Carbon material has widely been utilized in the synthesis of efficient carbon-supported Pt (Pt/C) catalysts, in which the structural properties greatly influence the electrocatalytic performances of Pt/C catalysts. However, the effects of intrinsic defects in carbon supports on the performance of the alkaline hydrogen evolution reaction (HER) have not been systematically investigated. Herein, porous carbon supports with different degrees of intrinsic defects were prepared by a simple template-assisted strategy, and the resulting samples were systematically studied by various analytical methods. The results suggested that the presence of abundant intrinsic defects (vacancy and topological defects) in the carbon support was advantageous in terms of favoring the dispersion and anchoring of Pt species, promoting electron transfer between Pt atoms and the carbon support, and tuning the electronic states of Pt species. These features improved the HER performance of Pt/C catalysts. Compared to the nontemplate-assisted carbon-supported Pt catalyst (Pt/NTC) with an overpotential of 178 mV, the optimized template-assisted carbon-supported Pt catalyst (Pt/TC) exhibited a lower overpotential of 58 mV at 10 mA cm^–2. Besides, the Pt/TC catalyst displayed better HER durability than the Pt/NTC catalyst owing to its strong metal–support interaction. The DFT calculations confirmed the important role played by intrinsic defects (vacancy and topological defects) in stabilizing Pt atoms, with Pt–C3 coordination identified as the most favorable structure for improving the HER performance of Pt. Overall, novel insights on the significant contribution of intrinsic defects in porous carbon supports on the HER performances of Pt/C catalysts were provided, useful for future design and fabrication of advanced carbon-supported catalysts or other carbon-based electrode materials.

中文翻译：

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Pt基碳载体的固有缺陷对碱性析氢反应的影响


碳材料已广泛用于合成高效碳载Pt（Pt/C）催化剂，其中结构性能极大地影响Pt/C催化剂的电催化性能。然而，碳载体固有缺陷对碱性析氢反应（HER）性能的影响尚未得到系统研究。在此，通过简单的模板辅助策略制备了具有不同程度内在缺陷的多孔碳载体，并通过各种分析方法对所得样品进行了系统研究。结果表明，碳载体中存在丰富的本征缺陷（空位和拓扑缺陷）有利于 Pt 物质的分散和锚定，促进 Pt 原子与碳载体之间的电子转移以及调节电子态。 Pt 物种。这些特性提高了 Pt/C 催化剂的 HER 性能。与过电势为 178 mV 的非模板辅助碳载 Pt 催化剂 (Pt/NTC) 相比，优化的模板辅助碳载 Pt 催化剂 (Pt/TC) 在 10 mA cm 下表现出较低的过电势 58 mV < b0> 。此外，由于其较强的金属-载体相互作用，Pt/TC 催化剂表现出比 Pt/NTC 催化剂更好的 HER 耐久性。 DFT 计算证实了本征缺陷（空位和拓扑缺陷）在稳定 Pt 原子方面发挥的重要作用，其中 Pt-C3 配位被认为是提高 Pt HER 性能的最有利结构。 总的来说，关于多孔碳载体的固有缺陷对 Pt/C 催化剂的 HER 性能的显着贡献提供了新颖的见解，对于先进碳负载催化剂或其他碳基电极材料的未来设计和制造很有用。