Synergy of dual-atom catalysts deviated from the scaling relationship for oxygen evolution reaction

• Published in: Nature communications Vol. 14; no. 1; p. 4449
• Main Authors: Fang, Cong, Zhou, Jian, Zhang, Lili, Wan, Wenchao, Ding, Yuxiao, Sun, Xiaoyan
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 24-07-2023; Nature Publishing Group; Nature Portfolio
• Subjects: 119/118; 639/638/563/979; 639/638/77/885; 639/638/77/886; Adsorption; Catalysts; Coupling; Density functional theory; Electrocatalysis; Evolution; Graphene; Humanities and Social Sciences; multidisciplinary; Optimization; Oxygen; Oxygen evolution reactions; Reaction mechanisms; Science; Science (multidisciplinary); Single atom catalysts
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-023-40177-1

Dual-atom catalysts, particularly those with heteronuclear active sites, have the potential to outperform the well-established single-atom catalysts for oxygen evolution reaction, but the underlying mechanistic understanding is still lacking. Herein, a large-scale density functional theory is employed to explore the feasibility of *O-*O coupling mechanism, which can circumvent the scaling relationship with improving the catalytic performance of N-doped graphene supported Fe-, Co-, Ni-, and Cu-containing heteronuclear dual-atom catalysts, namely, M’M@NC. Based on the constructed activity maps, a rationally designed descriptor can be obtained to predict homonuclear catalysts. Seven heteronuclear and four homonuclear dual-atom catalysts possess high activities that outperform the minimum theoretical overpotential. The chemical and structural origin in favor of *O-*O coupling mechanism thus leading to enhanced reaction activity have been revealed. This work not only provides additional insights into the fundamental understanding of reaction mechanisms, but also offers a guideline for the accelerated discovery of efficient catalysts.
The utilization of dual-atom catalysts holds the potential in surpassing single-atom catalysts for oxygen evolution reactions. Here, the authors examine the mechanism of dual-atom catalysts for oxygen evolution reaction and identify catalyst optimization recipes via large-scale computations.