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In recent years, metal-organic framework derivatives have been regarded as materials with great potential for water treatment applications. In this study, we employed a polyvinylpyrrolidone (PVP)-assisted copper-cobalt bimetallic zeolitic imidazole framework (ZIF) as a template to rationally design nanosheet-like mixed metal oxide embedded nitrogen-doped carbon (CuCoO-PC). CuCoO-PC exhibited excellent degradation potential towards metronidazole (MNZ) and achieved almost complete degradation within 7 min through the activation of peroxymonosulfate (PMS). Importantly, the introduction of copper into CuCoO-PC established strong interactions between copper and cobalt, accelerating the activation performance of PMS. Furthermore, PVP, rich in nitrogen atoms, formed strong coordination interactions with ZIF precursors, which effectively protected the morphological stability of ZIF at high temperature, preventing collapse and aggregation. Meanwhile, the formation of nitrogen-doped carbon networks provides a pathway for the generation of non-radical. The study found that CuCoO-PC continuously activated PMS, generating various reactive oxygen species (ROS), among which SO 4 •- and 1O 2 played decisive roles. By calculating the HOMO, LUMO, and Fukui functions, we identified the reactive sites of MNZ and proposed possible degradation pathways. CuCoO-PC demonstrated excellent catalytic performance, reduced toxicity of intermediate products, and good reusability, all of which highlight its enormous potential in practical applications. [Display omitted] • CuCoO-PC composites are prepared using PVP to enrich the nitrogen content. • CuCoO-PC/PMS system exhibits prominent catalytic performance for MNZ removal. • SO 4 •- and 1O 2 was the main active substance involved in the MNZ degradation. • CuCoO-PC was stable and effective in multiple cycles of MNZ degradation efficiency. • The most reactive site on MNZ molecule was predicted by DFT calculation. [ABSTRACT FROM AUTHOR]

[Display omitted] • N-doped La 2 CuO 4 had been synthesized using melamine as the N precursor. • N-doped La 2 CuO 4 showed enhanced catalytic activity and stability. • Density Functional Theory (DFT) calculations were performed to verify the results. • A mechanism of phenol degradation was proposed. • The toxicity of degradation intermediates was greatly reduced. Herein, N-doped perovskite La 2 CuO 4 (LCO) (N-LCO(M)) was fabricated by sol–gel rapid calcination method using melamine (M) as N source/ligand, and applied for the catalytic wet air oxidation (CWAO) to degrade high-concentration phenol-containing simulated wastewater. The experimental results exhibited that N-LCO(M) illustrated enhanced phenol degradation efficiency. Thereinto, 87.9% COD degradation efficiency was achieved in simulated wastewater containing 8000 mg/L phenol, while for undoped LCO prepared with citric acid (CA) as ligand (LCO(CA)) was only 43.8%. The systematic characterizations and density functional theory (DFT) calculations were utilized to verify the above results. The results revealed that N doping favored the formation of more oxygen vacancies (*) and facilitated the charge transfer between Cu and O. More oxygen vacancies (*) reinforced the ability of N-LCO(M) to adsorb O 2 to form reactive oxygen species (O*), and meanwhile, the charge transfer between Cu and O was manifested as the redox cycle of the catalytic active metal Cu2+/Cu1+. The redox cycle also promoted the formation of O 2 − and HO, making the more exhaustive degradation of phenol. This successfully proved that N doping was core to improving the activity and stability of N-LCO(M). Moreover, a possible mechanism of phenol degradation was proposed based on the experimental results and DFT calculations. Eventually, the toxicity of the intermediate products was further evaluated by quantitative structure–activity relationship (QSAR) analysis, showing the significantly reduced toxicity of the intermediate products. Overall, the proposed CWAO technique is a green and promising wastewater treatment method. [ABSTRACT FROM AUTHOR]

[Display omitted] • A composite PMS activator of S-doped g-C 3 N 4 /NiCo 2 O 4 was obtained. • S doping widens the difference in the work functions of CNS and NCO. • Enhanced BIEF promotes the directional transfer of electrons from CNS to NCO. • 1O 2 was formed mainly through SO 4 •−, •OH and •O 2 − conversion. Transition metal oxide-mediated heterogeneous peroxymonosulfate (PMS) activation on organic pollutant degradation has attracted much attention, where continuous redox cycling between high and low valence metal ions is the key step as it relates to the radical generation. Herein, a composite PMS activator of S-doped g-C 3 N 4 /NiCo 2 O 4 (CNS_NCO) was constructed and exhibited excellent tetracycline (TC) degradation performance with 96.9% removal efficiency within 30 min. Experimental and theoretical calculations indicated that S doping not only widened the difference in the work function of CNS and NCO, but also enhanced the built-in electric field intensity of CNS_NCO heterojunctions, resulting in more electron transfer from CNS to NCO in a directional manner and accelerating the Co(III)/Co(II) and Ni(III)/Ni(II) redox cycle to form more reactive oxygen species (ROS). It was demonstrated that 1O 2 (main ROS) was formed mainly through SO 4 •−, •OH and •O 2 − (minor ROS) conversion. Meanwhile, high-valent cobalt-oxo (CoIV = O) species also played an important role in TC degradation. [ABSTRACT FROM AUTHOR]