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

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(46), С. 31825 - 31835

Опубликована: Ноя. 8, 2024

During the high-temperature oxygen evolution reaction for CO

Язык: 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, Год журнала: 2025, Номер 16(1)

Опубликована: Март 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.

Язык: Английский

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

ChemCatChem, Год журнала: 2023, Номер 16(7)

Опубликована: Ноя. 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.

Язык: Английский

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

Angewandte Chemie, Год журнала: 2024, Номер 136(20)

Опубликована: Март 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.

Язык: Английский

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Enhanced Conversion of Methane to Liquid-phase Oxygenates via Hollow Ferrite Nanotube@Horseradish Peroxidase Based Photoenzymatic Catalysis

Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер 361, С. 124593 - 124593

Опубликована: Сен. 10, 2024

Язык: Английский

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

Journal of Materials Chemistry A, Год журнала: 2024, Номер 12(36), С. 24328 - 24338

Опубликована: Янв. 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.

Язык: Английский

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Highly Selective Catalytic Oxidation of Methane to Methanol using Cu-Pd/Anatase

Energy & Environmental Science, Год журнала: 2024, Номер unknown

Опубликована: Янв. 1, 2024

Cu–Pd/anatase is highly efficient in converting methane to methanol, exhibiting a relatively high methanol yield rate of ∼31 800 μmol g cat −1 h and near-exclusive selectivity liquid products (methanol).

Язык: Английский

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

Chemical Engineering Journal, Год журнала: 2025, Номер unknown, С. 159227 - 159227

Опубликована: Янв. 1, 2025

Язык: Английский

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High-Efficiency Photooxidation of Methane to the C1 Product

ACS Applied Materials & Interfaces, Год журнала: 2025, Номер unknown

Опубликована: Фев. 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.

Язык: Английский

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Photothermal direct methane conversion to formaldehyde at the gas-solid interface under ambient pressure

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

Опубликована: Март 15, 2025

Photocatalytic direct oxidation of methane to C1 oxygenates offers a green alternative conventional energy-intensive and high-carbon-footprint multi-step processes. However, current batch-type gas–liquid–solid reaction systems under high-pressure conditions face critical challenges in real-time product separation concentration for industrial implementation. Here, we demonstrate continuous-flow gas–solid photothermal catalytic route conversion formaldehyde ambient pressure, where the generated gas-phase can be easily collected by water absorption. The Ag single-atom modified ZnO photocatalyst achieves production rate 117.8 ± 1.7 μmol h−1 with 71.2 0.8% selectivity. Meanwhile, highly concentrated solution (514.2 33.7 µmol mL−1, 1.54 0.10 wt.%) is obtained through 12-hour absorption, effectively overcoming enrichment barrier that plagues batch route. This study establishes robust technological foundation sustainable industrial-scale value-added chemicals. introduces phase catalysis approach pressure. more scalable conversion.

Язык: Английский

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