21:T4ac,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-N₄ 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 progress. 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 ¹O₂. 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).22:T49f,Enhancing the peroxymonosulfate (PMS) activation efficiency to generate more radicals is vital to promote the Fenton-like reaction activity, however, how to promote the PMS adsorption and accelerate the interfacial electron transfer to boost its activation kinetics remains a great challenge. Herein, we prepared Cu-doped defect-rich In₂ O₃ (Cu-In₂ O₃ /O_v ) catalysts containing asymmetric Cu-O_v -In sites for PMS activation in water purification. The intrinsic catalytic activity is that the side-on adsorption configuration of the O-O bond (Cu-O-O-In) at the Cu-O_v -In sites significantly stretches the O-O bond length. Meanwhile, the Cu-O_v -In sites increase the electron density near the Fermi energy level, promoting more and faster electron transfer to the O-O bond for generating more SO₄ ⋅^- and ⋅OH. The degradation rate constant of tetracycline achieved by Cu-In₂ O₃ /O_v is 31.8 times faster than In₂ O₃ /O_v , and it shows the possibility of membrane reactor for practical wastewater treatment.

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