The optimized Fenton- like activity of Fe single- atom sites by Fe atomic clusters-mediated electronic configuration modulation

The performance optimization of isolated atomically dispersed metal active sites is critical but challenging. Here, TiO2@Fe species -N -C catalysts with Fe atomic clusters (ACs) and satellite Fe-N-4 active sites were fabricated to initiate peroxymonosulfate (PMS) oxidation reaction. The AC-induced charge redistribution of single atoms (SAs) was verified, thus strengthening the interaction between SAs and PMS. In detail, the incorporation of ACs optimized the HSO5- oxidation and SO5.- desorption steps, accelerating the reaction pro-gress. As a result, the Vis/TiFeAS/PMS system rapidly eliminated 90.81% of 45 mg/L tetracycline (TC) in 10 min. The reaction process characterization suggested that PMS as an electron donor would transfer electron to Fe species in TiFeAS, generating O-1(2). Subsequently, the h(VB)(+) can induce the generation of electron-deficient Fe species, promoting the reaction circulation. This work provides a strategy to construct catalysts with multiple atom assembly-enabled composite active sites for high-efficiency PMS- based advanced oxidation processes (AOPs).

Automated summary

TiO2@Fe -N -C catalysts with Fe atomic clusters and Fe-N-4 active sites were fabricated for efficient peroxymonosulfate oxidation reactions. The charge redistribution induced by atomic clusters strengthened the interaction between single atoms and peroxymonosulfate. The reaction efficiency was enhanced by optimizing the oxidation and desorption steps, resulting in rapid degradation of tetracycline in the Vis/TiFeAS/PMS system.