In aforementioned CHE calculations, Ni1/CrBr3 was found to undergo a 4e -ORR reaction, while Ni2/CrBr3 and Ni8/CrBr3 favor a 2e -ORR reaction. Employing the CPM mechanism, the most stable magnetic states or those with the best catalytic performance were selected for the three catalysts. All ORR pathway intermediates were optimized under various charges, and their energies were depicted as functions of the applied electrode potential relative to the SHE, as illustrated in Figure in AFM1 before an applied potential of 0.1 V/SHE. However, after an applied potential greater than 0.1 V/SHE, ∠NiOH in AFM2 surpasses that in AFM1. Catalytically, the ORR onset potentials for the three magnetic states shown in the Figure (a-c), at pH = 1 are determined to be 0.81 V/RHE for FIM, 0.89 V/RHE for AFM1, and 0.87 V/RHE for AFM2, respectively, which are lower than those at pH = 13, which are 0.86 V/RHE for FIM, 0.93 V/RHE for AFM1, and 0.90 V/RHE for AFM2. In reaction pathways, FIM and AFM2 favor 2e -ORR with *OOH formation as the RDS, while under AFM1 magnetic state, the ORR pathway shifts to 4e -ORR under acidic conditions, with the RDS transitioning to *OH removal.