Construction of 2D S‐Scheme Heterojunction Photocatalyst

Advanced Materials, Год журнала: 2023, Номер 36(8)

Опубликована: Ноя. 22, 2023

Abstract Semiconductor photocatalytic technology holds immense promise for converting sustainable solar energy into chemically storable energy, with significant applications in the realms of and environment. However, inherent issue rapid recombination photogenerated electrons holes hinders performance single photocatalysts. To overcome this challenge, construction 2D S‐scheme heterojunction photocatalysts emerges as an effective strategy. The deliberate design dimensionality ensures a substantial interfacial area; while, charge transfer mechanism facilitates efficient separation maximizes redox capabilities. This review commences fresh perspective on heterojunctions, followed by comprehensive exploration preparation methods characterization techniques. Subsequently, recent advancements are summarized. Notably, behind activity enhancement is elucidated. Finally, prospects development presented.

Язык: Английский

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Ultrafast electron transfer at the In2O3/Nb2O5 S-scheme interface for CO2 photoreduction

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Июнь 5, 2024

Abstract Constructing S-scheme heterojunctions proves proficient in achieving the spatial separation of potent photogenerated charge carriers for their participation photoreactions. Nonetheless, restricted contact areas between two phases within heterostructures lead to inefficient interfacial transport, resulting low photocatalytic efficiency from a kinetic perspective. Here, In 2 O 3 /Nb 5 are fabricated through straightforward one-step electrospinning technique, enabling intimate and thereby fostering ultrafast electron transfer (<10 ps), as analyzed via femtosecond transient absorption spectroscopy. As result, powerful photo-electrons holes accumulate Nb conduction band valence band, respectively, exhibiting extended long lifetimes facilitating involvement subsequent Combined with efficient chemisorption activation stable CO on , hybrid nanofibers demonstrate improved performance conversion.

Язык: Английский

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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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Enhancing photocatalytic H2O2 production with Au co-catalysts through electronic structure modification

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Апрель 13, 2024

Abstract Gold-based co-catalysts are a promising class of materials with potential applications in photocatalytic H 2 O production. However, current approaches Au show limited production due to intrinsically weak adsorption at the site. We report an approach strengthen sites, and improve production, through formation electron-deficient δ+ sites by modifying electronic structure. In this case, we synthesis TiO /MoS x -Au, following selective deposition onto MoS surface which is then further anchored . that catalyst achieves significantly increased rate 30.44 mmol g −1 h -saturated solution containing ethanol. Density functional theory calculations X-ray photoelectron spectroscopy analysis reveal mediator induces thereby decreasing antibonding-orbital occupancy Au-O ads subsequently enhancing adsorption. This strategy may be useful for rationally designing structure surfaces facilitate artificial photosynthesis.

Язык: Английский

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COF/In₂S₃ S‐Scheme Photocatalyst with Enhanced Light Absorption and H₂O₂‐Production Activity and fs‐TA Investigation

Advanced Materials, Год журнала: 2024, Номер 36(24)

Опубликована: Фев. 27, 2024

Photocatalytic hydrogen peroxide (H

Язык: Английский

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Highly Selective Photoconversion of CO₂ to CH₄ over SnO₂/Cs₃Bi₂Br₉ Heterojunctions Assisted by S-Scheme Charge Separation

ACS Catalysis, Год журнала: 2023, Номер 13(19), С. 12623 - 12633

Опубликована: Сен. 13, 2023

Exploring photocatalysts to promote the conversion of CO2 valuable chemical fuels is a highly promising approach for mitigating energy scarcity and environmental pollution. Lead-free perovskite Cs3Bi2Br9 quantum dots (QDs) have attracted considerable attention in photoreduction due robust reduction capability controllable product selectivity. Nevertheless, their potential has been impeded by rapid recombination charge carriers, leading unsatisfactory photocatalytic efficiency. Here, unique SnO2/Cs3Bi2Br9 S-scheme heterojunctions are constructed electrostatically self-assembling SnO2 nanofibers with QDs enhance performance. Density functional theory calculations, along experimental studies, reveal that electrons transfer from SnO2, creating directed interfacial electric field bending bands at interfaces. This facilitates transport photoelectrons Cs3Bi2Br9, forming enabling effective separation powerful photoexcited electron/hole pairs. Additionally, profiting enhanced light absorption contributed narrow-bandgap lower barrier CH4 production over surface, heterostructures unveil superior activities high selectivity 70%, without assistance any molecular catalyst or scavenger.

Язык: Английский

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Twistedly hydrophobic basis with suitable aromatic metrics in covalent organic networks govern micropollutant decontamination

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

Опубликована: Окт. 24, 2023

Abstract The pre-designable structure and unique architectures of covalent organic frameworks (COFs) render them attractive as active porous medium for water crisis. However, the effect functional basis with different metrics on regulation interfacial behavior in advanced oxidation decontamination remains a significant challenge. In this study, we pre-design fabricate molecular interfaces by creating ordered π skeletons, incorporating pore sizes, engineering hydrophilic or hydrophobic channels. These synergically break through adsorption energy barrier promote inner-surface renewal, achieving high removal rate typical antibiotic contaminants (like levofloxacin) BTT-DATP-COF, compared BTT-DADP-COF BTT-DAB-COF. experimental theoretical calculations reveal that such enable hole-driven levofloxacin at interface BTT fragments to occur, accompanying electron-mediated oxygen reduction terphenyl motif radicals, endowing it facilitate balanced extraction holes electrons.

Язык: Английский

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Bifunctional CdS/COF S-scheme photocatalyst for enhanced H2 evolution and organic synthesis

Chemical Engineering Journal, Год журнала: 2023, Номер 476, С. 146818 - 146818

Опубликована: Окт. 20, 2023

It is an efficient strategy to construct photocatalysts by integrating the advantages of inorganic semiconductors and covalent organic frameworks (COFs) for H2 generation along with simultaneous oxidation. Herein, inorganic/organic CdS/COF (denoted as TpBD) 2D heterostructure fabricated electrostatic self-assembly method. The ultrathin structure can reduce charge transfer distance, enhance light absorption, multiply reaction sites while S-scheme heterojunction improves separation efficiency. composite acquires outstanding photocatalytic activity 15.1 mmol/g/h, simultaneously convert cheap ascorbic acid value-added 2,3-diketo-L-gulonic acid. Hall effect test elucidates dynamics carrier migration. electron paramagnetic resonance analysis, photo-irradiated Kelvin probe force microscopy, femtosecond transient absorption spectroscopy, theoretical calculation, in-situ irradiation X-ray photoelectron spectroscopy measurements confirm superiority transfer. This research presents new inspiration develop hydrogen production green chemical production.

Язык: Английский

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g-C3N4-based S-scheme heterojunction photocatalysts

Science China Materials, Год журнала: 2024, Номер 67(2), С. 444 - 472

Опубликована: Янв. 24, 2024

Язык: Английский

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In-situ formatting donor-acceptor polymer with giant dipole moment and ultrafast exciton separation

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Фев. 13, 2024

Abstract Donor-acceptor semiconducting polymers present countless opportunities for application in photocatalysis. Previous studies have showcased their advantages through direct bottom-up methods. Unfortunately, these approaches often involve harsh reaction conditions, overlooking the impact of uncontrolled polymerization degrees on Besides, mechanism behind separation electron-hole pairs (excitons) donor-acceptor remains elusive. This study presents a post-synthetic method involving light-induced transformation building blocks hyper-cross-linked from donor-carbon-donor to donor-carbon-acceptor states, resulting polymer with substantial intramolecular dipole moment. Thus, excitons are efficiently separated transformed polymer. The utility this strategy is exemplified by enhanced photocatalytic hydrogen peroxide synthesis. Encouragingly, our observations reveal formation charge transfer states using time-resolved techniques, confirming transient exciton behavior and relaxation. not only guides development highly efficient photocatalysts but also applies various fields, including organic solar cells, light-emitting diodes, sensors.

Язык: Английский

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