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Tailoring Ruthenium Exposure to Enhance the Performance of fcc Platinum@Ruthenium Core-Shell Electrocatalysts in the Oxygen Evolution Reaction

机译:量身定制钌暴露量,以提高fcc铂@钌核壳电催化剂在析氧反应中的性能

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摘要

The catalytic properties of noble metal nanocrystals are a function of their size, structure, and surface composition. In particular, achieving high activity without sacrificing stability is essential for designing commercially viable catalysts. A major challenge in designing state-of-the-art Ru-based catalysts for the oxygen evolution reaction (OER), which is a key step in water splitting, is the poor stability and surface tailorability of these catalysts. In this study, we designed rapidly synthesizable size-controlled, morphology-selective, and surface-tailored platinum-ruthenium core-shell (Pt@Ru) and alloy (PtRu) nanocatalysts in a scalable continuous-flow reactor. These core-shell nanoparticles with atomically precise shells were produced in a single synthetic step with carbon monoxide as the reducing agent. By varying the metal precursor concentration, a dendritic or layer-by-layer ruthenium shell can be grown. The catalytic activities of the synthesized Pt@Ru and PtRu nanoparticles exhibit noticeably higher electrocatalytic activity in the OER compared to that of pure Pt and Ru nanoparticles. Promisingly, Pt@Ru nanocrystals with a ~2-3 atomic layer Ru cuboctahedral shell surpass conventional Ru nanoparticles in terms of both durability and activity.
机译:贵金属纳米晶体的催化性能是其尺寸,结构和表面组成的函数。特别地,在不牺牲稳定性的情况下实现高活性对于设计商业上可行的催化剂是必不可少的。设计最先进的用于氧气析出反应(OER)的Ru基催化剂的主要挑战是这些催化剂的稳定性和表面适应性差,这是水分解的关键步骤。在这项研究中,我们在可扩展的连续流反应器中设计了可快速合成的尺寸控制,形态选择性和表面定制的铂-钌核-壳(Pt @ Ru)和合金(PtRu)纳米催化剂。这些具有原子精确壳的核壳纳米粒子是在一个合成步骤中使用一氧化碳作为还原剂生产的。通过改变金属前体的浓度,可以生长树枝状或逐层钌壳。与纯Pt和Ru纳米颗粒相比,合成的Pt @ Ru和PtRu纳米颗粒在OER中表现出明显更高的电催化活性。令人信服的是,具有约2-3个原子层Ru立方八面体壳的Pt @ Ru纳米晶体在耐久性和活性方面都超过了传统的Ru纳米颗粒。

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