Strong metal-support interactions of TiO interface-loaded Pt constructed under different atmospheres for adjusting the hydrogen storage reaction performance of -ethylcarbazole.

In this study, two series of samples (r-Pt/TiO prepared with a hydrogen pretreatment and r-Pt/TiO prepared with an oxygen pretreatment) were prepared by treating commercial TiO supports in different atmospheres to establish different TiO interfacial structures, followed by the addition of platinum nanoparticles (NPs) for the catalyzed hydrogenation/dehydrogenation cycle of -ethylcarbazole (NEC). The kinetic analysis and reaction mechanism were investigated by combining XRD, Raman, CO-DRIFT, HRTEM, XPS, H-TPD and DFT calculations. It was found that the performance of the samples for the NEC system's cyclic hydrogen storage could be modulated by treating the TiO interfacial structure with different atmospheres varying the extent of strong metal-support interaction (SMSI). In addition, a turnover frequency (TOF) of 191.52 min for dehydrogenation was achieved at 170 °C, which is better than the previously reported catalysts. Experimental studies (characterization and kinetic studies) and DFT calculations confirmed that the SMSI of the r-Pt/TiO series samples promoted the escape of H and enhanced the catalytic activity for 4H-NEC in the 12H-NEC dehydrogenation reaction. In the NEC hydrogenation reaction, the r-Pt/TiO series samples were pretreated with H before loading platinum metal, which led to the early activation of Ti in their carriers, and thus suppressed the SMSI effect of the reduction process after loading platinum. This process caused the interface formed by r-Pt/TiO to have a higher energy barrier to 6H-NEC, which is an intermediate product of the NEC hydrogenation process, and this interrupted the hydrogenation process of 6H-NEC.