Fully dispersed cobalt diatomic site with significantly improved Fenton-like catalysis performance for organic pollutant degradation.

ABSTRACT

A novel strategy for better catalytic performance in terms of precisely tuning the metal atom number of active centers is gradually getting attention. In this paper, the Co atom pair sites on N-doped porous carbon was engineered. The binuclear Co2 site structure was identified by aberration-corrected scanning transmission electron microscopy and X-ray absorption spectroscopy. As expected, the Co2NC display an outstanding Fenton-like catalysis activity in tetracycline degradation with turnover frequency exceeding 0.91 min-1 that is approximately 4 times higher than the conventional CoN4 site. The EPR tests indicated that the ROS strength stimulated by the binuclear site was much stronger than that of single site. Theoretical density functional theory calculations reveal that the optimized adsorption configuration is the O1 of peroxymonosulfate (PMS) interacting with two Co atoms, leading to stronger interaction effect and electron transfer for PMS comparing to single atom sites.