Abstract
The catalytic performance of single-atom catalysts (SACs) strongly depends on their electronic occupation at 3d-orbitals and spin exchange interaction. However, the correlation between catalytic activity and the optimal spin configuration in accelerating oxygen evolution reaction (OER) still needs to be understood. Herein, we suggest a bimetallic single-atom dimer with asymmetric spin polarization to eliminate the antiferromagnetic contribution, in which the bonding interaction and charge transfer between active sites and reactants can be effectively optimized by this intriguing residual ferromagnetic behavior. As a result, the activation barrier of OER at rate-limiting step reduces effectively due to this asymmetric spin occupation. This work provides a new insight into accelerating the OER by regulating spin electron occupation in SACs.
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