Operando identification of the oxide path mechanism with different dual-active sites for acidic water oxidation

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Sept. 16, 2024

The microscopic reaction pathway plays a crucial role in determining the electrochemical performance. However, artificially manipulating still faces considerable challenges. In this study, we focus on classical acidic water oxidation based RuO

Language: Английский

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A polymerization-mediated confinement strategy to fabricate Fenton-like catalysts with high H2O2 utilization for water decontamination

Journal of environmental chemical engineering, Journal Year: 2025, Volume and Issue: 13(1), P. 115325 - 115325

Published: Jan. 5, 2025

Language: Английский

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Boosting Fe3+/Fe2+ cycling under visible-light-driven TiO2-based membrane with electron-deficient center for wastewater decontamination

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125070 - 125070

Published: Jan. 1, 2025

Language: Английский

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

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

Published: Jan. 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.

Language: Английский

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Selective Liquid Chemical Production in Waste Polyolefin Photorefinery by Controlling Reactive Species

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 29, 2025

Photocatalytic upcycling of waste polyolefins into value-added chemicals provides promise in plastic management and resource utilization. Previous works demonstrate that can be converted carboxylic acids, with CO2 as the final oxidation product. It is still challenging to explore more transformation products, particularly mild-oxidation products such alcohols, because their instability compared polymer substrates, which are prone during catalytic reactions. In this work, we propose an efficient strategy regulate product type through precise control radicals, intermediates, reaction paths. Taking commonly used photocatalyst C3N4 example, its major acids CO2. When MoS2 introduced construct a Z-scheme heterostructure, gas significantly reduced alcohols appear high yield 1358.8 μmol gcat-1 selectivity up 80.3%. This primarily attributed presence •OH radicals from oxygen reduction, acting key role alcohol formation while simultaneously suppressing competing pathways •O2- 1O2, thus reducing overoxidation products. The β-scission C-C bonds chains generates intermediate alkyl species, followed by combination produce methanol, energetically favorable for MoS2/C3N4. contrast, species couple form formic acid, C3N4. work new approaches controlling types offers insights involved polyolefin photorefinery.

Language: Английский

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Data‐Driven Accelerated Discovery Coupled with Precise Synthesis of Single‐Atom Catalysts for Robust and Efficient Water Purification

Angewandte Chemie International Edition, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 31, 2025

Abstract The development of advanced catalysts frequently employs trial‐and‐error methods and is lack highly controlled synthesis, resulting in unsatisfactory efficiency performance. Here we propose a data‐driven prediction coupled with precise synthesis strategy to accelerate the single‐atom (SACs) for efficient water purification. approach enables rapid screening high‐performance SACs from 43 metals‐N 4 structures comprising transition main group metal elements, followed by validation structural modulation improved performance through controllable hard‐template method. Impressively, well‐designed Fe‐SAC high loading Fe‐pyridine‐N sites (~3.83 wt %) mesoporous structure, exhibits ultra‐high decontamination (rate constant 100.97 min −1 g −2 ), representing best Fenton‐like activities sulfonamide antibiotics date. Furthermore, optimized shows excellent robust environmental resistance cyclic stability almost 100 % degradation 100‐h continuous operation. Density functional theory calculations reveal that can reduce energy barrier intermediate O* formation, rate‐determining step, selective generation singlet oxygen. integration method provides novel paradigm field as well other important fields including sustainable catalysis.

Language: Английский

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Confinement Improves Mass Transfer and Chemical Reactivity in Electrified Membranes for Micropollutant Degradation

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

Published: Feb. 14, 2025

Abstract Micropollutants (MPs) pose a significant threat to global water environments, necessitating advanced treatment technologies. Distributed electrochemical systems utilizing electrified membranes (EMs) show promise but face challenges due unclear mass transfer and reaction mechanisms within membrane pores of varying sizes surface chemistry. This review examines the interplay between spatial confinement, transfer, chemical reactions in EMs, focusing on reactive species (RSs), EM‐MPs system evolution, phenomena across pore from microns sub‐nanometer scales. Despite advances RS research, coherent mechanistic understanding MP degradation under confinement remains elusive, particularly extreme where deviate bulk behavior. Gaps knowledge stem complex dynamics, thermodynamics kinetics, need for detailed theoretical describe effects. summarizes generation detection methods RSs, outlines progress EM operational modes, elucidates how impacts both reactions. Future research shall focus precise identification quantitative regulation optimization processes relation RSs MPs, investigation active sites energetic barriers confined environments.

Language: Английский

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Selective activation of peroxymonosulfate through gating heteronuclear diatomic distance for flexible generation of high-valent cobalt-oxo species or sulfate radicals

Water Research, Journal Year: 2025, Volume and Issue: unknown, P. 123488 - 123488

Published: March 1, 2025

Language: Английский

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Interfacial electronic structure engineering on nano-confined cobalt nanoparticles to enhance Fenton-like reaction

Journal of Hazardous Materials, Journal Year: 2025, Volume and Issue: unknown, P. 137930 - 137930

Published: March 1, 2025

Language: Английский

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Nanoconfined catalytic macrostructures for advanced water remediation: From basic understanding to future application strategies

Water Research, Journal Year: 2024, Volume and Issue: 272, P. 122960 - 122960

Published: Dec. 11, 2024

Language: Английский

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