2D Transition Metal Dichalcogenides for Photocatalysis

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(13)

Опубликована: Янв. 3, 2023

Abstract Two‐dimensional (2D) transition metal dichalcogenides (TMDs), a rising star in the post‐graphene era, are fundamentally and technologically intriguing for photocatalysis. Their extraordinary electronic, optical, chemical properties endow them as promising materials effectively harvesting light catalyzing redox reaction Here, we present tutorial‐style review of field 2D TMDs photocatalysis to educate researchers (especially new‐comers), which begins with brief introduction fundamentals along synthesis this type material, then look deeply into merits co‐catalysts active photocatalysts, followed by an overview challenges corresponding strategies photocatalysis, finally ahead topic.

Язык: Английский

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Synergy of Pd atoms and oxygen vacancies on In2O3 for methane conversion under visible light

Nature Communications, Год журнала: 2022, Номер 13(1)

Опубликована: Май 25, 2022

Methane (CH4) oxidation to high value chemicals under mild conditions through photocatalysis is a sustainable and appealing pathway, nevertheless confronting the critical issues regarding both conversion selectivity. Herein, visible irradiation (420 nm), synergy of palladium (Pd) atom cocatalyst oxygen vacancies (OVs) on In2O3 nanorods enables superior photocatalytic CH4 activation by O2. The optimized catalyst reaches ca. 100 μmol h-1 C1 oxygenates, with selectivity primary products (CH3OH CH3OOH) up 82.5%. Mechanism investigation elucidates that such induced dedicated function Pd single atoms boosting hole electron transfer, respectively. O2 proven be only source for CH3OH production, while H2O acts as promoter efficient ·OH production facilitates product desorption indicated DFT modeling. This work thus provides new understandings simultaneous regulation activity cocatalysts vacancies.

Язык: Английский

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Enabling Specific Photocatalytic Methane Oxidation by Controlling Free Radical Type

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(4), С. 2698 - 2707

Опубликована: Янв. 17, 2023

Selective CH4 oxidation to CH3OH or HCHO with O2 in H2O under mild conditions provides a desired sustainable pathway for synthesis of commodity chemicals. However, manipulating reaction selectivity while maintaining high productivity remains huge challenge due the difficulty kinetic control formation oxygenate against its overoxidation. Here, we propose highly efficient strategy, based on precise type as-formed radicals by rational design photocatalysts, achieve both and photooxidation first time. Through tuning band structure size active sites (i.e., single atoms nanoparticles) our Au/In2O3 catalyst, show alternative two important radicals, •OOH •OH, which leads distinctly different paths HCHO, respectively. This approach gives rise remarkable yield 97.62% 6.09 mmol g-1 In2O3-supported Au (Au1/In2O3) an exceptional 89.42% 5.95 nanoparticles (AuNPs/In2O3), respectively, upon photocatalytic 3 h at room temperature. work opens new avenue toward selective delicate composite photocatalysts.

Язык: Английский

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Construction of Ultrathin S‐Scheme Heterojunctions of Single Ni Atom Immobilized Ti‐MOF and BiVO₄ for CO₂ Photoconversion of nearly 100% to CO by Pure Water

Advanced Materials, Год журнала: 2022, Номер 34(41)

Опубликована: Авг. 20, 2022

To rationally design single-atom metal-organic framework (MOF)-involving photocatalysts remains an ongoing challenge for efficient CO2 conversion. Here, cuppy microstructures, consisting of a Ti(IV)-oxo node and three linked carboxylic moieties, in the single-coordination-layer Ti2 (H2 dobdc)3 MOF (NTU-9) are exploited to immobilize abundant single Ni(II) sites (Ni@MOF). The coupling Ni@MOF with BiVO4 (BVO) nanosheets by H-bonding-induced assembly process obtains wide-spectrum 2D heterojunctions. optimal heterojunction exhibits competitive performance enables around 66-fold conversion that BVO nanoparticles pure water, nearly 100% CO selectivity. exceptional photoactivity is attributed favorable S-scheme charge transfer from then sites. Noteworthily, anchored vicinal moieties serving as unique local microenvironment (LME) found synergistically catalyze Specifically, hydroxyl groups can form H-bonds promote its adsorption on sites, also provide accessible protons facilitate H-assisted reduction. Moreover, desorption subsequent LME proved be thermodynamically favored, hence dominates high This work highlights significance modulating atoms realizing carbon neutralization.

Язык: Английский

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Active Site Engineering on Plasmonic Nanostructures for Efficient Photocatalysis

ACS Nano, Год журнала: 2023, Номер 17(5), С. 4193 - 4229

Опубликована: Фев. 20, 2023

Plasmonic nanostructures have shown immense potential in photocatalysis because of their distinct photochemical properties associated with tunable photoresponses and strong light–matter interactions. The introduction highly active sites is essential to fully exploit the plasmonic photocatalysis, considering inferior intrinsic activities typical metals. This review focuses on site-engineered enhanced photocatalytic performance, wherein are classified into four types (i.e., metallic sites, defect ligand-grafted interface sites). synergy between discussed detail after briefly introducing material synthesis characterization methods. Active can promote coupling solar energy harvested by metal catalytic reactions form local electromagnetic fields, hot carriers, photothermal heating. Moreover, efficient potentially regulates reaction pathway facilitating excited state formation reactants, changing status creating additional using photoexcited Afterward, application emerging summarized. Finally, a summary perspective existing challenges future opportunities presented. aims deliver some insights from expediting discovery high-performance photocatalysts.

Язык: Английский

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Efficient hole abstraction for highly selective oxidative coupling of methane by Au-sputtered TiO2 photocatalysts

Nature Energy, Год журнала: 2023, Номер 8(9), С. 1013 - 1022

Опубликована: Авг. 17, 2023

Abstract Photocatalytic oxidative coupling of methane (OCM) produces C 2 molecules that can be used as building blocks for synthesis fuels and chemicals. However, the yield rate selectivity products are still moderate due to stable nature molecules. Here we develop a Au nanocluster-loaded TiO photocatalyst by sputtering approach, achieving high conversion 1.1 mmol h −1 , ~90% apparent quantum efficiency 10.3 ± 0.6%. The /C 2+ is on same order magnitude benchmark thermal catalysts in OCM processes operated at temperature (>680 °C). nanoparticles shown prolong photoelectron lifetimes factor 66 O reduction, together with acting hole acceptor catalytic centre promote adsorption, C–H activation C–C coupling. This work underscores importance multifunctional co-catalysts mechanistic understanding improve photocatalytic OCM.

Язык: Английский

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Urea catalytic oxidation for energy and environmental applications

Chemical Society Reviews, Год журнала: 2024, Номер 53(3), С. 1552 - 1591

Опубликована: Янв. 1, 2024

This review evaluates state-of-the-art advances in electrocatalytic and photo(electro)catalytic urea oxidation from fundamentals materials to energy environmental applications.

Язык: Английский

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Nearly 100% selective and visible-light-driven methane conversion to formaldehyde via. single-atom Cu and Wδ+

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Май 10, 2023

Direct solar-driven methane (CH4) reforming is highly desirable but challenging, particularly to achieve a value-added product with high selectivity. Here, we identify synergistic ensemble effect of atomically dispersed copper (Cu) species and partially reduced tungsten (Wδ+), stabilised over an oxygen-vacancy-rich WO3, which enables exceptional photocatalytic CH4 conversion formaldehyde (HCHO) under visible light, leading nearly 100% selectivity, very yield 4979.0 μmol·g-1 within 2 h, the normalised mass activity 8.5 × 106 μmol·g-1Cu·h-1 HCHO at ambient temperature. In-situ EPR XPS analyses indicate that Cu serve as electron acceptor, promoting photo-induced transfer from conduction band O2, generating reactive •OOH radicals. In parallel, adjacent Wδ+ act hole acceptor preferred adsorption activation site H2O produce hydroxyl radicals (•OH), thus activate methyl (•CH3). The synergy dual active sites boosts overall efficiency selectivity process.

Язык: Английский

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Asymmetrically coordinated cobalt single atom on carbon nitride for highly selective photocatalytic oxidation of CH4 to CH3OH

Chem, Год журнала: 2023, Номер 9(4), С. 1017 - 1035

Опубликована: Март 13, 2023

Язык: Английский

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The synergistic effect of surface vacancies and heterojunctions for efficient photocatalysis: A review

Separation and Purification Technology, Год журнала: 2023, Номер 325, С. 124636 - 124636

Опубликована: Июль 20, 2023

Язык: Английский

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