Accelerating Fe(III)/Fe(II) redox cycling in heterogeneous electro-Fenton process via S/Cu-mediated electron donor-shuttle regime

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 342, P. 123457 - 123457

Published: Nov. 1, 2023

In this study, we developed a Cu0.5Fe2.5S4 nanocatalyst through facile sulfidation of the Cu-MIL-88B(Fe) precursor to expedite surface Fe(III) reduction and enhance H2O2 activation in heterogeneous electro-Fenton (HEF). The as-prepared catalyst possesses relatively large specific area uniformly dispersed metal active sites. catalyzed HEF system allowed compete removal naproxen with minimal leaching, surpassing that or Fe3S4. Quantitative XPS analysis, electrochemical characterization density functional theory calculations elucidate an electron donor-shuttle regime S2- Cu species serve as donor shuttle, respectively. significantly accelerate internal transfer between S Fe mitigate dissolution adjacent iron sites, securing sustainable reducing capacity. Moreover, Cu0.5Fe2.5S4-based exhibits great practicability for treatment various organics urban wastewater. This study opens new avenue addressing challenge sluggish Fe(III)/Fe(II) cycling HEF.

Language: Английский

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Overlooked Role of Coexistent Hydrogen Peroxide in Activated Peracetic Acid by Cu(II) for Enhanced Oxidation of Organic Contaminants

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: 58(35), P. 15741 - 15754

Published: Feb. 15, 2024

Cu(II)-catalyzed peracetic acid (PAA) processes have shown significant potential to remove contaminants in water treatment. Nevertheless, the role of coexistent H

Language: Английский

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

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(17)

Published: March 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.

Language: Английский

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Surface Redox Chemistry Regulates the Reaction Microenvironment for Efficient Hydrogen Peroxide Generation

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(22), P. 15356 - 15365

Published: May 22, 2024

Electrosynthesis has emerged as an enticing solution for hydrogen peroxide (H2O2) production. However, efficient H2O2 generation encounters challenges related to the robust gas–liquid–solid interface within electrochemical reactors. In this work, we introduce effective hydrophobic coating modified by iron (Fe) sites optimize reaction microenvironment. This modification aims mitigate radical corrosion through Fe(II)/Fe(III) redox chemistry, reinforcing microenvironment at three-phase interface. Consequently, achieved a remarkable yield of up 336.1 mmol h–1 with sustained catalyst operation extensive duration 230 h 200 mA cm–2 without causing damage Additionally, Faradaic efficiency exceeded 90% across broad range test current densities. surface chemistry approach manipulating not only advances long-term electrosynthesis but also holds promise other gas-starvation reactions.

Language: Английский

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Novel photoelectrocatalytic system of oxygen vacancy-rich black TiO2-x nanocones photoanode and natural air diffusion cathode for efficient water purification and simultaneous H2O2 production

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 352, P. 124042 - 124042

Published: April 21, 2024

Language: Английский

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High-Valence Cu Induced by Photoelectric Reconstruction for Dynamically Stable Oxygen Evolution Sites

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(28), P. 19295 - 19302

Published: June 29, 2024

Oxygen vacancies are generally considered to play a crucial role in the oxygen evolution reaction (OER). However, generation of active sites created by is inevitably restricted their condensation and elimination reactions. To overcome this limitation, here, we demonstrate novel photoelectric reconstruction strategy incorporate atomically dispersed Cu into ultrathin (about 2-3 molecular) amorphous oxyhydroxide (a-CuM, M = Co, Ni, Fe, or Zn), facilitating deprotonation reconstructed generate high-valence Cu. The situ XAFS results first-principles calculations reveal that atoms stabilized at high valence during OER process due Jahn-Teller distortion, resulting para-type double as dynamically stable catalytic sites. optimal a-CuCo catalyst exhibits record-high mass activity 3404.7 A g

Language: Английский

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Enhanced oxidation of organic pollutants by regulating the interior reaction region of reactive electrochemical membranes

Journal of Hazardous Materials, Journal Year: 2024, Volume and Issue: 466, P. 133584 - 133584

Published: Jan. 22, 2024

Language: Английский

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Amorphous CoSx in heterogeneous electro-Fenton: A 1O2-mediated system for efficient and selective water decontamination

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 359, P. 124501 - 124501

Published: Aug. 13, 2024

Language: Английский

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Combined coagulation-adsorption-VUV (persulfate)-electrochemical oxidation processes for efficient treatment of aged landfill leachate

Journal of Water Process Engineering, Journal Year: 2025, Volume and Issue: 71, P. 107281 - 107281

Published: Feb. 20, 2025

Language: Английский

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Hydrophobic Trinuclear Copper Cluster‐Containing Organic Framework for Synergetic Electrocatalytic Synthesis of Amino Acids

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(5)

Published: Dec. 5, 2023

Abstract Electrocatalytic synthesis of amino acids provides a promising green and efficient pathway to manufacture the basic substances life. Herein, reaction 2,5‐perfluroalkyl‐terepthalohydrazide tris(4‐µ 2 ‐O‐carboxaldehyde‐pyrazolato‐N, N′)‐tricopper affords crystalline trinuclear copper cluster‐containing organic framework, named F‐Cu 3 ‐OF. Incorporation abundant hydrophobic perfluroalkyl groups inside channels ‐OF is revealed successfully suppress hydrogen evolution via preventing H + cation with large polarity from framework in turn increasing adsorption other substrates relatively small like NO − keto on active sites. The atoms short distance clusters enable simultaneous activization acids, facilitating following synergistic C─N coupling basis situ spectroscopic investigations together theoretical calculation. Combination these effects leads electroproduction various including glycine, alanine, leucine, valine, phenylalanine Faraday efficiency 42%–71% yield 187–957 µmol cm −2 h −1 , representing thus far best performance. This work shall be helpful for developing economical, eco‐friendly, high‐efficiency strategy production life substances.

Language: Английский

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