Zhu Hui, Liu Houyi, Yang Lei, Xiao Beibei
School of Energy and Power Engineering, Jiangsu University of Science and Technology, Zhenjiang 212003, China.
Materials (Basel). 2019 May 13;12(9):1560. doi: 10.3390/ma12091560.
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. 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 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 electrocatalyst for the future fuel cells.
开发具有高铂利用率以及出色氧还原反应（ORR）性能的优化电催化剂引起了广泛关注。在此，通过密度泛函理论（DFT）计算系统研究了夹层ZrC、HfC或TiN以及多层铂壳对TiC@Pt核壳结构吸附能力和催化活性的影响。对于三明治结构，TiN的存在显著增强了铂壳的吸附能力，导致活性下降，而插入ZrC和HfC的影响可忽略不计，其性能与TiC@Pt相当。此外，增加铂壳的厚度会降低亲氧能力，进而减轻OH中毒。从自由能图可以看出，与1ML和3ML铂壳相比，TiC@Pt具有更高的活性。在此，其具有高铂原子利用率的改进活性使其成为未来燃料电池潜在的电催化剂。
