Rapid Charge Transfer Endowed by Interfacial Ni‐O Bonding in S‐scheme Heterojunction for Efficient Photocatalytic H₂ and Imine Production

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(50)

Опубликована: Ноя. 1, 2023

Cooperative coupling of H2 evolution with oxidative organic synthesis is promising in avoiding the use sacrificial agents and producing hydrogen energy value-added chemicals simultaneously. Nonetheless, photocatalytic activity obstructed by sluggish electron-hole separation limited redox potentials. Herein, Ni-doped Zn0.2 Cd0.8 S quantum dots are chosen after screening DFT simulation to couple TiO2 microspheres, forming a step-scheme heterojunction. The configuration tunes highly active site for augmented evolution, interfacial Ni-O bonds provide fast channels at atomic level lower barrier charge transfer. Also, calculations reveal an enhanced built-in electric field heterojunction superior migration separation. Kinetic analysis femtosecond transient absorption spectra demonstrates that expedited electrons first transfer Ni2+ then sites. Therefore, designed catalyst delivers drastically elevated yield (4.55 mmol g-1 h-1 ) N-benzylidenebenzylamine production rate (3.35 ). This work provides atomic-scale insights into coordinated modulation sites fields ameliorative performance.

Язык: Английский

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Photoredox-catalyzed coupling of CO2 reduction and amines oxidation by Cu doped CdS quantum dots

Molecular Catalysis, Год журнала: 2024, Номер 554, С. 113858 - 113858

Опубликована: Янв. 20, 2024

Язык: Английский

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MoS2 decorated CdS composite catalyst for photoredox-mediated C–N coupling of amines to imines and hydrogen production

Molecular Catalysis, Год журнала: 2024, Номер 557, С. 113991 - 113991

Опубликована: Фев. 29, 2024

Язык: Английский

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Full‐Space Electric Field in Mo‐Decorated Zn₂In₂S₅ Polarization Photocatalyst for Oriented Charge Flow and Efficient Hydrogen Production

Advanced Materials, Год журнала: 2024, Номер 36(31)

Опубликована: Май 18, 2024

Integration of photocatalytic hydrogen (H

Язык: Английский

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Visible-Light-Driven Highly Selective 5-Hydroxymethylfurfural Upgrading and H₂ Generation via Atomically Dispersed Ni Sites on ZnIn₂S₄ Nanosheets

ACS Catalysis, Год журнала: 2024, Номер 14(11), С. 8343 - 8352

Опубликована: Май 14, 2024

Solar-driven biomass upgrading coupled with H2 generation is promising for achieving carbon neutrality. However, identification of the active sites simultaneous photocatalytic redox reactions remains elusive at atomic level. Herein, through rational construction atomically dispersed Ni on ZnIn2S4 nanosheets (Ni1/ZIS), we decipher reactive that enable high-performance 5-hydroxymethylfurfural (HMF) oxidation evolution. Under visible-light irradiation, Ni1/ZIS greatly outperforms its pristine ZIS counterpart and can deliver high selectivity (>97%) 2,5-diformylfuran (DFF), along high-activity DFF production (394 μmol g–1 h–1) evolution (342.2 in a near stoichiometric ratio. Combined detailed experiments theoretical calculations uncover species act as HMF oxidation, while S are favored This work provides new insights into development artificial photosynthesis value-added chemicals from via sites.

Язык: Английский

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Modulating Adsorption–Redox Sites and Charge Separation of Cs₃Bi₂Br_9–x@AgBr Core–Shell Heterostructure for Selective Toluene Photooxidation

ACS Energy Letters, Год журнала: 2024, Номер 9(4), С. 1743 - 1752

Опубликована: Март 26, 2024

Constructing vacancy-decorated heterojunction photocatalysts is a feasible strategy for highly efficient photooxidation of toluene to benzaldehyde. However, poor interface interaction and vacancy-triggered mismatched redox kinetics seriously impede photocatalytic activity improvement. Herein, chemically bonded Cs3Bi2Br9–x@AgBr core–shell with unified adsorption-redox sites fabricated via an in-situ light-assisted Ag+ insertion method. Experiments theoretical calculations demonstrate that the type-II band alignment interfacial Bi–Br–Ag bonds boosts charge separation. Moreover, because greater oxygen adsorption energy steric-hindrance effect AgBr shell, preferred site O2 modulated from Br vacancy (VBr, trapping holes) its corresponding reduction (AgBr, gathering electrons), thereby ensuring VBr-enhancing adsorption/oxidation on Cs3Bi2Br9. Therefore, exhibits improved benzaldehyde production rate 5.61 mmol g–1 h–1 (selectivity: 91%), outperforming pure Cs3Bi2Br9 by factor 6. This work underlines importance rational design heterointerface at atomic level in photocatalysis.

Язык: Английский

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Rationally designed photothermal-pyroelectric Fe0.9Ni0.1S2/ZnSnO3 Z-scheme heterojunction for promoting electrical charge polarization towards optimized photocatalytic H2 evolution and intermolecular N-N coupling reaction

Separation and Purification Technology, Год журнала: 2024, Номер unknown, С. 130201 - 130201

Опубликована: Окт. 1, 2024

Язык: Английский

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Photocatalytic benzylamine coupling dominated by modulation of linkers in donor-acceptor covalent organic frameworks

Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер 352, С. 124020 - 124020

Опубликована: Апрель 21, 2024

Язык: Английский

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Selective Imines Synthesis by Designing an Atomic-Level Cu–Pt Electron Transfer Channel over CdS Nanosheets

ACS Catalysis, Год журнала: 2023, Номер 14(2), С. 657 - 669

Опубликована: Дек. 29, 2023

The precise design of the charge carrier relay channel and active sites semiconductor-based photocatalysts is highly crucial for target selective photoredox synthesis. In this context, we report an atomic-level catalyst strategy based on depositing Pt single atoms (SAs) onto Cu-doped ultrathin cadmium sulfide nanosheets (CdS/Cu/Pt) to enable optimized band structure, a directional transfer channel, favorable catalytic efficient dehydrocoupling amines imines hydrogen (H2). Cu dopant acts as unique electron bridge construct Cu–Pt with assistance atomically dispersed sites, thereby promoting separation kinetics. introduction SAs not only facilitates H2 generation by decreasing overpotential proton reduction but also improves selectivity synthesis because weak adsorption prevents further hydrogenation secondary amines. This work anticipated inspire rational atomic precision coproduction renewable fuels value-added fine chemicals.

Язык: Английский

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Fabrication of Co3O4@ZnIn2S4 for photocatalytic hydrogen evolution: Insights into the synergistic mechanism of photothermal effect and heterojunction

Journal of Colloid and Interface Science, Год журнала: 2023, Номер 650, С. 1974 - 1982

Опубликована: Июль 25, 2023

Язык: Английский

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