Separation and Purification Technology, Год журнала: 2024, Номер 337, С. 126462 - 126462
Опубликована: Янв. 21, 2024
Язык: Английский
Separation and Purification Technology, Год журнала: 2024, Номер 337, С. 126462 - 126462
Опубликована: Янв. 21, 2024
Язык: Английский
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
Процитировано
236Nature 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
Процитировано
217Journal 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
Процитировано
180Advanced 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
Процитировано
114ACS 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
Процитировано
110Nature 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
Процитировано
106Chemical 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
Процитировано
99Nature 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
Процитировано
88Chem, Год журнала: 2023, Номер 9(4), С. 1017 - 1035
Опубликована: Март 13, 2023
Язык: Английский
Процитировано
69Separation and Purification Technology, Год журнала: 2023, Номер 325, С. 124636 - 124636
Опубликована: Июль 20, 2023
Язык: Английский
Процитировано
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