Long-range interactions driving neighboring Fe–N4 sites in Fenton-like reactions for sustainable water decontamination

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Сен. 5, 2024

Язык: Английский

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Deciphering Structure‐Activity Relationship Towards CO₂ Electroreduction over SnO₂ by A Standard Research Paradigm

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(12)

Опубликована: Янв. 29, 2024

Abstract Authentic surface structures under reaction conditions determine the activity and selectivity of electrocatalysts, therefore, knowledge structure‐activity relationship can facilitate design efficient catalyst for specific reactivity requirements. However, understanding between a more realistic active its performance is challenging due to complicated interface microenvironment in electrocatalysis. Herein, we proposed standard research paradigm effectively decipher electrocatalysis, which exemplified CO 2 electroreduction over SnO . The practice has aided discovering authentic/resting states (Sn layer) accountable electrochemical reduction (CO RR) electrocatalytic conditions, then corroborated subsequent RR experiments with different morphologies (nanorods, nanoparticles, nanosheets) combination situ characterizations. This methodology further extended providing helpful insights into catalytic structures. It believed that our also applicable other systems, meantime, decreases discrepancy theory experiments, accelerates achieve sustainable energy conversion.

Язык: Английский

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Non-metallic iodine single-atom catalysts with optimized electronic structures for efficient Fenton-like reactions

Nature Communications, Год журнала: 2025, Номер 16(1)

Опубликована: Янв. 18, 2025

In this study, we introduce a highly effective non-metallic iodine single-atom catalyst (SAC), referred to as I-NC, which is strategically confined within nitrogen-doped carbon (NC) scaffold. This configuration features distinctive C-I coordination that optimizes the electronic structure of nitrogen-adjacent sites. As result, arrangement enhances electron transfer from peroxymonosulfate (PMS) active sites, particularly electron-deficient carbon. followed by deprotonation process generates radical (SO5•-). Subsequently, SO5•- undergoes disproportionation reaction, leading production singlet oxygen (1O2). Furthermore, energy barrier for rate-limiting step generation in I-NC significantly lower at 1.45 eV, compared 1.65 eV NC reduction effectively overcomes kinetic obstacles, thereby facilitating an enhanced 1O2. Consequently, exhibits remarkable catalytic efficiency and unmatched reactivity PMS activation. leads accelerated degradation pollutants, evidenced relatively high observed rate constant (kobs ~ 0.436 min-1) other metallic SACs. study offers valuable insights into rational design SACs, showcasing their promising potential Fenton-like reactions water treatment applications.

Язык: Английский

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Atomically Dispersed Fe‐Mo Catalysts Mediate Fenton‐Like Reaction to Efficiently Degrade Chlorophenol Pollutants Through Synergistic Oxidation and Dechlorination Reactions

Small, Год журнала: 2025, Номер unknown

Опубликована: Янв. 15, 2025

Chlorophenols are difficult to degrade and mineralize by traditional advanced oxidation processes due the strong electronegativity of chlorine. Here, a dual-site atomically dispersed catalyst (FeMoNC) is reported, which Fe/Mo supported on mesoporous nitrogen-doped carbon prepared through high-temperature migration. The FeMoNC exhibits high dechlorination rate 93.3% within 1 min. Theoretical calculation suggested that doping high-valence Mo6+ as electron reservoir, promoted electronic delocalization at Fe sites, thereby enhancing adsorption dissociation peroxymonosulfate (PMS), subsequent generation (IV) = O singlet oxygen (1O2) species. An interesting finding Mo sites can adsorb chlorine in 4-chlorophenol (4-CP) induce C─Cl bond fracture. Thus, FeMoNC/PMS system has catalytic performance synergistic effects Mo-induced non-radical species (Fe(IV) 1O2) degradation pathways, efficiency 99.1% 4-CP 5 min without significant decline after 168 h ≈15,120-bed volumes. These findings advance mechanistic understanding PMS activation molecular level guide rational design efficient eco-friendly single-atom catalysts (SACs) with bimetallic atomic sites.

Язык: Английский

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Innovative asymmetric CoSA‐N‐Ti3C2Tx catalysis: unleashing superoxide radicals for rapid self‐coupling removal of phenolic pollutant

Angewandte Chemie International Edition, Год журнала: 2025, Номер unknown

Опубликована: Фев. 3, 2025

The polymerization pathway of contaminants rivals the traditional mineralization in water purification technologies. However, designing suitable oxidative environments to steer toward remains challenging. This study introduces a nitrogen-oxygen double coordination strategy create an asymmetrical microenvironment for Co atoms on Ti3C2Tx MXenes, resulting novel Co-N2O3 microcellular structure that efficiently activates peroxymonosulfate. unique activation capability led complete removal various phenolic pollutants within 3 min, outperforming representative single-atom catalysts reported past three years. Identifying and recognizing reactive oxygen species highlight crucial role ⋅O2 -. efficient pollutant occurs through --mediated radical pathway, functioning as self-coupling reaction rather than deep oxidation. Theoretical calculations demonstrate electron-rich transfer more electrons catalyst surface, inducing reduction dissolved - microregion. In practical continuous flow-through application, system achieved 100 % acetaminophen efficiency 6.5 h, with hydraulic retention time just 0.98 s. provides new insights into previously underappreciated purification, offering simple advancing aggregation technology field wastewater treatment.

Язык: Английский

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Controllable Supply–Demand Effect during Superior Fe Single-Atom Catalyst Synthesis for Targeted Guanine Oxidation of Antibiotic Resistance Genes

Environmental Science & Technology, Год журнала: 2025, Номер unknown

Опубликована: Март 6, 2025

Nonradical Fenton-like catalysis offers an opportunity to degrade extracellular antibiotic resistance genes (eARGs). However, high-loading single-atom catalysts (SACs) with controllable configurations are urgently required selectively generate high-yield nonradicals. Herein, we constructed Fe SACs (5.4-34.2 wt %) uniform Fe-N4 sites via optimized coordination balance of supermolecular assembly for peroxymonosulfate activation. The selectivity singlet oxygen (1O2) generation and its contribution eARGs degradation were both >98%. This targeting strategy oxidizing guanines low ionization potentials by 1O2 allowed 7 log within 10 min eliminated their transformation 2 min, outperforming most reported advanced oxidation processes. Relevant interactions between revealed at a single-molecule resolution. exhibited excellent universality stability different water matrices. These findings provide promising route constructing efficient selective treatment.

Язык: Английский

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Two-dimensional MBene combined with cobalt nanoparticles enabling highly efficient peroxymonosulfate activation for ornidazole degradation

Separation and Purification Technology, Год журнала: 2024, Номер 354, С. 128647 - 128647

Опубликована: Июль 2, 2024

Язык: Английский

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Peracetic acid-induced nanoengineering of Fe-based metallic glass ribbon in application of efficient drinking water treatment

Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер 355, С. 124161 - 124161

Опубликована: Май 9, 2024

Язык: Английский

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Tailoring the selective generation of high-valent cobalt-oxo by asymmetrically coordinated single-atom cobalt-activated peracetic acid for efficient water decontamination

Chemical Engineering Journal, Год журнала: 2024, Номер unknown, С. 156042 - 156042

Опубликована: Сен. 1, 2024

Язык: Английский

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Single-Atom Iron Can Steer Atomic Hydrogen toward Selective Reductive Dechlorination: Implications for Remediation of Chlorinated Solvents-Impacted Groundwater

Environmental Science & Technology, Год журнала: 2024, Номер 58(26), С. 11833 - 11842

Опубликована: Июнь 24, 2024

Atomic hydrogen (H*) is a powerful and versatile reductant has tremendous potential in the degradation of oxidized pollutants (e.g., chlorinated solvents). However, its application for groundwater remediation hindered by scavenging side reaction H

Язык: Английский

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