Photocatalytic Conversion of Methane: Current State of the Art, Challenges, and Future Perspectives

ACS Environmental Au, Год журнала: 2023, Номер 3(5), С. 252 - 276

Опубликована: Июнь 20, 2023

With 28-34 times the greenhouse effect of CO

Язык: Английский

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Selective Cleavage of Chemical Bonds in Targeted Intermediates for Highly Selective Photooxidation of Methane to Methanol

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(15), С. 8609 - 8620

Опубликована: Апрель 6, 2023

Restrained by the uncontrollable cleavage process of chemical bonds in methane molecules and corresponding formed intermediates, target product reaction selective oxidation to methanol would suffer from an inevitable overoxidation process, which is considered be one most challenging issues field catalysis. Herein, we report a conceptually different method for modulating conversion pathway through key intermediates suppress generation peroxidation products. Taking metal oxides, typical semiconductors as model catalysts, confirm that CH3O* could greatly affect methane, has vital role selectivity. Specifically, it revealed formation products significantly prevented C-O instead metal-O bonds, proved combination density functional theory calculations situ infrared spectroscopy based on isotope labeling. By manipulating lattice oxygen mobility electrons transferring surface directionally inject into antibonding orbitals bond, resulting its cleavage. As result, gallium oxide with low shows 3.8% rate high (∼325.4 μmol g-1 h-1) selectivity (∼87.0%) under room temperature atmospheric pressure absence extra oxidants, superior among reported studies (reaction pressure: <20 bar).

Язык: Английский

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Synergy of Ag and AgBr in a Pressurized Flow Reactor for Selective Photocatalytic Oxidative Coupling of Methane

ACS Catalysis, Год журнала: 2023, Номер 13(6), С. 3768 - 3774

Опубликована: Март 2, 2023

Oxidation of methane into valuable chemicals, such as C2+ molecules, has been long sought after but the dilemma between high yield and selectivity desired products remains. Herein, is upgraded through photocatalytic oxidative coupling (OCM) over a ternary Ag–AgBr/TiO2 catalyst in pressurized flow reactor. The ethane 35.4 μmol/h with 79% obtained under 6 bar pressure. These are much better than most previous benchmark performance OCM processes. results attributed to synergy Ag AgBr, where serves an electron acceptor promotes charge transfer AgBr forms heterostructure TiO2 not only facilitate separation also avoid overoxidation process. This work thus demonstrates efficient strategy for conversion by both rational design reactor engineering conversion.

Язык: Английский

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Synergistic Enhancement of Photocatalytic CO₂ Reduction by Built‐in Electric Field/Piezoelectric Effect and Surface Plasmon Resonance via PVDF/CdS/Ag Heterostructure

Small, Год журнала: 2023, Номер 19(52)

Опубликована: Авг. 30, 2023

Photocatalytic reduction of CO2 using solar energy is an effective means to achieve carbon neutrality. However, the photocatalytic efficiency still requires improvements. In this study, polyvinylidene fluoride (PVDF) ferroelectric/piezoelectric nanofiber membranes are prepared by electrospinning. Cadmium sulfide (CdS) nanosheets assembled in situ on surface PVDF based coordination between F- and Cd2+ , then Ag nanoparticles deposited CdS. Because synergistic effect localized plasmon resonance built-in electric field PVDF, PVDF/CdS/Ag under visible light irradiation significantly higher than that any combination CdS, CdS/Ag, or PVDF/CdS. Under micro-vibration simulate air flow, three times static conditions, reaching 240.4 µmol g-1 h-1 . The piezoelectric caused micro-vibrations helps prevent from becoming saturated with carriers provides a continuous driving force for carrier separation.

Язык: Английский

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Heterogeneous catalysis via light-heat dual activation: A path to the breakthrough in C1 chemistry

Joule, Год журнала: 2024, Номер 8(2), С. 312 - 333

Опубликована: Янв. 21, 2024

Язык: Английский

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