How to Boost the Activity of the Monolayer Pt Supported on TiC Catalysts for Oxygen Reduction Reaction: A Density Functional Theory Study.

Developing the optimized electrocatalysts with high Pt utilization as well as the outstanding performance for the oxygen reduction reaction (ORR) has raised great attention. Herein, the effects of the interlayer ZrC, HfC, or TiN and the multilayer Pt shell on the adsorption ability and the catalytic activity of the TiC@Pt core-shell structures are systemically investigated by density functional theory (DFT) calculations. For the sandwich structures, the presence of TiN significantly enhances the adsorption ability of the Pt shell, leading to the deterioration of the activity whilst the negligible influence of the ZrC and HfC insertion results the comparable performance with respect to TiC@Pt_1ML. In addition, increasing the thickness of the Pt shell reduces the oxyphilic capacity and then mitigates the OH poisoning. From the free energy plots, the superior activity of TiC@Pt_2ML is identified in comparison with 1ML and 3ML Pt shell. Herein, the improved activity with its high Pt atomic utilization makes the potential TiC@Pt_2ML electrocatalyst for the future fuel cells.