Nonprecious metal catalysts (NPMCs) FeNC are promising alternatives to noble metal Pt as the oxygen reduction reaction (ORR) catalysts for proton‐exchange‐membrane fuel cells. Herein, a new modulation strategy is reported to the active moiety FeN₄ via a precise “single‐atom to single‐atom” grafting of a Pt atom onto the Fe center through a bridging oxygen molecule, creating a new active moiety of Pt₁O₂Fe₁N₄. The modulated FeNC exhibits remarkably improved ORR stabilities in acidic media. Moreover, it shows unexpectedly high catalytic activities toward oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), with overpotentials of 310 mV for OER in alkaline solution and 60 mV for HER in acidic media at a current density of 10 mA cm⁻², outperforming the benchmark RuO₂ and comparable with Pt/C(20%), respectively. The enhanced multifunctional electrocatalytic properties are associated with the newly constructed active moiety Pt₁O₂Fe₁N₄, which protects Fe sites from harmful species. Density functional theory calculations reveal the synergy in the new active moiety, which promotes the proton adsorption and reduction kinetics. In addition, the grafted Pt₁O₂ dangling bonds may boost the OER activity. This study paves a new way to improve and extend NPMCs electrocatalytic properties through a precisely single‐atom to single‐atom grafting strategy.

中文翻译：

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Pt1在Fe上的单原子至单原子接枝？N4中心：Pt1 @ Fe ？N ？具有显着增强性能的C多功能电催化剂

非贵重金属催化剂（NPMCs）的Fe  Ñ  C被看好替代贵金属Pt作为氧还原反应（ORR）催化剂的质子交换膜燃料电池。在本文中，一个新的调制策略被报告为活性部分的Fe  Ñ ₄经由精确的“单原子的单原子”的Pt原子上通过桥联氧分子中的Fe中心的接枝，产生的Pt的新活性部分₁  Ò ₂ 铁₁  ñ ₄。经调制的Fe  Ñ C在酸性介质中显示出显着改善的ORR稳定性。此外，它显示了以10mA cm 2的电流密度朝向析氧反应出乎意料的高催化活性（OER）和析氢反应（HER），与在碱性溶液和在酸性介质310毫伏OER的超电势60毫伏HER ^{-如图2所示}，其性能优于基准RuO ₂并与Pt / C（20％）相当。增强的多功能电催化性能与新构建的活性部分相关联的Pt ₁  Ò ₂ 铁₁  Ñ ₄，可以保护铁部位免受有害物质的侵害。密度泛函理论计算揭示了新活性部分中的协同作用，从而促进了质子的吸附和还原动力学。另外，接枝的Pt ₁  Ò ₂ 悬空键可促进OER活性。这项研究为通过精确的单原子至单原子接枝策略改善和扩展NPMC的电催化特性开辟了一条新途径。