Wu Cheng-Yu, Hsiao Yueh-Chun, Chen Yi, Lin Kun-Han, Lee Tsung-Ju, Chi Chong-Chi, Lin Jui-Tai, Hsu Liang-Ching, Tsai Hsin-Jung, Gao Jia-Qi, Chang Chun-Wei, Kao I-Ting, Wu Chia-Ying, Lu Ying-Rui, Pao Chih-Wen, Hung Sung-Fu, Lu Ming-Yen, Zhou Shan, Yang Tung-Han
Department of Chemical Engineering, National Tsing Hua University, Hsinchu 30013, Taiwan.
Department of Applied Chemistry, National Yang Ming Chiao Tung University, Hsinchu 30010, Taiwan.
Sci Adv. 2024 Jul 26;10(30):eadl3693. doi: 10.1126/sciadv.adl3693.
We report a catalyst family of high-entropy alloy (HEA) atomic layers having three elements from iron-group metals (IGMs) and two elements from platinum-group metals (PGMs). Ten distinct quinary compositions of IGM-PGM-HEA with precisely controlled square atomic arrangements are used to explore their impact on hydrogen evolution reaction (HER) and hydrogen oxidation reaction (HOR). The PtRuFeCoNi atomic layers perform enhanced catalytic activity and durability toward HER and HOR when benchmarked against the other IGM-PGM-HEA and commercial Pt/C catalysts. Operando synchrotron x-ray absorption spectroscopy and density functional theory simulations confirm the cocktail effect arising from the multielement composition. This effect optimizes hydrogen-adsorption free energy and contributes to the remarkable catalytic activity observed in PtRuFeCoNi. In situ electron microscopy captures the phase transformation of metastable PtRuFeCoNi during the annealing process. They transform from random atomic mixing (25°C), to ordered L1 (300°C) and L1 (400°C) intermetallic, and finally phase-separated states (500°C).
我们报道了一种高熵合金（HEA）原子层催化剂家族，其包含三种铁族金属（IGM）元素和两种铂族金属（PGM）元素。十种具有精确控制的方形原子排列的不同五元IGM-PGM-HEA组成被用于探究它们对析氢反应（HER）和氢氧化反应（HOR）的影响。与其他IGM-PGM-HEA和商业Pt/C催化剂相比，PtRuFeCoNi原子层对HER和HOR表现出增强的催化活性和耐久性。原位同步加速器X射线吸收光谱和密度泛函理论模拟证实了多元素组成产生的协同效应。这种效应优化了氢吸附自由能，并促成了在PtRuFeCoNi中观察到的显著催化活性。原位电子显微镜捕捉到了亚稳PtRuFeCoNi在退火过程中的相变。它们从随机原子混合（25°C）转变为有序的L1（300°C）和L1（400°C）金属间化合物，最终转变为相分离状态（500°C）。
