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[Display omitted] • mAg 3 PO 4 @g-C 3 N 4 /PDS/Vis enhance CBZ degradation rate by 3.6-fold. • 87.15 % mineralization of CBZ was achieved in 30 min via mAg 3 PO 4 @g-C 3 N 4 /PDS/Vis. • 1O 2 -dominated ring-opening is identified to be key for improved mineralization. • Multiple PhACs in the effluent are simultaneously degraded with high mineralization. The wide occurrence of pharmaceutically active contaminants (PhACs) in aquatic environments has received more and more concern owing to the associated high risks to ecosystems. Even worse, conventional wastewater treatment techniques fail to provide effective decontamination for these emerging contaminants. Herein, we designed and constructed mAg 3 PO 4 @g-C 3 N 4 heterojunction for a persulfate-assisted photocatalytic system (mAg 3 PO 4 @g-C 3 N 4 /PDS/Vis) for the rapid and effective degradation of PhACs. Superior mineralization of CBZ (87.15 %) was achieved within 30-minute treatment with mAg 3 PO 4 @g-C 3 N 4 /PDS/Vis, exhibiting 11-fold enhancement compared to mAg 3 PO 4 /Vis system. Integrating experimental investigations with theoretical calculations, singlet oxygen (1O 2) was identified as the key reactive species, while the 1O 2 -dominated ring-opening pathway contributed significantly to the high mineralization of CBZ. Moreover, mAg 3 PO 4 @g-C 3 N 4 /PDS/Vis showed robust degradation performance of multiple PhACs across various water matrices. Multiple PhACs could be simultaneously degraded with high mineralization efficiency in the wastewater effluent, demonstrating the promising application of mAg 3 PO 4 @g-C 3 N 4 /PDS/Vis for decontaminating emerging contaminants in wastewater treatment. [ABSTRACT FROM AUTHOR]

Singlet oxygen (1O 2) plays a crucial role in Fenton-like reactions due to its high efficiency and selectivity in removing trace organic pollutants from complex water matrices. Defect engineering, which allows the efficient exposure of active sites and optimization of electronic structures, has rapidly emerged as a fundamental strategy for enhancing 1O 2 yield. Herein, we introduce tunable sulfur vacancy (V S) density into Co 9 S 8 catalysts for peroxymonosulfate (PMS) activation. The modulation of the octahedral Co (CoS 6) and tetrahedral Co (CoS 4) electronic structures by V S triggers the unexpected selective generation of 1O 2. The V S /PMS system exhibits excellent resistance to interference and highly selective degradation of electron-donating organic pollutants. Experimental and theoretical calculations revealed a new evolutionary route for 1O 2 involving two phases (Phase I: HSO 5 − → *O, Phase II: *O + HSO 5 − →*OO → 1O 2). This study provides a molecular-level understanding of V S -mediated catalytic selectivity for high-efficient decontamination applications. [Display omitted] • Co 9 S 8 catalysts with tunable V S was fabricated to PMS activation for contaminants degradation. • The optimized V S /PMS system achieved 1O 2 -dominated degradation mechanism. • Regulation d-band center of Co-3d orbital boosted the process of HSO 5 − adsorption and activation. • Combining experiment and DFT results revealed a new evolutionary route of 1O 2. [ABSTRACT FROM AUTHOR]

• Fe and O codopants substantially accelerated the electron transfer of g-C 3 N 4 for PMS activation. • Efficient BPA removal was achieved at high salinity and within wider pH ranges. • High-valent iron-oxo species and singlet oxygen were identified as two main reactive species. • Nonradical pathways were elucidated based on experimental and theoretical analyses. Peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs) for wastewater treatment have recently attracted widespread interests. However, the degradation of organic pollutants via traditional radical-dominated pathway is severely limited by the side reactions between radicals and the co-existing inorganic anions, especially under high salinity conditions. Herein, an efficient Fe/O co-doped g-C 3 N 4 nanosheet catalyst was synthesized to dominantly activate PMS through a dual non-radical pathway with the singlet oxygen and high-valent iron-oxo species (Fe(V)=O). The rapid degradation of model pollutant bisphenol A (BPA) was achieved by dosing PMS (1 mM), catalyst (0.1 g/L) in a simulated high-salt wastewater (≥200 mM) of the developed Fe/O-doped g-C 3 N 4 +PMS system with a reaction rate constant of 1204-fold higher than that in g-C 3 N 4 +PMS system. The O and Fe co-dopants could reconfigurate the electronic structure of pristine g-C 3 N 4 to produce more non-radical active species. The formed Fe(V)=O played a main role in the BPA degradation by promoting electron transfer from BPA molecule to the "metastable PMS/catalyst complex", which was verified by electrochemical tests and density functional theory calculations. The auxiliary transient productions of · OH+SO 4 · – species were also favorable for the pollutant degradation. Excellent reusability in a wide pH range confirmed the practical application prospects of the Fe/O-doped g-C 3 N 4 +PMS system. The successive addition of PMS with a low dosage into the system rich in pollutants was confirmed to favor the PMS utilization. Our work unveils the potential applications of a non-radical dominated process for the decontamination of organic pollutants in saline water. [ABSTRACT FROM AUTHOR]