The spin of the electron is decisive to understand electronic interactions in heterogeneous catalysis, mainly because the stabilizing Quantum Spin Exchange Interactions (QSEI) are always a significant contribution to the energy of magnetic catalysts and absorbates during reaction events. Cooperative QSEI in compositions with multi-atomic open-shell configurations (QSEI-OS) maximize the influence of the spin dependent potentials, determining the electronic properties of magnetic materials and shaping their reactivity. In this paper, we explain that because of the intra- and inter- atomic QSEI-OS, high-spin (3d⁵) antiferromagnetic (AFM) metals like Cr and Mn can be more inert (or “noble”) than Au itself towards the formation of covalent bonds with hydrogen atoms. AFM QSEI-OS lead to a relative higher destabilization of the unoccupied (spin-)orbitals (Mott upper band) in Cr and Mn compared with other metals. In oxygen adsorption, QSEI-OS lead to the reduction of the electronic repulsions in occupied 3d⁵ orbitals with a concomitant decrease of the chemisorption enthalpy of the oxygen atoms. Since hydrogen and oxygen atoms are the most important intermediates in relevant catalytic processes like oxygen reduction reaction and water splitting, we observe how the effect of QSEI-OS needs to be properly incorporated as a critical factor to understand the activity of catalysts based on magnetic metals.

电子的自旋对于理解非均相催化中的电子相互作用具有决定性的作用，这主要是因为稳定的量子自旋交换相互作用（QSEI）始终是反应过程中对磁性催化剂和被吸收物能量的重要贡献。具有多原子开壳构型（QSEI-OS）的组合物中的协同QSEI可最大程度地发挥自旋相关电位的影响，从而确定磁性材料的电子性质并影响其反应性。在本文中，我们解释说，由于原子内和原子间QSEI-OS，高自旋（3d ⁵）诸如Cr和Mn这样的反铁磁（AFM）金属在与氢原子形成共价键方面比Au本身更惰性（或“贵重”）。与其他金属相比，AFM QSEI-OS导致Cr和Mn中未占据的（自旋）轨道（Mott上带）的相对不稳定。在氧吸附中，QSEI-OS导致在被占据的3d ⁵轨道中的电子排斥力降低，同时氧原子的化学吸附焓降低。由于氢和氧原子是氧气还原反应和水分解等相关催化过程中最重要的中间体，因此我们观察到如何适当地结合QSEI-OS的作用作为了解基于磁性金属的催化剂活性的关键因素。