One-Pot Synthesis of Au/Pd Core/Shell Nanoparticles Supported on Reduced Graphene Oxide with Enhanced Dehydrogenation Performance for Dodecahydro-N-ethylcarbazole

The unsatisfactory performance of dehydrogenation catalysts has been the bottleneck for liquid organic hydrogen carrier (LOHC) development. After systematic experiments, the Au/Pd core/shell catalysts were screened from a series of Pd–M (M = Au, Ag, Ru, Rh) combinations for dehydrogenation of dodecahydro-N-ethylcarbazole (12H-NEC) through a one-pot wet chemical synthesis. The ratio of Pd to Au is also within the scope of the experiment, and it was found that the catalytic activity was following the order of Au1Pd1.3 > Au1Pd2 > Au1Pd1 > Ru1Pd1.3 > Au1Pd0.7 > Rh1Pd1.3 > Ag1Pd1.3 supported on rGO for the dehydrogenation process. Au1Pd1.3/rGO greatly improves the efficiency of the dehydrogenation reaction, specifically; while maintaining selectivity and conversion rate of 100%, the reaction time was shortened by 43% compared to the monometallic Pd/rGO catalyst with the highest activity we prepared before, and compared to the best performing bimetallic catalyst in the literature, the optimal reaction time in this work was reduced by 71% when the hydrogen storage requirements of the US DOE (Department of Energy) are met. A cycle performance experiment was performed to verify its excellent catalytic stability. Further catalyst characterization also proves that it has good morphology and stability. A kinetics calculation was carried out to obtain fundamental reaction parameters.