Strong metal-support interactions of TiO 2 interface-loaded Pt constructed under different atmospheres for adjusting the hydrogen storage reaction performance of N -ethylcarbazole.

In this study, two series of samples (r T -Pt/TiO 2 prepared with a hydrogen pretreatment and T r-Pt/TiO 2 prepared with an oxygen pretreatment) were prepared by treating commercial TiO 2 supports in different atmospheres to establish different TiO 2 interfacial structures, followed by the addition of platinum nanoparticles (NPs) for the catalyzed hydrogenation/dehydrogenation cycle of N -ethylcarbazole (NEC). The kinetic analysis and reaction mechanism were investigated by combining XRD, Raman, CO-DRIFT, HRTEM, XPS, H 2 -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 2 interfacial structure with different atmospheres varying the extent of strong metal-support interaction (SMSI). In addition, a turnover frequency (TOF) of 191.52 min -1 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 T r-Pt/TiO 2 series samples promoted the escape of H 2 and enhanced the catalytic activity for 4H-NEC in the 12H-NEC dehydrogenation reaction. In the NEC hydrogenation reaction, the r T -Pt/TiO 2 series samples were pretreated with H 2 before loading platinum metal, which led to the early activation of Ti 4+ in their carriers, and thus suppressed the SMSI effect of the reduction process after loading platinum. This process caused the interface formed by r T -Pt/TiO 2 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.