Zhan Changhong, Xu Yong, Bu Lingzheng, Zhu Huaze, Feng Yonggang, Yang Tang, Zhang Ying, Yang Zhiqing, Huang Bolong, Shao Qi, Huang Xiaoqing
State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, 361005, Xiamen, China.
Guangzhou Key Laboratory of Low-Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy, Guangdong University of Technology, 510006, Guangzhou, China.
Nat Commun. 2021 Oct 29;12(1):6261. doi: 10.1038/s41467-021-26425-2.
High-entropy alloys (HEAs) with unique physicochemical properties have attracted tremendous attention in many fields, yet the precise control on dimension and morphology at atomic level remains formidable challenges. Herein, we synthesize unique PtRuNiCoFeMo HEA subnanometer nanowires (SNWs) for alkaline hydrogen oxidation reaction (HOR). The mass and specific activities of HEA SNWs/C reach 6.75 A mg and 8.96 mA cm, respectively, which are 2.8/2.6, 4.1/2.4, and 19.8/18.7 times higher than those of HEA NPs/C, commercial PtRu/C and Pt/C, respectively. It can even display enhanced resistance to CO poisoning during HOR in the presence of 1000 ppm CO. Density functional theory calculations reveal that the strong interactions between different metal sites in HEA SNWs can greatly regulate the binding strength of proton and hydroxyl, and therefore enhances the HOR activity. This work not only provides a viable synthetic route for the fabrication of Pt-based HEA subnano/nano materials, but also promotes the fundamental researches on catalysis and beyond.
具有独特物理化学性质的高熵合金（HEAs）在许多领域引起了极大关注，然而在原子水平上精确控制尺寸和形态仍然是巨大挑战。在此，我们合成了用于碱性氢氧化反应（HOR）的独特的PtRuNiCoFeMo高熵合金亚纳米纳米线（SNWs）。高熵合金亚纳米线/碳（HEA SNWs/C）的质量活性和比活性分别达到6.75 A mg和8.96 mA cm，分别比高熵合金纳米颗粒/碳（HEA NPs/C）、商业PtRu/C和Pt/C高2.8/2.6、4.1/2.4和19.8/18.7倍。在存在1000 ppm CO的情况下，它在氢氧化反应期间甚至能表现出增强的抗CO中毒能力。密度泛函理论计算表明，高熵合金亚纳米线中不同金属位点之间的强相互作用可以极大地调节质子和羟基的结合强度，从而提高氢氧化反应活性。这项工作不仅为制备基于Pt的高熵合金亚纳米/纳米材料提供了一条可行的合成路线，而且推动了催化及其他领域的基础研究。
