铁磁性
金属
催化作用
过渡金属
密度泛函理论
铁磁性
自旋(空气动力学)
电解质
电催化剂
材料科学
交换电流密度
化学物理
化学
无机化学
凝聚态物理
计算化学
冶金
物理
磁化
物理化学
电化学
电极
热力学
磁场
塔菲尔方程
量子力学
生物化学
作者
Yi-jie Chen,Jun Wen,Zhenlin Luo,Fu-li Sun,Wen‐Xian Chen,Gui‐Lin Zhuang
摘要
Magnetic property (e.g. spin order) of support is of great importance in the rational design of heterogeneous catalysts. Herein, we have taken the Ni-supported ferromagnetic (FM) CrBr3 support (Nix/CrBr3) to thoroughly investigate the effect of spin-order on electrocatalytic oxygen reduction reaction (ORR) via spin-polarized density functional theory calculations. Specifically, Ni loading induces anti-FM coupling in Ni–Cr, leading to a transition from FM-to-ferrimagnetic (FIM) properties, while Ni–Ni metallic bonds create a robust FM direct exchange, benefiting the improvement of the phase transition temperature. Interestingly, with the increase in Ni loading, the easy magnetic axis changes from out-of-plane (2D-Heisenberg) to in-plane (2D-XY). The adsorption properties of Nix/CrBr3, involving O2 adsorption energy and configuration, are not governed by the d-band center but strongly correlate with magnetic anisotropy. It is noteworthy that the applied potential and electrolyte acidity triggers spin-order transition phenomena during the ORR and induces the catalytic pathway change from 4e− ORR to 2e− ORR with the excellent onset potential of 0.93 V/reversible hydrogen electrode, comparable to the existing most excellent noble-metal catalysts. Generally, these findings offer new avenues to understand and design heterogeneous catalysts with magnetic support.
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