Angstrom Confinement‐Triggered Adaptive Spin State Transition of CoMn Dual Single Atoms for Efficient Singlet Oxygen Generation

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 3, 2025

Abstract To achieve high selectivity in the transformation from peroxymonosulfate to singlet oxygen, adaptive tuning of atomic spin state as structure varied is crucial. The angstrom confinement can effectively tune state, but developing an angstrom‐confined system challenging. Angstrom‐confined cobalt (Co) manganese (Mn) dual single atoms within flexible 2D carbon nitride interlayer are constructed drive by changing coordination under confinement. situ characterizations and density functional theory calculations showed that medium‐spin Co Co─N 4 absorbed electrons after adsorption on CoMn single‐atom sites then cleaved O─H facilitate * SO 5 generation, while introduction increased distance Mn─N, resulting transition medium high. Subsequently, high‐spin Mn 2 Mn─N desorbed O , restoring initial state. enhanced 38.6‐fold oxygen yield compared unconfined control. proposed diatomic strategy applicable serial catalysts, providing efficient universal design scheme for oxygen‐mediated selective wastewater treatment technology at level.

Language: Английский

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Efficient degradation of bisphenol A by a novel ternary synergistic dielectric barrier discharge plasma advanced oxidation process: The role of peracetic acid and ferrous ions

Separation and Purification Technology, Journal Year: 2024, Volume and Issue: 354, P. 129568 - 129568

Published: Sept. 6, 2024

Language: Английский

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Picolinic acid-mediated Mn(II) activated periodate for ultrafast and selective degradation of emerging contaminants: Key role of high-valent Mn-oxo species

Water Research, Journal Year: 2024, Volume and Issue: 266, P. 122428 - 122428

Published: Sept. 10, 2024

Language: Английский

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Mechanochemically synthesized peroxymonosulfate activators from spent zinc-manganese battery electrode material: correlation between pollutant electrophilicity index and electron transfer process

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125054 - 125054

Published: Jan. 1, 2025

Language: Английский

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Catalytic wastewater dephosphorization for phosphorus recycling to fertilizers

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125154 - 125154

Published: Feb. 1, 2025

Language: Английский

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Surface-hydroxylated single-atom catalyst with an isolated Co-O-Zn configuration achieves high selectivity in regulating active species

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: March 11, 2025

Single-atom catalysts (SACs) are emerging as potent tools for the selective regulation of active species, offering substantial promise green and sustainable Fenton catalysis. However, current SACs face limitations due to specificity their supports, which only allow within certain oxidant systems. This constraint makes targeted across different systems challenging. In response, this study designs a SAC, termed CoSAs-ZnO, featuring surface hydroxylation an isolated asymmetric Co-O-Zn configuration. SAC can realize nearly 100% generation sulfate radicals (SO4•−) singlet oxygen (1O2) in peroxymonosulfate (PMS) peracetic acid (PAA) systems, respectively. Moreover, PMS-activated system efficiently treat electron-deficient-dominated refractory benzoic wastewater, achieving 100.0% removal multiple consecutive pilot-scale experiments. The PAA-activated facilitates rapid conversion benzyl alcohol benzaldehyde, with high selectivity 89.0%. Detailed DFT calculations reveal that hydroxyl groups on ZnO play critical role modulating adsorption configurations oxidants, thus enabling specific species each system. provides insights into design multifunctional applications paves way deployment wastewater treatment high-value chemical conversion. supports. Here, authors synthesised selectively generate

Language: Английский

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Activation of peracetic acid by electrodes using biogenic electrons: A novel energy- and catalyst-free process to eliminate pharmaceuticals

Water Research, Journal Year: 2024, Volume and Issue: 261, P. 122065 - 122065

Published: July 9, 2024

Peracetic acid (PAA) has received increasing attention as an alternative oxidant for wastewater treatment. However, existing processes PAA activation to generate reactive species typically require external energy input (e.g., electrically and UV-mediated activation) or catalysts Co2+), inevitably treatment costs introducing potential new contaminants that necessitate additional removal. In this work, we developed a catalyst-free, self-sustaining bioelectrochemical approach within two-chamber system (BES), where cathode electrode in-situ activates using renewable biogenic electrons generated by anodic exoelectrogens Geobacter) degrading biodegradable organic matter acetic acid) in at the anode. This innovative BES-PAA technique achieved 98 % 81 removal of 2 µM sulfamethoxazole (SMX) two hours pH (cation exchange membrane) 6 (bipolar 100 μM without voltage. Mechanistic studies, including radical quenching, molecular probe validation, electron spin resonance (ESR) experiments, density functional theory (DFT) calculations, revealed SMX degradation was driven via electron-mediated OO cleavage PAA, with CH3C(O)OO• contributing 68.1 %, •OH 18.4 CH3C(O)O• 9.4 initial formation rapidly reacts produce CH3C(O)OO•. The presence common water constituents such anions Cl−, NO3−, H2PO4−) humic (HA) significantly hinders technique, whereas CO32− HCO3− ions have comparatively minor impact. Additionally, study investigated various pharmaceuticals present secondary treated municipal wastewater, attributing differences efficiency selective action research demonstrates novel method is ecologically benign, inexpensive, capable overcoming catalyst deactivation pollution issues.

Language: Английский

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Overlooked role of boron precursors in tuning engineered zero-valent iron to activate peracetic acid for sustainable micropollutant oxidation

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 361, P. 124580 - 124580

Published: Sept. 8, 2024

Language: Английский

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Unusually improved peracetic acid activation for ultrafast organic compound removal through redox-inert Mg incorporation into active Co3O4

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: unknown, P. 124601 - 124601

Published: Sept. 1, 2024

Language: Английский

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Interfacial catalysis of peroxides for water decontamination: A critical review on fundamental origins and selective oxidation

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 488, P. 151156 - 151156

Published: April 10, 2024

Language: Английский

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