Journal of Colloid and Interface Science ( IF 9.4 ) Pub Date : 2023-07-20 , DOI: 10.1016/j.jcis.2023.07.121
Nannan Zhang 1 , Kewang Zhang 1 , Jie Li 1 , Changqing Ye 2 , Yukou Du 3
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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−1 and 5113 mA mg−1 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.
中文翻译:

一锅合成 3D 表面皱纹 PdAu 纳米球,用于稳健的醇电催化
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、导电性和大的比表面积而被认为是高性能的醇氧化催化剂。尽管人们在制备具有优异活性和稳定性的3D Pd基催化剂方面付出了广泛的努力,但设计一种简单、有效和环境友好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来合成一系列具有可调Pd/Au原子比的3D表面皱纹PdAu纳米球(NSs),并找到了一种制备表面皱纹PdM(M = Au,Pt, Cu 和 Pb) NS。受益于表面活性剂十六烷基三甲基氯化铵(CTAC)的作用,合成的不同成分的PdAu NSs具有丰富的表面皱纹,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,PdAu-2 NSs在乙二醇氧化反应(EGOR)和乙醇氧化反应中表现出8103 mA mg -1和5113 mA mg -1的最佳质量活度(MA)。 EOR),分别是商业 Pd/C 的 6.1 和 4.1 倍。此外,PdAu-2 NSs 在 EGOR 和 EOR 的长期电流-时间 (it) 和循环伏安 (CV) 测试后表现出极好的稳定性。这项工作不仅为设计具有增强电催化性能的 PdAu NS 提供了新途径,而且还为将具有新颖形态的更多 3D PdM(M = 其他金属)NS 应用于燃料电池领域提供了指导。