Heterogeneous catalysts promoting efficient production of reactive species and dynamically stabilized electron transfer mechanisms for peroxomonosulfates (PMS) still lack systematic investigation. Herein, a more stable magnetic layered double oxides (CFLDO/N-C), was designed using self-polymerization and high temperature carbonization of dopamine. The CFLDO/N-C/PMS system effectively activated PMS to remove 99% (k = 0.737 min⁻¹) of tetracycline (TC) within 10 min. The CFLDO/N-C/PMS system exhibited favorable resistance to inorganic anions and natural organics, as well as satisfactory suitability for multiple pollutants. The magnetic properties of the catalyst facilitated the separation of catalysts from the liquid phase, resulting in excellent reproducibility and effectively reducing the leaching of metal ions. An electronic bridge was constructed between cobalt (the active platform of the catalyst) and PMS, inducing PMS to break the O–O bond to generate the active species. The combination of static analysis and dynamic evolution confirmed the effective adsorption of PMS on the catalyst surface as well as the strong radical-assisted electron transfer process. Eventually, we further identified the sites where the reactive species attacked the TC and evaluated the toxicity of the intermediates. These findings offer innovative insights into the rapid degradation of pollutants achieved by transition metals in SR-AOPs and its mechanistic elaboration.

The photocatalytic performances are highly dependent on the charge separation and surface reaction kinetics of photocatalysts. Aiming at figuring out the effects of co-catalyst with the lower Fermi level on photocatalytic activity, we tuned the Fermi level of Pt nanoparticles on g-C₃N₄(GCN) by introducing Co atom. Experimental results show that lowering the Fermi level of co-catalyst does not alter light absorption of GCN due to the invariable structure. Besides, Pt₃Co with a lower Fermi level contributes less positive influence on charge separation in GCN due to an opposite effect from the stronger electron-trap ability of Pt₃Co and increased band bending in GCN-Pt₃Co. The density functional theory (DFT) calculations indicate that GCN-Pt₃Co has faster surface reaction kinetics than GCN-Pt, owing to easier dissociation of H₂O molecules and faster desorption of H* on Pt₃Co. Consequently, GCN-Pt₃Co exhibits an excellent H₂ evolution rate with 2.91 mmol·g^-1·h^-1, which 2.67 times that of GCN-Pt.