School of Textile Science and Engineering, Xi'an Polytechnic University, Xi'an 710048, Shaanxi, China.
Key Laboratory of Functional Textile Material and Product, Ministry of Education, Xi'an Polytechnic University, Xi'an 710048, China.
ACS Appl Mater Interfaces. 2023 Jan 25;15(3):3934-3940. doi: 10.1021/acsami.2c17883. Epub 2023 Jan 12.
Rational design and controllable synthesis of catalysts with unique structure and composition are effective ways to promote electrocatalytic ethanol oxidation, thus contributing the direct ethanol fuel cells to gain ground. Herein, 2.5 nm-thin PtIrCu ternary alloy ultrathin nanowires (UNWs) with high-density planar defects are synthesized via oriented attachment with the assistance of H. By adjusting the contents of Ir and Cu atoms, we find that the structure of the products changed from nanowires (NWs) to nanoparticles with the increase of Ir content. Density functional theory calculations show that when Cu atoms are replaced by Ir atoms, the vacancy formation energy of Pt atoms is increased, making the Pt atoms difficult to be activated by H, which is not conducive to the formation of a one-dimensional structure. The optimal PtIrCu UNWs achieve excellent ethanol electrooxidation reaction activity (1.05 A·mg and 1.67 mA·cm), for it can significantly reduce the onset potential and improve the ability of CO anti-poisoning. The significant improvement in catalytic performance is attributed to the synergistic effect of the alloy and the NW structure with high-density planar defects.
通过取向附生在 H 的辅助下合成了具有高密度平面缺陷的 2.5nm 厚的 PtIrCu 三元合金超薄纳米线(UNWs)。通过调整 Ir 和 Cu 原子的含量,我们发现随着 Ir 含量的增加,产物的结构从纳米线(NWs)转变为纳米颗粒。密度泛函理论计算表明,当 Cu 原子被 Ir 原子取代时,Pt 原子的空位形成能增加,使得 Pt 原子难以被 H 激活,这不利于一维结构的形成。最佳的 PtIrCu UNWs 表现出优异的乙醇电氧化反应活性(1.05A·mg 和 1.67mA·cm),因为它可以显著降低起始电位并提高 CO 抗中毒能力。催化性能的显著提高归因于合金和具有高密度平面缺陷的 NW 结构的协同效应。