Contact‐Electro‐Catalysis for Direct Oxidation of Methane under Ambient Conditions

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(20)

Published: March 16, 2024

Abstract The conversion of methane under ambient conditions has attracted significant attention. Although advancements have been made using active oxygen species from photo‐ and electro‐ chemical processes, challenges such as complex catalyst design, costly oxidants, unwanted byproducts remain. This study exploits the concept contact‐electro‐catalysis, initiating reactions through charge exchange at a solid–liquid interface, to report novel process for directly converting conditions. Utilizing electrification commercially available Fluorinated Ethylene Propylene (FEP) with water ultrasound, we demonstrate how this interaction promote activation molecules. Our results show that yield HCHO CH 3 OH can reach 467.5 151.2 μmol ⋅ g cat −1 , respectively. We utilized electron paramagnetic resonance (EPR) confirm evolution hydroxyl radicals (⋅OH) superoxide (⋅OOH). Isotope mass spectrometry (MS) was employed analyze elemental origin OH, which be further oxidized HCHO. Additionally, conducted density functional theory (DFT) simulations assess reaction energies FEP H 2 O, O 4 these implications methodology, its potential applicability wider array gas‐phase catalytic reactions, underscore advance in catalysis.

Language: Английский

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Preparation of Heterojunction Catalysts for Photocatalysis byin‐situSynthesis: What We Should Do Next?

ChemCatChem, Journal Year: 2023, Volume and Issue: 16(7)

Published: Nov. 21, 2023

Abstract The construction of heterojunction is one the most effective ways to improve activity photocatalysts, while in‐situ synthesis technology can provide intimate interfacial contact during preparation heterojunction. Heterojunction photocatalysts prepared by have shown excellent performance in solar energy conversion and environmental purification. convenient process also suitable for large‐scale production. In this review, we summarize common methods characterization techniques heterojunctions, list applications these catalysts photocatalytic field. Finally, discuss limitations current research on look forward its great prospects.

Language: Английский

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Pd-loaded unique urchin-structured Ga₂O₃ for selective CO₂ photoreduction to CH₄

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: 12(36), P. 24328 - 24338

Published: Jan. 1, 2024

An innovative urchin-structured Ga 2 O 3 -based photocatalyst with a high specific surface area and highly selective CO photoreduction to CH 4 is designed by constructing dual microemulsion mixed system.

Language: Английский

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Atomically Dispersed Ru Species Induced by Strong Metal–Support Interaction for Electrochemical Methane Reforming

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(46), P. 31825 - 31835

Published: Nov. 8, 2024

During the high-temperature oxygen evolution reaction for CO

Language: Английский

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Optimizing oxygen vacancies through crystal facets engineering to enhance the photooxidation of methane

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 159227 - 159227

Published: Jan. 1, 2025

Language: Английский

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High-Efficiency Photooxidation of Methane to the C1 Product

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 25, 2025

The efficient conversion of methane (CH4) to high-value-added chemicals using a photocatalyst at room temperature and pressure faces great challenges compared harsh reaction conditions. However, achieving this would yield substantial cost advantages hold immense potential for development. Here, we demonstrate the enhanced photocatalytic efficiency CH4 conditions without requiring any oxidant through construction bimetal Ag–Cu-loaded brookite TiO2 photocatalyst. C1 products were ultimately obtained with 100% selectivity 936 μmol·g–1·h–1. performance exceeds that similar research by tens times. high system is attributed optimal number ·OH, which strikes balance between excess deficiency. Ag effectively enhances electron transport in process on dual active site photocatalyst, while Cu significantly improves products. In system, hydroxyl radical (·OH) activates generate methyl (·CH3), then binds lattice oxygen TiO2, breaking Ti–O bond resulting formation *OCH3. *OCH3 undergoes further CH3OH, subsequently oxidized HCHO ·OH. This work presents cost-effective highly approach directly oxidizing into valuable chemicals, ensuring superior selectivity.

Language: Английский

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Integrating photochemical and photothermal effects for selective oxidative coupling of methane into C2+ hydrocarbons with multiple active sites

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

Published: March 22, 2025

The direct photocatalytic oxidation of methane to value-added chemicals has garnered considerable interest in recent years. However, achieving high productivity while maintaining selectivity at an appreciable conversion rate remains a formidable challenge. Here, we present photochemically-triggered and photothermally-enhanced oxidative coupling multi-carbon C2+ alkanes over Au CeO2 nanoparticle-decorated ZnO photocatalyst, which exhibits record-breaking production 17,260 μmol g−1 h−1 with ~90% under wide-spectrum light irradiation without secondary source heating. Comprehensive characterizations computational studies reveal that CH4 activation is photochemical reaction initiated by ultraviolet light-excited ZnO, the introduction substantially enhances O2 due cooperative interaction between CeO2. Concurrently, nanoparticles capture visible near-infrared generate localized heating, greatly promotes subsequent desorption produced methyl radical for C–C prior undergoing further undesired overoxidation. Achieving both activity photooxidation hydrocarbons challenging. This work shows integrating photothermal effects both, enabling efficient alkanes.

Language: Английский

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Ag‐ZnO Nanoflowers Enable Highly Selective Photocatalytic Conversion of CH₄ to CH₃OH at Atmospheric Pressure: Unraveling Reactive Interfaces and Intermediate Control

Small, Journal Year: 2025, Volume and Issue: unknown

Published: March 21, 2025

At atmospheric pressure, the main challenge in photocatalytic oxidation of CH4 to CH3OH is absorb and activate inert C─H bond while preventing excessive CH3OH. In this study, metal-supported ZnO nanoflowers (Ag-ZnO) are designed produce abundant active interfacial oxygen sites for at with a yield reaching 1300 µmol gcat -1 h-1 selectivity 94%. DFT calculation situ analysis show that addition Ag regulates electron state density band center O, which beneficial adsorption CH4, decreases dissociation energy barrier OL(Lattice oxygen) site. The further selective conversion ·CH3 involves two different pathways: one pathway consists by OL, other combination ·OH generated from dissolved O2 (0.28 mm) water. Notably, photochemical flow device, increased 5200 close 100%. This work offers valuable insights into reactive interfaces, morphological engineering, control intermediate evolution toward oxygenates pressure.

Language: Английский

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NiB₂O_4-x Nanospheres for Methane Dry Reforming to Hydrogen-Rich Syngas

ACS Applied Nano Materials, Journal Year: 2025, Volume and Issue: unknown

Published: May 2, 2025

Language: Английский

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Photocatalytic oxidation of methane to C1 oxygenates promoted by Fe−N−Ti electron bridge

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 358, P. 124417 - 124417

Published: July 19, 2024

Language: Английский

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