Selectively exposing active surfaces and judiciously tuning the near‐surface composition of electrode materials represent two prominent means of promoting electrocatalytic performance. Here, a new class of Pt₃Fe zigzag‐like nanowires (Pt‐skin Pt₃Fe z‐NWs) with stable high‐index facets (HIFs) and nanosegregated Pt‐skin structure is reported, which are capable of substantially boosting electrocatalysis in fuel cells. These unique structural features endow the Pt‐skin Pt₃Fe z‐NWs with a mass activity of 2.11 A mg⁻¹ and a specifc activity of 4.34 mA cm⁻² for the oxygen reduction reaction (ORR) at 0.9 V versus reversible hydrogen electrode, which are the highest in all reported PtFe‐based ORR catalysts. Density function theory calculations reveal a combination of exposed HIFs and formation of Pt‐skin structure, leading to an optimal oxygen adsorption energy due to the ligand and strain effects, which is responsible for the much enhanced ORR activities. In contrast to previously reported HIFs‐based catalysts, the Pt‐skin Pt₃Fe z‐NWs maintain ultrahigh durability with little activity decay and negligible structure transformation after 50 000 potential cycles. Overcoming a key technical barrier in electrocatalysis, this work successfully extends the nanosegregated Pt‐skin structure to nanocatalysts with HIFs, heralding the exciting prospects of high‐effcient Pt‐based catalysts in fuel cells.

中文翻译：

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之字形PtFe纳米线上稳定的高折射率多面铂皮增强了减氧催化作用

选择性地暴露活性表面并明智地调整电极材料的近表面成分是提高电催化性能的两种主要方法。在此，报道了一种新型的具有稳定的高折射率小面（HIF）和纳米偏析的Pt皮肤结构的Pt ₃ Fe锯齿状纳米线（Pt皮肤Pt ₃ Fe z-NWs），能够显着增强纳米管中的电催化作用。燃料电池。这些独特的结构特征赋予Pt-皮肤Pt ₃ Fe z-NWs以2.11 A mg ^-1的质量活度和4.34 mA cm ^-2的比活度相对于可逆的氢电极，在0.9 V时的氧还原反应（ORR）的效率最高，在所有报告的基于PtFe的ORR催化剂中最高。密度函数理论计算揭示了暴露的HIF和Pt皮肤结构的形成的组合，由于配体和应变效应，导致了最佳的氧吸附能，这是ORR活性大大增强的原因。与以前报道的基于HIFs的催化剂相比，Pt皮肤Pt ₃Fe z-NW在5万个潜在循环后保持极高的耐用性，几乎没有活性衰减，并且结构转变可忽略不计。这项工作克服了电催化技术中的关键技术障碍，成功地将纳米分离的Pt皮肤结构扩展为具有HIF的纳米催化剂，预示了燃料电池中高效Pt基催化剂的令人兴奋的前景。