Zeng Qing, Ma Mengyuan, Liu Hui, Xu Lin, Tian Shaonan, Chen Dong, Wang Jing, Yang Jun
State Key Laboratory of Mesoscience and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China; Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China.
State Key Laboratory of Mesoscience and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China.
Sci Bull (Beijing). 2025 Aug 30;70(16):2604-2615. doi: 10.1016/j.scib.2025.04.051. Epub 2025 Apr 29.
Atomic surface engineering for nanostructures significantly contributes to the enhancement of electrocatalysis for a given chemical reaction. However, exploring a facile method to elaborately regulate surfaces at atomic scale remains a grand challenge. Herein, we report the construction of atomically rough surfaces (ARSs) on Au-based binary alloys through a novel and controllable gold (Au)-catalyzed strategy, which involves the first synthesis of Au-based bimetallic nanoalloys, i.e., AuPd and AuAg, and subsequent reduction of another metal ions (Pt, Pd, or Ag) initiated by Au sites on the alloy particle surfaces. By combining ARSs with low-coordinated atoms with ligand effect induced by vicinal Au atoms, the as-prepared ARSs exhibit good activity and durability toward ethanol oxidation reaction (EOR) in an alkaline medium. In particular, the Pd-Pt ARSs on the AuPd alloy particle surface (denoted as AuPd-Pt) exhibit the highest electrocatalytic EOR performance in terms of both specific activity (14.9 mA cm) and mass activity (28.5 A mg), surpassing those of their AuPd alloy counterparts, commercial Pd/C catalyst, and most Pd-based electrocatalysts reported recently. In situ Fourier transform infrared (FTIR) spectroscopy reveals that the EOR process on the Pd-Pt ARSs strongly prefers incomplete oxidation, which is further authenticated by the density functional theory (DFT) calculations.
用于纳米结构的原子表面工程对增强特定化学反应的电催化作用有显著贡献。然而，探索一种在原子尺度上精细调控表面的简便方法仍然是一个巨大的挑战。在此，我们报告了通过一种新颖且可控的金（Au）催化策略在金基二元合金上构建原子粗糙表面（ARSs），该策略包括首先合成金基双金属纳米合金，即AuPd和AuAg，以及随后由合金颗粒表面的Au位点引发另一种金属离子（Pt、Pd或Ag）的还原。通过将ARSs与由相邻Au原子诱导的配体效应的低配位原子相结合，所制备的ARSs在碱性介质中对乙醇氧化反应（EOR）表现出良好的活性和耐久性。特别是，AuPd合金颗粒表面的Pd-Pt ARSs（表示为AuPd-Pt）在比活性（14.9 mA cm）和质量活性（28.5 A mg）方面均表现出最高的电催化EOR性能，超过了其AuPd合金对应物、商业Pd/C催化剂以及最近报道的大多数钯基电催化剂。原位傅里叶变换红外（FTIR）光谱表明，Pd-Pt ARSs上的EOR过程强烈倾向于不完全氧化，这通过密度泛函理论（DFT）计算得到进一步证实。
