Charge and spin manipulations of electrons are considered to be of great significance in boosting the catalytic activity of MNC electrocatalysts. However, to the best of our knowledge, most current studies focus only on the charge engineering, the interplay between spin and charge is not well understood, and the simultaneous manipulation of both charge and spin remains challenging. Herein, we show that the cooperative interplay between charge itineration and spin-polarization of electrons has a profound impact on the catalytic behavior through density functional theory (DFT) calculations for the first time. Following this concept, we report a Fe-Ni atomic pair as a superior bifunctional catalyst for high performance ORR and OER, with a very small potential difference (ΔE) of 0.691 V. We confirm that the coexistence of Fe 3d itinerant charge and moderate spin polarization (magnetic moment: 1.48 μ_B) is responsible for the superior functional catalytic activity for the FeNi atomic pairs.

电子的电荷和自旋操纵被认为对提高M N的催化活性具有重要意义。C电催化剂。然而，据我们所知，当前大多数研究仅集中在电荷工程上，对自旋和电荷之间的相互作用尚不甚了解，并且同时操纵电荷和自旋仍然具有挑战性。本文中，我们首次展示了电荷迭代和电子的自旋极化之间的协同相互作用，对密度的变化，首次通过密度泛函理论（DFT）计算对催化行为产生了深远的影响。遵循这一概念，我们报告了Fe-Ni原子对是高性能ORR和OER的优良双功能催化剂，其电势差（ΔE）很小，为0.691V。我们证实了Fe 3d流动剂电荷和适度自旋共存偏振（磁矩：1.48μ_乙）负责Fe Ni原子对的出色功能催化活性。