The superoxide radical (•O)-mediated peroxymonosulfate (PMS)-based photo-Fenton-like reaction enables highly selective water decontamination. Nevertheless, the targeted construction of •O-mediated photo-Fenton-like system has been challenging. Herein, we developed an electron-rich/-poor dual sites driven •O-mediated cascade photo-Fenton-like system by modulating electron density. Experimental and theoretical results demonstrated that PMS was preferentially adsorbed on electron-poor Co site. This adsorption promoted O-O bond cleavage of PMS to generate hydrogen peroxide (HO), which then migrated to electron-rich O site to extract e electrons for O-H bond cleavage, rather than competing with PMS for Co site. The developed versatile cascade reaction system could selectively eliminate contaminants with low n-octanol/water partition constants (K) and dissociation constants (pKa) and remarkably resist inorganics (Cl, HPO and NO), humic acid (HA) and even real water matrices (tap water and secondary effluent). This finding provided a novel and plausible strategy to accurately and efficiently generate •O for the selective water decontamination.
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http://dx.doi.org/10.1016/j.jhazmat.2024.133749 | DOI Listing |
Nanoscale Horiz
January 2025
Center for Research on Advanced Fiber Technologies (CRAFT), Materials Research Institute and Huck Institute of Life Sciences, Pennsylvania State University, University Park, Pennsylvania 16802, USA.
Molecular composites, such as bone and nacre, are everywhere in nature and play crucial roles, ranging from self-defense to carbon sequestration. Extensive research has been conducted on constructing inorganic layered materials at an atomic level inspired by natural composites. These layered materials exfoliated to 2D crystals are an emerging family of nanomaterials with extraordinary properties.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Nankai University, Department of Chemistry, Weijin road, 300071, Tianjin, CHINA.
Localized surface plasmon resonance (LSPR) metals exhibit remarkable light-absorbing property and unique catalytic activity, attracting significant attention in photocatalysts recently. However, the practical application of plasmonic nanometal is hindered by challenge of energetic electrons extraction and low selectivity. The energetic carriers generated in nanometal under illumination have extremely short lifetimes, leading to rapid energy loss.
View Article and Find Full Text PDFNat Chem Biol
January 2025
Shanghai Key Laboratory of Regulatory Biology, Institute of Biomedical Sciences and School of Life Sciences, East China Normal University, Shanghai, China.
Voltage-gated ion channels (VGICs) are crucial targets for neuropsychiatric therapeutics owing to their role in controlling neuronal excitability and the established link between their dysfunction and neurological diseases, highlighting the importance of identifying modulators with distinct mechanisms. Here we report two small-molecule modulators with the same chemical scaffold, Ebio2 and Ebio3, targeting a potassium channel KCNQ2, with opposite effects: Ebio2 acts as a potent activator, whereas Ebio3 serves as a potent and selective inhibitor. Guided by cryogenic electron microscopy, patch-clamp recordings and molecular dynamics simulations, we reveal that Ebio3 attaches to the outside of the inner gate, employing a unique non-blocking inhibitory mechanism that directly squeezes the S6 pore helix to inactivate the KCNQ2 channel.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Department of Chemistry, 1102 Natural Sciences II, University of California, Irvine, California 92697, United States.
The development of molecular species with switchable magnetic properties has been a long-standing challenge in chemistry. One approach involves binding an analyte, such as protons, to a compound to trigger a change in magnetism. Transition metal complexes have been targeted for this type of magnetic modulation because they can undergo changes in their spin states.
View Article and Find Full Text PDFInorg Chem
January 2025
Key Laboratory of Materials Modification by Laser, Ion and Electron Beams (Dalian University of Technology), Ministry of Education, Dalian 116024, China.
Atomically precise nanoclusters, distinguished by their unique nuclearity- and structure-dependent properties, hold great promise for applications of energy conversion and electronic transport. However, the relationship between ligands and their properties remains a mystery yet to be unrevealed. Here, the influence of ligands on the electronic structures, optical properties, excited-state dynamics, and transport behavior of ReS dimer clusters with different ligands is explored using density functional theory combined with time-domain nonadiabatic molecular dynamic simulations.
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