Computational High-Throughput Screening of Transition-Metal C 2 N 2 Electrocatalysts for Oxygen Reduction Reactions

With the increasing demand for efficient energy conversion technologies, stable and highly active electrocatalysts have become a key area of research. In recent years, transition-metal (TM) nitrogen-doped carbon-based catalysts have emerged as promising electrocatalysts due to their unique physical and chemical properties. Among the various catalysts aimed at overcoming the efficiency bottlenecks of traditional energy conversion, TM-C2N2 has garnered significant attention for its high activity and excellent atomic utilization, demonstrating outstanding performance in the electrochemical oxygen reduction reaction (ORR). However, despite the substantial potential of TM-C2N2 in ORR, the impact of different central atoms on the electronic structure and catalytic performance of C2N2 has not been systematically studied or deeply explored. In this study, density functional theory combined with high-throughput screening methods was employed to systematically screen TM-C2N2 monolayer catalysts composed of different central atoms and to investigate their interaction patterns and catalytic mechanisms in ORR. The computational results indicate that altering the d-band center can effectively reduce excessive adsorption of intermediates, and that the interaction strength between intermediates and TM-C2N2 is a key factor determining ORR catalytic activity. Among the 38 candidate materials, we identified two promising candidates, Ti–C2N2 and Mn–C2N2, which not only exhibit low overpotentials of 0.34 and 0.41 V, respectively, but also possess high thermodynamic and electrochemical stability. This study introduces a novel nonprecious metal catalyst for ORR and reveals the catalytic mechanism of TM-C2N2 materials in ORR, providing valuable theoretical guidance for structural optimization and performance enhancement in future catalyst design.