen-doped graphene-based monolith catalysts for oxidative dehydrogenation of propane. The synthetic strategy combines the hydrothermal-aerogel and the post thermo-treatment procedures with urea and graphene as precursors. The structural characterization and kinetic analysis show that the monolithic catalyst well maintains the structural advantages of graphene with relatively high surface area and excellent thermal stability. The homogeneous distributed nitrogen species can effectively improve the yield of propylene (5.3% vs. 1.9%) and lower the activation energy (62.6 kJ mol−1 vs. 80.1 kJ mol−1) in oxidative dehydrogenation of propane reaction comparing with un-doped graphene monolith. An optimized doping amount at 1:1 weight content of the graphene to urea precursors could exhibit the best catalytic performance. The present work paves the way for developing novel and efficient nitrogen-doped graphene monolithic catalysts for oxidative dehydrogenation reactions of propane.

Upgrading of Bio-Syngas via Steam-CO2 Reforming Using Rh/Alumina Monolith Catalysts

Steam-CO2 reforming of biomass derived synthesis gas (bio-syngas) was investigated with regard to the steam concentration in the feed using Rh-loaded alumina foam monolith catalysts, which was also accompanied by thermodynamic equilibrium calculation. With 40 vol % steam addition, steam methane reforming and water gas shift reaction were prevailed at the temperature below 640 °C, above which methane dry reforming and reverse-water gas shift reaction were intensified. Substantial change of activation energy based on the methane conversion was observed at 640 °C, where the reaction seemed to be shifted from the kinetic controlled region to the mass transfer controlled region. At the reduced steam of 20 vol %, the increase in the gas velocity led to the increase in the contribution of steam reforming. Comparing to the absence of steam, the addition of steam (40 vol %) resulted in the increase in the production of H2 and CO2, which in turn increased the H2/CO ratio by 95% and decreased the CO/CO2 ratio by 60%. Rh-loaded alumina monolith was revealed to have a good stability in upgrading of the raw bio-syngas.