Selective Photocatalytic Oxidation of Methane to Methanol by Constructing a Rapid O₂ Conversion Pathway over Au–Pd/ZnO

ACS Catalysis, Год журнала: 2024, Номер 14(2), С. 955 - 964

Опубликована: Янв. 5, 2024

Photocatalytic oxidation of methane to methanol is an attractive process under mild conditions, nevertheless confronting significant challenges in achieving high conversion and selectivity simultaneously. Herein, we propose a strategy for the direct rapid generation hydroxyl radicals (•OH) from O2 (O2 → *OOH •OH) by rational design Au–Pd/ZnO photocatalyst, skipping water-soluble H2O2 avoiding diffusion. For photocatalytic at ambient temperature, yield CH3OH over optimized 1.0% AuPd0.5/ZnO catalyst were as 81.0 μmol·h–1 88.2%, respectively, exceeding that most reported systems. The formation Au–Pd alloys could improve adsorption cleavage O–O bond *OOH, facilitating efficient •OH increasing selectivity. This work provides some guidance delicate composite photocatalysts selective utilization.

Язык: Английский

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Single‐Atom Alloys Materials for CO₂ and CH₄ Catalytic Conversion

Advanced Materials, Год журнала: 2024, Номер 36(16)

Опубликована: Янв. 5, 2024

The catalytic conversion of greenhouse gases CH

Язык: Английский

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Bimetallic Single Atom/Nanoparticle Ensemble for Efficient Photochemical Cascade Synthesis of Ethylene from Methane

Angewandte Chemie, Год журнала: 2024, Номер 136(34)

Опубликована: Июнь 11, 2024

Abstract Light‐driven photoredox catalysis presents a promising approach for the activation and conversion of methane (CH 4 ) into high value‐added chemicals under ambient conditions. However, C−H bond dissociation energy CH absence well‐defined sites on catalysts significantly limit highly efficient toward multicarbon (C 2+ hydrocarbons, particularly ethylene 2 H ). Herein, we demonstrate bimetallic design Ag nanoparticles (NPs) Pd single atoms (SAs) ZnO cascade C with highest production rate compared previous works. Mechanistic studies reveal that synergistic effect NPs SAs, upon effecting key bond‐breaking ‐forming events, lowers overall barrier process both resulting 6 , constituting truly catalytic system to facilitate generation. This work offers novel perspective advancement photocatalytic directional hydrocarbons through subtle catalyst strategy.

Язык: Английский

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Optimizing the reaction pathway of methane photo-oxidation over single copper sites

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

Опубликована: Окт. 21, 2024

Язык: Английский

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Bimetallic Single Atom/Nanoparticle Ensemble for Efficient Photochemical Cascade Synthesis of Ethylene from Methane

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(34)

Опубликована: Июнь 11, 2024

Abstract Light‐driven photoredox catalysis presents a promising approach for the activation and conversion of methane (CH 4 ) into high value‐added chemicals under ambient conditions. However, C−H bond dissociation energy CH absence well‐defined sites on catalysts significantly limit highly efficient toward multicarbon (C 2+ hydrocarbons, particularly ethylene 2 H ). Herein, we demonstrate bimetallic design Ag nanoparticles (NPs) Pd single atoms (SAs) ZnO cascade C with highest production rate compared previous works. Mechanistic studies reveal that synergistic effect NPs SAs, upon effecting key bond‐breaking ‐forming events, lowers overall barrier process both resulting 6 , constituting truly catalytic system to facilitate generation. This work offers novel perspective advancement photocatalytic directional hydrocarbons through subtle catalyst strategy.

Язык: Английский

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Interstitial Zinc Defects Enriched ZnO Tuning O₂ Adsorption and Conversion Pathway for Superior Photocatalytic CH₄ Oxygenation

ACS Catalysis, Год журнала: 2024, Номер 14(12), С. 9104 - 9114

Опубликована: Май 30, 2024

Photocatalytic methane conversion into liquid oxygenates using O2 oxidants provides a promising approach for high-value chemicals. The generation of reactive oxygen species and their reaction pathway are key to determine the oxygenate selectivity. Here, an interstitial Zni defect ZnO (ZnO(Zni)) is developed through thermal decomposition ZnO2 precursor. favors adsorption at terminal configuration induces effectively desired •OOH instead •OH improving yield selectivity oxygenates. For comparison, adsorbed in lateral tends be converted excessive on typical Au/ZnO. As result, ZnO(Zni) shows 6080 μmol g–1 with 98.6% selectivity, which leads 10 times lower than Au/ZnO CO2 release overoxidation. This work activation regulate photocatalytic CH4 oxidation

Язык: Английский

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Outlook of Cobalt-Based Catalysts for Heterogeneous Hydroformylation of Olefins: From Nanostructures to Single Atoms

Energy & Fuels, Год журнала: 2023, Номер 38(4), С. 2526 - 2547

Опубликована: Окт. 19, 2023

Hydroformylation of olefins, as a study olefinic downstream derivative production, is great relevance in chemical production. Heterogeneous hydroformylation beneficial for catalyst separation and recycling compared to homogeneous systems. Cobalt cheap metal with excellent catalytic activity well the precious rhodium. Therefore, research on cobalt-based catalysts heterogeneous has value significance. The nano or atomic structures have significant impact behaviors process. There rarely design principles report how achieve improvement performance by regulating structure catalyst. Herein, we review recent progress different sizes (from nanostructures single atoms). On basis difference mechanism between hydroformylation, summarize propose regulation enhance stability where single-atom engineering expected unity high applications. At end this review, present an outlook opportunities challenges developing hydroformylation.

Язык: Английский

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Selective photocatalytic oxidative coupling of methane via directional activation of oxygen over Au-loaded ZnSn-LDH with defect structure

Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер unknown, С. 124670 - 124670

Опубликована: Окт. 1, 2024

Язык: Английский

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Polydopamine‐Mediated Contact‐Electro‐Catalysis for Efficient Partial Oxidation of Methane

Angewandte Chemie International Edition, Год журнала: 2024, Номер 64(1)

Опубликована: Окт. 17, 2024

The direct conversion and efficient utilization of methane pose a critical scientific challenge. Indirect activation via reactive oxygen species (ROS) offers high probability contact with efficiency under mild conditions. However, reported product yields are suboptimal due to challenges in activating facilitating mass transfer suspension systems. We propose the use contact-electro-catalysis (CEC), employing polydopamine (PDA) as catalyst that undergoes electron ultrasound, generating ROS drives partial oxidation (POM). Corresponding experimental results indicate CH

Язык: Английский

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Light-driven C1 Chemical Conversion with LDH-based Nanomaterials

Applied Clay Science, Год журнала: 2024, Номер 258, С. 107488 - 107488

Опубликована: Июль 14, 2024

Язык: Английский

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