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

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(50)

Published: Nov. 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.

Language: Английский

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Reticular framework materials for photocatalytic organic reactions

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(22), P. 7949 - 8004

Published: Jan. 1, 2023

Photocatalytic organic reactions, harvesting solar energy to produce high value-added chemicals, have attracted increasing attention as a sustainable approach address the global crisis and environmental issues. Reticular framework materials, including metal-organic frameworks (MOFs) covalent (COFs), are widely considered promising candidates for photocatalysis owing their crystallinity, tailorable pore environment extensive structural diversity. Although design synthesis of MOFs COFs been intensively developed in last 20 years, applications photocatalytic transformations still preliminary stage, making systematic summary necessary. Thus, this review aims provide comprehensive understanding useful guidelines exploration suitable MOF COF photocatalysts towards appropriate reactions. The commonly used reactions categorized facilitate identification reaction types. From practical viewpoint, fundamentals experimental design, active species, performance evaluation external conditions, discussed detail easy experimentation. Furthermore, latest advances COFs, composites, comprehensively summarized according actual sites, together with discussion structure-property relationship. We believe that study will be helpful researchers novel reticular various synthetic applications.

Language: Английский

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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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Construction of a 2D/2D Crystalline Porous Materials Based S‐Scheme Heterojunction for Efficient Photocatalytic H₂ Production

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(11)

Published: Jan. 7, 2024

Abstract Generally, the low electron–hole separation efficiency of covalent organic frameworks (COFs) prevents their catalytic performance from reaching satisfactory results. For this reason, creation heterojunctions is considered an effective strategy but usually suffers dimensional mismatch integrated material, even at expense its redox capacity. To overcome these difficulties, a novel 2D/2D S‐scheme heterojunction between H 2 N–Cu–MOF (NCM) and TpPa–1–COF (TP1C) successfully constructed for efficient photocatalytic production. The matching dimensions two crystalline porous materials enables with abundant surface reactive sites, strong interaction optimized electronic structure. Moreover, combination can also form S–scheme heterojunction, which not only promote pair, preserve ability, thus remarkably boosting competence. Consequently, rate optimal 20% NCM/TP1C in production reaches 4.19 mmol g −1 h , 46.5 times higher than that bare NCM, 22.1 folds over pure TP1C. This research offers innovative perspective formation based on crystal solar energy utilization.

Language: Английский

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An interfacial C-S bond bridged S-scheme ZnS/C3N5 for photocatalytic H2 evolution: Opposite internal-electric-field of ZnS/C3N4, increased field strength, and accelerated surface reaction

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 664, P. 960 - 971

Published: March 2, 2024

Language: Английский

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Constructing host–guest recognition electrolytes promotes the Li⁺ kinetics in solid-state batteries

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(2), P. 780 - 790

Published: Jan. 1, 2024

Ti-MOFs with synergetic various sites are designed to serve as a “host” platform for GPE tune the electrolyte properties. This unique system can improve Li + ion conduction, mechanical strength and ability withstand high voltage.

Language: Английский

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Confining non-porous MOF in amine-functionalized aerogel for efficient sequestration of iodine contaminants

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 159595 - 159595

Published: Jan. 1, 2025

Language: Английский

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Core-shell MOF@COF photocatalysts for synergistic enhanced U(VI) and tetracycline cleanup through space and carrier separation

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 485, P. 150026 - 150026

Published: Feb. 28, 2024

Language: Английский

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Hollow core-shell B-g-C3N4-x@Bi2S3/In2S3 dual S-scheme heterojunction photothermal nanoreactor: Boosting photothermal catalytic activity in confined space

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 484, P. 149399 - 149399

Published: Feb. 7, 2024

Language: Английский

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Enhancing CO2 photoreduction by construction of g-C3N4/Co-MOFs S-scheme heterojunction

Applied Surface Science, Journal Year: 2025, Volume and Issue: unknown, P. 162752 - 162752

Published: Feb. 1, 2025

Language: Английский

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