Atomically dispersed materials: Ideal catalysts in atomic era

Nano Research, Год журнала: 2023, Номер 17(1), С. 18 - 38

Опубликована: Май 25, 2023

Язык: Английский

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Hydroxyl-Bonded Ru on Metallic TiN Surface Catalyzing CO₂ Reduction with H₂O by Infrared Light

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(50), С. 27415 - 27423

Опубликована: Дек. 11, 2023

Synchronized conversion of CO2 and H2O into hydrocarbons oxygen via infrared-ignited photocatalysis remains a challenge. Herein, the hydroxyl-coordinated single-site Ru is anchored precisely on metallic TiN surface by NaBH4/NaOH reforming method to construct an infrared-responsive HO-Ru/TiN photocatalyst. Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (ac-HAADF-STEM) X-ray absorption spectroscopy (XAS) confirm atomic distribution species. XAS density functional theory (DFT) calculations unveil formation HO-RuN5-Ti Lewis pair sites, which achieves efficient polarization/activation dual coordination with C O atoms HO-Ru/TiN. Also, implanting species powerfully boosts separation transfer photoinduced charges. Under infrared irradiation, catalyst shows superior CO2-to-CO transformation activity coupled oxidation release O2, reduction rate can further be promoted about 3-fold under simulated sunlight. With key reaction intermediates determined in situ diffuse reflectance Fourier transform (DRIFTS) predicted DFT simulations, possible photoredox mechanism system proposed.

Язык: Английский

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Carbon nitride based materials: more than just a support for single-atom catalysis

Chemical Society Reviews, Год журнала: 2023, Номер 52(15), С. 4878 - 4932

Опубликована: Янв. 1, 2023

Recently, the missing link between homogeneous and heterogeneous catalysis has been found it was named single-atom (SAC). However, SAC field still faces important challenges, one of which is controlling bonding/coordination single atoms support in order to compensate for increase surface energy when particle size reduced due atomic dispersion. Excellent candidates meet this requirement are carbon nitride (CN)-based materials. Metal can be firmly trapped nitrogen-rich coordination sites CN materials, makes them a unique class hosts preparing catalysts (SACs). As most promising two-dimensional supports stabilize isolated metal atoms, materials have increasingly employed SACs. Herein, we will cover recent advances single-atoms supported by In review, characterization techniques challenges faced topic discussed, commonly synthetic methods delineated different Finally, catalytic performance SACs based on nitrides reviewed with special focus their photocatalytic applications. particular, prove as non-innocent support. The relationship two-way, where change electronic properties support, while features matrix tune activity reactions. highlight frontiers field, including analytical method development, truly controlled methods, allowing fine control loading multi-element synthesis, how understanding two-way exchange behind push next level.

Язык: Английский

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Atomically Dispersed Au-Assisted C–C Coupling on Red Phosphorus for CO₂ Photoreduction to C₂H₆

Journal of the American Chemical Society, Год журнала: 2022, Номер 144(48), С. 22075 - 22082

Опубликована: Ноя. 22, 2022

Single-atom catalysts have exhibited great potential in the photocatalytic conversion of CO2 to C2 products, but generation gaseous multi-carbon hydrocarbon products is still challenging. Previously, supports a single atom consist multiple elements, making C-C coupling difficult because coordination environment single-atom sites diversified and control. Here, we steer by implanting an Au on red phosphorus (Au1/RP), support with uniform structure composed element, lower electronegativity, better ability absorb CO2. The electron-rich atoms near can function as active for activation. effectively reduce energy barrier coupling, boosting reaction kinetics formation C2H6. Notably, C2H6 selectivity turnover frequency Au1/RP reach 96% 7.39 h-1 without sacrificial agent, respectively, which almost represents best photocatalyst chemical synthesis date. This research will provide new ideas design high-efficiency photocatalysts products.

Язык: Английский

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Metal-sulfide-based heterojunction photocatalysts: Principles, impact, applications, and in-situ characterization

CHINESE JOURNAL OF CATALYSIS (CHINESE VERSION), Год журнала: 2023, Номер 49, С. 42 - 67

Опубликована: Июнь 1, 2023

Язык: Английский

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Controlled synthesis of hollow carbon ring incorporated g-C3N4 tubes for boosting photocatalytic H2O2 production

Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 337, С. 122933 - 122933

Опубликована: Май 31, 2023

Язык: Английский

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Single-atom Nb anchored on graphitic carbon nitride for boosting electron transfer towards improved photocatalytic performance

Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 328, С. 122495 - 122495

Опубликована: Фев. 20, 2023

Язык: Английский

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Dual Atom Catalysts for Energy and Environmental Applications

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(40)

Опубликована: Июнь 7, 2023

The pursuit of high metal utilization in heterogeneous catalysis has triggered the burgeoning interest various atomically dispersed catalysts. Our aim this review is to assess key recent findings synthesis, characterization, structure-property relationship and computational studies dual-atom catalysts (DACs), which cover full spectrum applications thermocatalysis, electrocatalysis photocatalysis. In particular, combination qualitative quantitative characterization with cooperation DFT insights, synergies superiorities DACs compare counterparts, high-throughput catalyst exploration screening machine-learning algorithms are highlighted. Undoubtably, it would be wise expect more fascinating developments field as tunable

Язык: Английский

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Dinuclear metal synergistic catalysis for energy conversion

Chemical Society Reviews, Год журнала: 2023, Номер 52(9), С. 3170 - 3214

Опубликована: Янв. 1, 2023

An exclusive review focusing on catalysts exhibiting the dinuclear metal synergistic catalysis (DMSC) effect for energy conversion reactions is presented.

Язык: Английский

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Electronic Transmission Channels Promoting Charge Separation of Conjugated Polymers for Photocatalytic CO₂ Reduction with Controllable Selectivity

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(22)

Опубликована: Апрель 3, 2023

Conjugated polymers (CPs) represent a promising platform for photocatalytic CO2 fixation owing to their suitable band structures that meet the requirements of reduction potential value-added fuels. However, performance CPs is rather restrained by low charge transfer efficiency. Herein, we rationally designed three with more delocalized electronic transmission channel and planar molecular structure, which are regarded evidently reduce exciton binding energy (Eb ) accelerate internal process. Besides, assembly electron-output "tentacles" cocatalysts on surface could effectively facilitate interfacial electron delivery. Accordingly, optimal P-2CN exhibits an apparent quantum yield 4.6 % at 420 nm CO. Further adjusting amounts cyano groups cocatalysts, CO selectivity be obtained in range 0-80.5 %.

Язык: Английский

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