Partial positively charged Pt in Pt/MgAl2O4 for enhanced dehydrogenation activity.

• Pt/MgAl 2 O 4 shows robust dehydrogenation activity being twice that of Pt/CNF. • Edge Pt sites are discriminated to be the dominant active sites. • Partial positively charged Pt prevents the strong adsorption of products on catalyst. Platinum group metals hold pronounced potential for the dehydrogenation process of liquid organic hydrogen carriers (LOHCs) such as decalin, but the strong adsorption of dehydrogenation product has suppressed the moving forward of these catalysts. Herein, we described that the strong interactions between Pt and MgAl 2 O 4 trigger partial positively charged Pt, which mitigates the adsorption of naphthalene on highly active Pt sites, thus achieving an outstanding decalin dehydrogenation activity that is nearly twice that of state-of-the-art Pt/CNF catalysts. As revealed by various characterization outcomes and DFT calculations, the strong electronic interactions between Pt and spinel oxygen surface resulted in partial positively charged Pt on MgAl 2 O 4 , which inhibits the electron transfer from Pt to unsaturated carbon of naphthalene, thus weakening the bond strength between Pt and naphthalene. As a result, the combination of small-sized Pt nanoparticles and facile desorption of products endows tremendous dehydrogenation activity of Pt/MgAl 2 O 4. This study may shed new light on the rational construction of highly efficient metal catalysts for the application of LOHCs. [ABSTRACT FROM AUTHOR]