1. Ultra-high-density double-atom catalyst with spin moment as activity descriptor for oxygen reduction reaction
- Author
-
Lv, Peng, Lv, Wenjing, Wu, Donghai, Tang, Gang, Yan, Xunwang, Lu, Zhansheng, and Ma, Dongwei
- Subjects
Condensed Matter - Materials Science - Abstract
One of the great challenges facing atomically dispersed catalysts, including single-atom catalyst (SAC) and double-atom catalyst (DAC) is their ultra-low metal loading (typically less than 5 wt%), basically limiting the practical catalytic application, such as oxygen reduction reaction (ORR) crucial to hydrogen fuel cell and metal-air battery. Although some important progresses have been achieved on ultra-high-density (UHD) SACs, the reports on UHD-DACs with stable uniform dispersion is still lacking. Herein, based on the experimentally synthesized M2N6 motif (M = Sc-Zn), we theoretically demonstrated the existence of the UHD-DACs with the metal loading > 40 wt%, which were confirmed by systematic analysis of dynamic, thermal, mechanical, thermodynamic, and electrochemical stabilities. Furthermore, ORR activities of the UHD-DACs are comparable with or even better than those of the experimentally synthesized low-density (LD) counterparts, and the Fe2N6 and Co2N6 UHD-DACs locate at the peak of the activity volcano with ultra-low overpotentials of 0.31 and 0.33 V, respectively. Finally, spin magnetic moment of active center is found to be a catalytic descriptor for ORR on the DACs. Our work will stimulate the experimental exploration of the ultra-high-density DACs and provides the novel insight into the relationship between ORR activity of the DACs and their spin states., Comment: Accept; Physical Review Applied, online https://journals.aps.org/prapplied/accepted/6e070Ad3M481130513b194765dfdaa4e7c6b6b46d
- Published
- 2023