Active Center Inheritance: A Design Principle for Constructing Atomically Dispersed Bimetallic OER/ORR Catalysts Derived from Single-Atom Catalysts

Abstract

Atomically dispersed bimetallic catalysts (ADCs), an emerging class of electrocatalysts, combine the synergistic advantages of dual-metal active sites with the atomic dispersion and high metal utilization efficiency characteristic of single-atom catalysts (SACs). Their unique structural features offer the potential to exceed the catalytic performance of conventional systems but simultaneously pose challenges due to the absence of well-established rational design principles. This paper proposes and validates a structural design strategy, “Active Center Inheritance,” wherein high-performance SACs are transformed into ADCs by retaining the same active center (M–Nx). This approach not only preserves high catalytic activity but also significantly reduces the computational cost associated with density functional theory (DFT) calculations over 13,500 candidate systems, thereby accelerating the discovery of bifunctional electrocatalysts. A total of 17 high-performance oxygen evolution reaction (OER)/oxygen reduction reaction (ORR) bifunctional catalysts were identified through this strategy. This strategy was successfully generalized to three other ADC structural systems with different spatial arrangements. Moreover, a unified descriptor (φ), composed of four key electronic and atomic features, was constructed to effectively correlate the adsorption behaviors of critical reaction intermediates (*OH, *O, and *OOH) across diverse systems. The results reveal that SACs and ADCs can achieve comparable catalytic activity when constructed with the same M–Nx active center, thereby enabling the synergistic optimization of active sites. This work provides a theoretical basis and a rational design framework for the development of efficient multisite electrocatalysts.