吉林大学张伟团队报道了碱性析氢反应中Fe-Pt金属间化合物催化剂表面末端的逐原子优化。相关研究成果于2024年2月7日发表在《科学通报》。

控制金属间催化剂中元素原子的原子排列以控制其表面和亚表面性质，是电催化反应中一项关键但具有挑战性的工作。在析氢反应（HER）中，通过引入Fe来调节传统贵金属Pt的d带中心，可以优化催化性能。然而，在碱性HER中，从无序的Fe/Pt合金到高度有序的金属间化合物（IMCs）（如FePt₃）的有效转变研究存在显著差距，阻碍了其更广泛的应用。

在该研究中，通过简单的浸渍方法以及一系列热处理过程，包括在还原气氛中退火，以调节FePt₃催化剂中Fe/Pt原子的排列顺序，合成了一系列负载在碳纳米管（CNTs）上的催化剂FePt₃-xH（x=5、6、7、8和9）。利用先进的显微镜和光谱技术，研究人员系统地探索了FePt₃在HER中的有序度的影响。

所制备的FePt₃-8H在j=10 mA cm^-2时表现出显著的HER催化活性，具有低过电位（在1.0 mol L^-1 KOH中η=37 mV）。L₁₂-FePt₃-8H催化剂的表面被证明是富Pt的。由于独特的Fe/Pt配位，表面的Pt不易被氧化，从而显著提高了HER的性能。

附：英文原文

Title: Atom-by-atom optimizing the surface termination of Fe-Pt intermetallic catalysts for alkaline hydrogen evolution reaction

Author: Qing Liang a, Fanling Meng a, Wenwen Li a, Xu Zou a, Kexin Song a, Xin Ge a, Zhou Jiang a, Yuhua Liu a, Meiqi Liu a, Zhenyu Li, Taowen Dong, Zhongjun Chen, Wei Zhang, Weitao Zheng

Issue&Volume: 2024/02/07

Abstract: Controlling the atomic arrangement of elemental atoms in intermetallic catalysts to govern their surface and subsurface properties is a crucial but challenging endeavor in electrocatalytic reactions. In hydrogen evolution reaction (HER), adjusting the d-band center of the conventional noble-metallic Pt by introducing Fe enables the optimization of catalytic performance. However, a notable gap exists in research on the effective transition from disordered Fe/Pt alloys to highly ordered intermetallic compounds (IMCs) such as FePt3 in the alkaline HER, hampering their broader application. In this study, a series of catalysts FePt3-xH (x = 5, 6, 7, 8 and 9) supported on carbon nanotubes (CNTs) were synthesized via a simple impregnation method, along with a range of heat treatment processes, including annealing in a reductive atmosphere, to regulate the order degree of the arrangement of Fe/Pt atoms within the FePt3 catalyst. By using advanced microscopy and spectroscopy techniques, we systematically explored the impact of the order degree of FePt3 in the HER. The as-prepared FePt3-8H exhibited notable HER catalytic activity with low overpotentials (η = 37 mV in 1.0 mol L1 KOH) at j = 10 mA cm2. The surface of the L12 FePt3-8H catalyst was demonstrated to be Pt-rich. The Pt on the surface was not easily oxidized due to the unique Fe/Pt coordination, resulting in significant enhancement of HER performance.

DOI: 10.1016/j.scib.2024.02.004

Source: https://www.sciencedirect.com/science/article/abs/pii/S2095927324000732