Luo Xianyou, Yuan Ping, Xiao Haoming, Li Shengwei, Luo Junhui, Li Junyi, Lai Wende, Chen Yong, Li De
Guangdong Key Laboratory for Hydrogen Energy Technologies, School of Materials Science and Hydrogen Energy, Foshan University, Foshan 528000, China.
State Key Laboratory of Marine Resource Utilization in South China Sea, Hainan Provincial Key Laboratory of Research on Utilization of Si-Zr-Ti Resources, School of Materials Science and Engineering, Hainan University, Haikou 570228, China.
ACS Appl Mater Interfaces. 2024 May 22;16(20):26044-26056. doi: 10.1021/acsami.4c00690. Epub 2024 May 8.
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. 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.
碳材料已广泛应用于高效碳载铂（Pt/C）催化剂的合成中，其中结构性质对Pt/C催化剂的电催化性能有很大影响。然而，碳载体中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，通过一种简单的模板辅助策略制备了具有不同程度固有缺陷的多孔碳载体，并采用各种分析方法对所得样品进行了系统研究。结果表明，碳载体中存在大量固有缺陷（空位和拓扑缺陷）有利于Pt物种的分散和锚定，促进Pt原子与碳载体之间的电子转移，并调节Pt物种的电子态。这些特性提高了Pt/C催化剂的HER性能。与过电位为178 mV的非模板辅助碳载铂催化剂（Pt/NTC）相比，优化后的模板辅助碳载铂催化剂（Pt/TC）在10 mA cm时表现出58 mV的较低过电位。此外，由于其强的金属-载体相互作用，Pt/TC催化剂比Pt/NTC催化剂表现出更好的HER耐久性。DFT计算证实了固有缺陷（空位和拓扑缺陷）在稳定Pt原子方面所起的重要作用，其中Pt-C3配位被确定为改善Pt的HER性能的最有利结构。总体而言，本研究提供了关于多孔碳载体中固有缺陷对Pt/C催化剂HER性能的重大贡献的新见解，有助于未来先进碳载催化剂或其他碳基电极材料的设计和制备。
