Artificial Photosynthetic System with Spatial Dual Reduction Site Enabling Enhanced Solar Hydrogen Production

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(9)

Published: Nov. 28, 2023

Abstract Although S‐scheme artificial photosynthesis shows promise for photocatalytic hydrogen production, traditional methods often overly concentrate on a single reduction site. This limitation results in inadequate redox capability and inefficient charge separation, which hampers the efficiency of evolution reaction. To overcome this limitation, double system is proposed that leverages dual sites, thereby preserving energetic photo‐electrons holes to enhance apparent quantum efficiency. The design features junction consisting CdS nanospheres decorated with anatase TiO 2 nanoparticles coupled graphitic C 3 N 4 . as‐prepared catalyst exhibits rate 26.84 mmol g −1 h an 40.2% at 365 nm. enhanced ascribed efficient separation transport induced by S‐scheme. Both theoretical calculations comprehensive spectroscopy tests (both situ ex situ) affirm across interface. Moreover, substituting reduction‐type other similar sulfides like ZnIn S , ZnS, MoS In further confirms feasibility configuration. findings provide pathway designing more effective photosynthetic systems, opening up fresh perspectives enhancing performance.

Language: Английский

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2D semiconductor nanosheets for solar photocatalysis

EcoEnergy, Journal Year: 2023, Volume and Issue: 1(2), P. 248 - 295

Published: Dec. 1, 2023

Abstract In the advancing world of graphene, highly anisotropic 2D semiconductor nanosheets, notable for their nanometer‐scale thickness, have emerged as a leading innovation, displaying immense potential in exploration renewable and clean energy production. These garnered significant attention from researchers. The nanosheets are marked by extraordinary electronic, optical, chemical attributes, positioning them attractive foundational components heterogeneous photocatalysts. This review diligently summarizes both seminal work ongoing developments pertaining to application solar within context photocatalysis. We begin detailing distinctive properties concentrating on pivotal roles augmenting photocatalytic efficiency, explaining intrinsic mechanisms that govern migration rate photogenerated carriers material's surface. Subsequently, we delineate methods employed synthesize typical nanosheets. alignment with overarching objective expanding light absorption capacity accelerating charge transfer, also examine current research hybridization techniques involving materials varied dimensions, well deployment diverse applications. conclude identifying promising avenues challenges await further this burgeoning field.

Language: Английский

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S-Scheme Heterojunction/Single-Atom Dual-Driven Charge Transport for Photocatalytic Hydrogen Production

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(10), P. 7308 - 7320

Published: April 25, 2024

The rational design and modification of heterojunction photocatalysts aimed at achieving fast charge transport efficient photocatalytic performance is a central goal solar-light-driven water splitting hydrogen evolution, yet this remains challenge. Herein, we prepare hierarchical photocatalyst composed few-layer violet phosphorene (VP), cadmium sulfide (CdS) nanoparticles (NPs), Pd single atoms (SAs) by facile one-step ball-milling strategy. underlying VP/CdS p–n heterojunctions are verified to adopt S-scheme directional transfer combining in situ irradiated X-ray photoelectron spectroscopy electron paramagnetic resonance. atomically dispersed sites the low-valence state coupled with synergistically achieve ultrafast (2.2 ps), which interfacial Pd–S Pd–P bonds serve as channels. In addition, density-functional theory calculations reveal key role enhancement light-harvesting capacity optimization proton adsorption thermodynamics. A visible-light production rate 82.5 mmol h–1 g–1 attained an optimal 1 wt % Pd–5 photocatalyst, manifests 54-fold increase respect that CdS NPs, addition apparent quantum efficiency (AQE) 25.7% 420 nm. This work showcases valid combination SAs for separation promoting others.

Language: Английский

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Dual-facet engineering of surface carboxyl functionalization and interlayer potassium ions regulation in carbon nitride for enhanced CO2 photoreduction

Science China Materials, Journal Year: 2024, Volume and Issue: 67(2), P. 473 - 483

Published: Jan. 12, 2024

Language: Английский

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Asymmetric Atomic Dual‐Sites for Photocatalytic CO₂ Reduction

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(38)

Published: July 23, 2024

Abstract Atomically dispersed active sites in a photocatalyst offer unique advantages such as locally tuned electronic structures, quantum size effects, and maximum utilization of atomic species. Among these, asymmetric dual‐sites are particular interest because their charge distribution generates local built‐in electric potential to enhance separation transfer. Moreover, the dual provide flexibility for tuning complex multielectron multireaction pathways, CO 2 reduction reactions. The coordination opens new possibilities engineering structure–activity–selectivity relationship. This comprehensive overview discusses efficient sustainable photocatalysis processes photocatalytic reduction, focusing on strategic active‐site design future challenges. It serves timely reference development conversion processes, specifically exploring here exemplified by into valuable chemicals.

Language: Английский

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General Design Concept of High‐Performance Single‐Atom‐Site Catalysts for H₂O₂ Electrosynthesis

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(24)

Published: March 5, 2024

Hydrogen peroxide (H

Language: Английский

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Regulating the Electronic Synergy of Asymmetric Atomic Fe Sites with Adjacent Defects for Boosting Activity and Durability toward Oxygen Reduction

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(29)

Published: March 17, 2024

Abstract The oxygen reduction reaction (ORR) plays a fundamental role in sustainable energy technologies. However, the creation of non‐precious metal electrocatalysts with high ORR activity and durability under all pH conditions is great significance but remains challenging. Herein, aim to overcome this challenge by creating Fe single atom catalyst on 2D defect‐containing nitrogen‐doped carbon support (Fe 1 /DNC) via microenvironment engineering strategy. Microkinetic modeling reveals that FeN 4 (OH) moieties are real active sites conditions. Due synergistic promotion effect denser accessible defect‐induced electronic properties, /DNC achieves extraordinary alkaline, acidic, neutral conditions, half‐wave potentials 0.95, 0.82, 0.70 V, respectively. Moreover, negligible performance decay observed stability methanol tolerance tests. Zn‐air battery employing delivers remarkable peak power density long‐term operational durability. Theoretical analysis provides compelling evidence defects adjacent can endow an inductive reshape properties balance OOH* formation OH* reduction. This work offers insight into regulation asymmetric coordination structure for boosting electrocatalytic stability.

Language: Английский

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Solvent-free selective hydrogenation of nitroaromatics to azoxy compounds over Co single atoms decorated on Nb2O5 nanomeshes

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: April 12, 2024

Abstract The solvent-free selective hydrogenation of nitroaromatics to azoxy compounds is highly important, yet challenging. Herein, we report an efficient strategy construct individually dispersed Co atoms decorated on niobium pentaoxide nanomeshes with unique geometric and electronic properties. use this supported single atom catalysts in the nitrobenzene azoxybenzene results high catalytic activity selectivity, 99% selectivity conversion within 0.5 h. Remarkably, it delivers exceptionally turnover frequency 40377 h –1 , which amongst similar state-of-the-art catalysts. In addition, demonstrates remarkable recyclability, reaction scalability, wide substrate scope. Density functional theory calculations reveal that are significantly promoted by properties strong metal-support interaction 1 /Nb 2 O 5 . absence precious metals, toxic solvents, reagents makes catalyst more appealing for synthesizing from nitroaromatics. Our findings suggest great potential access boosted thus offering blueprints design nanomaterials organocatalysis.

Language: Английский

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Photocatalytic H2O2 production over boron-doped g-C3N4 containing coordinatively unsaturated FeOOH sites and CoOx clusters

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Oct. 25, 2024

Graphitic carbon nitride (g-C

Language: Английский

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S‐Scheme g‐C₃N₄/CdS Heterostructures Grafting Single Pd Atoms for Ultrafast Charge Transport and Efficient Visible‐Light‐Driven H₂ Evolution

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(38)

Published: May 11, 2024

Abstract Emerging step‐scheme (S‐scheme) heterostructures hold unique superiority in steering directional charge transport and reinforcing redox capacity, yet rational modification of S‐scheme by single atoms (SAs) for efficient photocatalytic H 2 evolution is rarely reported. In this work, Pd SAs‐modulated organic–inorganic g‐C 3 N 4 /CdS are designed prepared a one‐pot mechanochemical approach allowing nanosheets/CdS nanoparticles to confine atomically dispersed co‐catalysts. The charge‐transfer pathway corroborated combination situ irradiated X‐ray photoelectron spectroscopy, electron paramagnetic resonance, Kelvin probe force microscopy. Density functional theory (DFT) calculations, high‐angle annular dark‐field scanning transmission microscopy, absorption fine structure identify Pd‐S Pd‐N atomic moieties underpinned the electronic interaction between SAs heterostructures, which d ‐band center optimized proton adsorption thermodynamically. Further, alongside concert boost rapid migration photogenerated electrons (1.05 ps) via Pd─S Pd─N bond‐derived channels. A maximal rate 85.66 mmol h −1 g achieved 1 wt% Pd‐20 hierarchical composites. This work may guide design high‐efficiency S‐scheme‐based photocatalysts solar‐to‐H conversion beyond.

Language: Английский

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