Efficient Removal of Antibiotic Resistance Genes through 4f‐2p‐3d Gradient Orbital Coupling Mediated Fenton‐Like Redox Processes

Abstract

Peroxymonosulfate (PMS) mediated radical and nonradical active substances can synergistically achieve the efficient elimination of antibiotic resistance genes (ARGs). However, enhancing interface electron cycling and optimizing the coupling of the oxygen‐containing intermediates to improve PMS activation kinetics remains a major challenge. Here, Co doped CeVO4 catalyst (Co‐CVO) with asymmetric sites was constructed based on Ce 4f‐O 2p‐Co 3d gradient orbital coupling. The catalyst achieved approximately 2.51×105 copies/mL of extracellular ARGs (eARGs) removal within 15 minutes, exhibited ultrahigh degradation rate (k = 1.24 min‐1). The effective gradient 4f‐2p‐3d orbital coupling precisely regulates the electron distribution of Ce‐O‐Co active center microenvironment, while optimizing the electronic structure of Co 3d states (especially the occupancy of eg), promoting the adsorption of oxygen‐containing intermediates. The generated radical and nonradical generated by interfacial electron cycling enhanced by the reduction reaction of PMS at the Ce site and the oxidation reaction at the Co site achieved a significant mineralization rate of ARGs (83.4%). The efficient removal of ARGs by a continuous flow reactor for 10 hours significantly reduces the ecological risk of ARGs in actual wastewater treatment.

Electronic Metal‐Support Interactions Boost *OOH Intermediate Generation in Cu/In2Se3 for Electrochemical H2O2 Production

“…It is worth noting that the brightness of the atomic columns depends on the atomic number in HAADF-STEM. [24] The brightness levels of Se (34) and In (49) are brighter than Cu (29). The weak intensity spot by the yellow cycle is Cu atom, which is determined by line scan x-y rectangle region (Figure 1f).…”

Precise Modulation of the Coordination Environment of Single Cu Site Catalysts to Regulate the Peroxymonosulfate Activation Pathway for Water Remediation

“…These results indicated that PMS was the easiest to be adsorbed on the Cu-N 3 site compared with Cu-N 4 and Cu-N 2 owing to the strongest O–O bond stretch effect. However, Cu-N 3 could not get the best BPA removal performance due to the strong adsorption energy that was not conducive to the desorption of the products. , …”

“…However, Cu-N 3 could not get the best BPA removal performance due to the strong adsorption energy that was not conducive to the desorption of the products. 42,43 The differential charge diagrams of PMS molecules adsorbed on Cu-N 2 , Cu-N 3 , and Cu-N 4 are shown in Figure 4d−f. The Cu sites of Cu-N x SACs further reveal a significant electron transfer from Cu-N x SACs to PMS, reflecting the chemisorption of PMS on the Cu site.…”

Unlocking Bimetallic Active Centers via Heterostructure Engineering for Exceptional Phosphate Electrosorption: Internal Electric Field-Induced Electronic Structure Reconstruction

“…Such dual metal composites generally express inherited properties from their single counterparts and have bonus synergistic effects. The different range coupling of the heteroatom center modulates the electronic structure and local electron density. , …”

“…The different range coupling of the heteroatom center modulates the electronic structure and local electron density. 12,13 Among various metallic materials, La-based materials are consistently regarded as effective tools for phosphate removal due to the strong affinity between La and P even at trace levels. 14 Ce-based materials, possessing a similar electronic configuration and physicochemical properties to La, also exhibit favorable potential in phosphate capture owing to their small ionic potential and strong alkalinity.…”