Zhang Nannan, Zhang Kewang, Li Jie, Ye Changqing, Du Yukou
College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123, China.
Jiangsu Key Laboratory for Environment Functional Materials, School of Materials Science and Engineering, Suzhou University of Science and Technology, Suzhou 215009, China.
J Colloid Interface Sci. 2023 Nov 15;650(Pt B):1509-1517. doi: 10.1016/j.jcis.2023.07.121. Epub 2023 Jul 20.
Three dimensional (3D) noble-metal nanomaterials with special surface structures have been regarded as high-performance catalysts for alcohol oxidation on account of their superior thermal stability, electrical conductivity and large specific surface area. Although extensive efforts have been devoted to the preparation of 3D Pd-based catalysts with superior activity and stability, designing a simple, effective and eco-friendly method remains a challenge. Herein, we developed a facile one-step coreduction strategy to synthesize a series of 3D surface-wrinkled PdAu nanospheres (NSs) with tunable Pd/Au atomic ratios and found a universal method to prepare surface-wrinkled PdM (M = Au, Pt, Cu and Pb) NSs. Benefiting from the function of the surfactant cetyltrimethylammonium chloride (CTAC), the synthesized PdAu NSs with different composition possess abundant surface wrinkles, which is beneficial for exposing more electroactive centers. Attributed to the unique geometric morphology and optimized atomic ratio, the PdAu-2 NSs exhibited an optimal mass activity (MA) of 8103 mA mg and 5113 mA mg for the ethylene glycol oxidation reaction (EGOR) and ethanol oxidation reaction (EOR), which was 6.1 and 4.1 times that of commercial Pd/C, respectively. Moreover, the PdAu-2 NSs exhibited superb stability after long-term current-time (i-t) and cyclic voltammetry (CV) tests of the EGOR and EOR. This work not only provides new avenues to engineer PdAu NSs with enhanced electrocatalytic performance but also offers guidance for extending to more 3D PdM (M = other metals) NSs with novel morphology applied to fuel cell fields.
具有特殊表面结构的三维（3D）贵金属纳米材料因其优异的热稳定性、导电性和大比表面积，被视为醇类氧化的高性能催化剂。尽管人们为制备具有优异活性和稳定性的3D钯基催化剂付出了巨大努力，但设计一种简单、有效且环保的方法仍然是一个挑战。在此，我们开发了一种简便的一步共还原策略，以合成一系列具有可调Pd/Au原子比的3D表面褶皱钯金纳米球（NSs），并找到了一种制备表面褶皱PdM（M = Au、Pt、Cu和Pb）NSs的通用方法。受益于表面活性剂十六烷基三甲基氯化铵（CTAC）的作用，合成的不同组成的钯金NSs具有丰富的表面褶皱，这有利于暴露更多的电活性中心。由于独特的几何形态和优化的原子比，钯金-2 NSs在乙二醇氧化反应（EGOR）和乙醇氧化反应（EOR）中分别表现出8103 mA mg和5113 mA mg的最佳质量活性（MA），分别是商业Pd/C的6.1倍和4.1倍。此外，在EGOR和EOR的长期电流-时间（i-t）和循环伏安法（CV）测试后，钯金-2 NSs表现出优异的稳定性。这项工作不仅为设计具有增强电催化性能的钯金NSs提供了新途径，也为扩展到更多具有新颖形态的3D PdM（M = 其他金属）NSs应用于燃料电池领域提供了指导。
