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首页> 外文期刊>Catalysis science & technology >A facile and surfactant-free route for nanomanufacturing of tailored ternary nanoalloys as superior oxygen reduction reaction electrocatalysts
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A facile and surfactant-free route for nanomanufacturing of tailored ternary nanoalloys as superior oxygen reduction reaction electrocatalysts

机译：一个简单和surfactant-free路线定制三元nanoalloys nanomanufacturing优越的氧还原反应electrocatalysts

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摘要

We have synthesized ternary nanoalloys (NAs) of Pt with transition metals (Co, Cu, Ni, Ti, Ru, Mn) as oxygen reduction reaction (ORR) electrocatalysts using our recently developed laser ablation synthesis in solution-galvanic replacement reaction (LASiS-GRR) technique as a facile and surfactant-free nanomanufacturing route. The specific choice of the elemental compositions is driven by the respective target metal/metal salt redox potential gaps as well as the target metal and/or metal oxide solubility in desired acids. The high-energy thermodynamics of the LASiS-GRR process enables control of the sizes, elemental compositions and distributions of the ternary NAs through systematic tuning of the initial metal salt concentration, pH, laser fluence and ablation time. Specifically, the PtCuCo NAs synthesized with an elemental composition of 72 : 12 : 16 (Pt : Co : Cu) exhibit the best ORR catalytic activity. The NAs largely possess a shell-core structure with the shell composed mostly of Pt and a minor amount of Cu, along with a uniformly alloyed PtCuCo core. Mass and specific activities for ORR performance of the NAs indicate a 4-and 6.5-fold improvement, respectively, over the corresponding activities of commercial Pt/C. We attribute the enhanced activity to 1) our surfactant/ligand-free synthesis technique that prevents catalytic site degradation and 2) minor alloying of the second transition metal Cu that shifts back the Pt d-band center to an optimal position between those of Pt and the PtCo binary NAs, thereby tuning their binding affinities for both oxygen and oxygenated species. Finally, this work establishes the versatility of the LASiS-GRR technique through the synthesis of other ternary NAs (PtRuNi, PtCoMn, PtNiTi) that also exhibit reasonably good ORR activities.
机译：我们已经合成了三元nanoalloys (NAs)的Pt与转变metals (Co、Cu、Ni, Ti . Ru, Mn)氧还原反应(ORR)electrocatalysts使用我们的最近发展激光消融在solution-galvanic合成作为一个置换反应(LASiS-GRR)技术肤浅和surfactant-free nanomanufacturing路线。作品是由各自的目标金属/金属盐氧化还原电位差距以及目标金属和/或金属氧化物的溶解性想要的酸。LASiS-GRR过程使控制大小、元素组成和分布三元的NAs系统的调优最初的金属盐浓度、pH值、激光影响和消融时间。PtCuCo NAs合成元素作文72:12:16 (Pt公司:铜)表现出最好的奥尔催化活性。主要有壳芯结构的外壳主要由Pt和组成一个小数量的铜以及均匀合金PtCuCo核心。质量和特定的活动或性能NAs表明4和6.5倍的改善,分别在相应的活动商业Pt / C。1)我们的表面活性剂/ ligand-free活动合成技术,防止催化部位退化和2)次要合金第二过渡金属铜,转变Ptd带中心之间的最优位置Pt和PtCo二进制NAs,从而优化他们的结合氧的亲和力和含氧物种。建立了LASiS-GRR的多功能性通过其他三元的合成技术相当不错或者活动。

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