Crystallinity engineering for overcoming the activity–stability tradeoff of spinel oxide in Fenton-like catalysis

Proceedings of the National Academy of Sciences, Год журнала: 2023, Номер 120(15)

Опубликована: Апрель 5, 2023

A precise modulation of heterogeneous catalysts in structural and surface properties promises the development more sustainable advanced oxidation water purification technologies. However, while with superior decontamination activity selectivity are already achievable, maintaining a long-term service life such materials remains challenging. Here, we propose crystallinity engineering strategy to break activity-stability tradeoff metal oxides Fenton-like catalysis. The amorphous/crystalline cobalt-manganese spinel oxide (A/C-CoMnOx) provided highly active, hydroxyl group-rich surface, moderate peroxymonosulfate (PMS)-binding affinity charge transfer energy strong pollutant adsorption, trigger concerted radical nonradical reactions for efficient mineralization, thereby alleviating catalyst passivation by intermediate accumulation. Meanwhile, surface-confined reactions, benefited from enhanced adsorption pollutants at A/C interface, rendered A/C-CoMnOx/PMS system ultrahigh PMS utilization efficiency (82.2%) unprecedented (rate constant 1.48 min-1) surpassing almost all state-of-the-art catalysts. cyclic stability environmental robustness real treatment was also demonstrated. Our work unveils critical role material modulating catalytic pathways oxides, which fundamentally improves our understanding structure-activity-selectivity relationships may inspire design application beyond.

Язык: Английский

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An anti-electrowetting carbon film electrode with self-sustained aeration for industrial H₂O₂ electrosynthesis

Energy & Environmental Science, Год журнала: 2023, Номер 17(2), С. 655 - 667

Опубликована: Ноя. 28, 2023

A novel concept of an anti-electrowetting carbon film electrode with self-sustained aeration was devised and demonstrated to develop next-generation cheap scalable metal-free electrodes for industry-scale H 2 O electrosynthesis.

Язык: Английский

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Efficient Homolytic Cleavage of H₂O₂ on Hydroxyl‐Enriched Spinel CuFe₂O₄ with Dual Lewis Acid Sites

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(17)

Опубликована: Март 1, 2024

Abstract Traditional H 2 O cleavage mediated by macroscopic electron transfer (MET) not only has low utilization of , but also sacrifices the stability catalysts. We present a non‐redox hydroxyl‐enriched spinel (CuFe 4 ) catalyst with dual Lewis acid sites to realize homolytic . The results systematic experiments, in situ characterizations, and theoretical calculations confirm that tetrahedral Cu optimal acidity strong delocalization can synergistically elongate O−O bonds (1.47 Å → 1.87 Å) collaboration adjacent bridging hydroxyl (another site). As result, free energy is decreased (1.28 eV 0.98 eV). be efficiently split into ⋅OH induced CuFe without MET, which greatly improves (65.2 %, nearly times than traditional catalysts). system assembled affords exceptional performance for organic pollutant elimination. scale‐up experiment using continuous flow reactor realizes long‐term (up 600 mL), confirming tremendous potential practical applications.

Язык: Английский

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Electronic structure modulation of iron sites with fluorine coordination enables ultra-effective H2O2 activation

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

Опубликована: Март 12, 2024

Abstract Electronic structure modulation of active sites is critical important in Fenton catalysis as it offers a promising strategy for boosting H 2 O activation. However, efficient generation hydroxyl radicals (•OH) often limited to the unoptimized coordination environment sites. Herein, we report rational design and synthesis iron oxyfluoride (FeOF), whose strongly coordinate with most electronegative fluorine atoms characteristic moiety F-(Fe(III)O 3 )-F, effective activation potent •OH generation. Results demonstrate that plays pivotal role lowering local electron density optimizing electronic structures sites, thus facilitating rate-limiting adsorption subsequent peroxyl bond cleavage reactions. Consequently, FeOF exhibits significant pH-adaptive yield (~450 µM) high selectivity, which 1 ~ orders magnitude higher than state-of-the-art iron-based catalysts, leading excellent degradation activities against various organic pollutants at neutral condition. This work provides fundamental insights into function atomic level, may inspire sustainable environmental remediation.

Язык: Английский

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Gambling of homogeneous and heterogeneous Fenton in wastewater treatment

Cell Reports Physical Science, Год журнала: 2024, Номер 5(5), С. 101966 - 101966

Опубликована: Май 1, 2024

Employing Fenton technology for efficiently removing pollutants in water stands as a significant method. Within the domain of traditional techniques, there exist both homogeneous and heterogeneous systems. Homogeneous systems tackle iron sludge concerns through incorporation co-catalysts, whereas adeptly manipulate surface microenvironments adjust active sites, enabling pollutant degradation across wide range pH. Each system boasts distinct advantages limitations. This perspective critically examines existing challenges associated solutions reactions comprehensive analysis typical case studies. The focus is on evaluating industrial potential these systems, forecasting future developmental trends, fostering more robust sustainable advancement within context carbon peaking neutrality goals.

Язык: Английский

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Advances in heterogeneous electro-Fenton processes for water treatment: A comprehensive review

Separation and Purification Technology, Год журнала: 2025, Номер unknown, С. 131470 - 131470

Опубликована: Янв. 1, 2025

Язык: Английский

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Flow-through electro-Fenton using nanoconfined Fe-Mn bimetallic oxides: Ionization potential-dependent micropollutants degradation mechanism

Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 328, С. 122538 - 122538

Опубликована: Фев. 26, 2023

Язык: Английский

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A sustainable solution for organic pollutant degradation: Novel polyethersulfone/carbon cloth/FeOCl composite membranes with electric field-assisted persulfate activation

Water Research, Год журнала: 2023, Номер 244, С. 120530 - 120530

Опубликована: Авг. 26, 2023

Язык: Английский

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Electrochemical‐Mediated Regenerable Fe^II Active Sites for Efficient Uranium Extraction at Ultra‐Low Cell Voltage

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(21)

Опубликована: Март 11, 2023

Abstract Nano‐reduced iron (NRI) is a promising uranium adsorbent due to its strong reducibility and good selectivity, but it still faces the challenges of slow kinetics, limited non‐renewable active sites. In this work, we realized high efficiency extraction under ultra‐low cell voltage (−0.1 V) in seawater with 20 ppm UO 2 (NO 3 ) solution by coupling electrochemical mediated Fe II /Fe III redox extraction. The adsorption capacity NRI after (EUE) could reach 452 mg/g 99.1 %, respectively. Combined quasi‐operando/operando characterization technologies, clarified mechanism EUE revealed that continuously regenerating sites electroreduction significantly enhance property EUE. This work here provides new low energy consumption strategy which also reference for other metal resource recovery.

Язык: Английский

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Highly selective electrosynthesis of H2O2 by N, O co-doped graphite nanosheets for efficient electro-Fenton degradation of p-nitrophenol

Journal of Hazardous Materials, Год журнала: 2023, Номер 446, С. 130733 - 130733

Опубликована: Янв. 9, 2023

Язык: Английский

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