Twin S-Scheme g-C₃N₄/CuFe₂O₄/ZnIn₂S₄ Heterojunction with a Self-Supporting Three-Phase System for Photocatalytic CO₂ Reduction: Mechanism Insight and DFT Calculations

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(7), P. 5326 - 5343

Published: March 26, 2024

The use of photocatalytic solar energy to drive CO2 reduction is beneficial for addressing fossil fuel shortages and environmental pollution issues. We synthesized a twin S-scheme g-C3N4/CuFe2O4/ZnIn2S4 heterojunction, which was used construct self-supporting three-phase system reduction. Two built-in electric fields in this heterojunction induced effective migration photogenerated carriers, resulting wide light response range strong oxidation ability. This without sacrificial agent had high CH4 selectivity (96.8%) surprise production rate (267.4 μmol g–1 h–1), still maintained an excellent cycle (249–267.4 h–1) during five cycles. In addition, possessed both hydrophilicity hydrophobicity, achieved efficient transformation into by controlling interface wettability. g-C3N4 as hydrophobic layer promoted mass transfer achieve the enrichment on surface; ZnIn2S4 hydrophilic could well adsorb H2O, further oxidized holes many protons (H+). Finally, DFT calculations found that Fe–N bonds located between CuFe2O4 played crucial role They served bridge electron induce bending adsorption CO2, enhanced *CO stabilization *H.

Language: Английский

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A superlattice interface and S-scheme heterojunction for ultrafast charge separation and transfer in photocatalytic H2 evolution

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

Published: Nov. 7, 2024

The rapid recombination of photoinduced charge carriers in semiconductors fundamentally limits their application photocatalysis. Herein, we report that a superlattice interface and S-scheme heterojunction based on Mn

Language: Английский

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Modulation of Sulfur Vacancies in ZnIn₂S₄/MXene Schottky Heterojunction Photocatalyst Promotes Hydrogen Evolution

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(37)

Published: April 15, 2024

Abstract The sustainable production of hydrogen utilizing solar energy is a pivotal strategy for reducing reliance on fossil fuels. ZnIn 2 S 4 (ZIS), as typical metal sulfide semiconductor, has received extensive attention in photocatalysis. Although the introduction sulfur (S) vacancies ZIS to enhance photocatalytic by creating defect levels been explored, detailed studies control and modulation S‐vacancies are sparce. This study demonstrates that while moderate can evolution, excessive may hinder process, underscoring importance S‐vacancy modulation. Guided theoretical calculations, We have designed synthesized with modulated realize favorable adsorption‐free integrated Schottky‐heterojunction MXene co‐catalysts enhanced evolution. optimized evolution performance /MXene (ZMX) reaches 14.82 mmol g −1 h under visible light irradiation, surpassing many reported ‐based photocatalysts. ascribed widened absorption carrier transportation realized co‐catalytic effect. Femtosecond ultrafast (fs‐TA) spectra other in‐situ/ex‐situ characterizations further prove an efficient separation transfer as‐prepared ZMX catalyst. These findings open up new perspectives designing catalysts vacancy

Language: Английский

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Fluorenone‐Based Covalent Triazine Frameworks/Twinned Zn_0.5Cd_0.5S S‐scheme Heterojunction for Efficient Photocatalytic H₂ Evolution

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(28)

Published: March 12, 2024

Abstract Photocatalytic hydrogen evolution reaction (HER) is a very promising and sustainable technology, yet precisely exploring effective HER photocatalysts remains critical challenge due to the rapid charge recombination. In this work, brand‐new S‐scheme heterojunction successfully designed constructed by in situ growth of twinned Zn 0.5 Cd S Solid Solution (CZS) on novel fluorenone‐based covalent triazine framework (FOCTF). The heterojunctions identified via irradiation XPS, electron spin resonance, which can greatly improve photocatalytic rate stability. Under illumination, highest well‐designed CZS‐FOCTF 247.62 mmolg −1 h , 3.83 times as high that pure CZS. Experimental theoretical investigations corroborate new FOCTF has well‐matched staggered band alignment work function difference with as‐fabricated establish favorable internal electric field, accelerates directional migration, thereby enhancing separation utilization efficiency carriers. This finding achieves spatially oriented powerful transport at interfaces inorganic–organic hybrid heterojunctions. It thus desirable furnish an alternative strategy rationally design CZS‐based based organic oxidation semiconductors for diversified reactions.

Language: Английский

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Upgrading Single S-Scheme Heterojunction to Multi-S-Scheme Ones for Better Synergy of Photocatalytic CO₂ Reduction and H₂O Oxidation: The Third Component Location Matters

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(16), P. 12529 - 12540

Published: Aug. 6, 2024

Upgrading single S-scheme heterojunctions to multi-S-scheme ones through implanting another component provides a promising means of simultaneously optimizing the charge transport dynamics and surface reaction kinetics, which, however, is challenged by uncontrollable loading position third component. Herein, component-directed growth strategy implemented for deliberate deposition ZnIn2S4 onto diverse locations In2O3/CdS, constructing twin triple heterojuctions with distinct transfer pathways. The photocatalytic performances as-synthesized ternary in CO2 reduction coupled H2O oxidation strongly correlate location ZnIn2S4. selective coating CdS expedites separation, ensures large-area exposure In2O3 smooth oxidation, modulates energy barriers promoted CO2-to-CO transformation while suppressing side H2 evolution, raises electron density proton supply methanation. Consequently, In2O3/CdS@ZnIn2S4 achieves optimum activities selectivities CO CH4 production, along nearly stoichiometric O2 evolution. This work not only offers valuable insights rational design three-component heterojunction photocatalysts multiple pathways but also opens up fresh avenue precisely regulate enhancing overall efficiency photoredox catalysis.

Language: Английский

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Highly efficient nitrogen fixation over S-scheme heterojunction photocatalysts with enhanced active hydrogen supply

National Science Review, Journal Year: 2024, Volume and Issue: 11(5)

Published: March 8, 2024

ABSTRACT Photocatalytic N2 fixation is a promising strategy for ammonia (NH3) synthesis; however, it suffers from relatively low yield due to the difficulty in design of photocatalysts with both high charge transfer efficiency and desirable adsorption/activation capability. Herein, an S-scheme CoSx/ZnS heterojunction dual active sites designed as efficient photocatalyst. The exhibits unique pocket-like nanostructure small ZnS nanocrystals adhered on single-hole CoSx hollow dodecahedron. Within heterojunction, electronic interaction between creates electron-deficient Zn enhanced chemisorption electron-sufficient Co hydrogen supply hydrogenation, cooperatively reducing energy barrier activation. In combination promoted photogenerated electron-hole separation facilitated mass by nanostructure, excellent performance NH3 1175.37 μmol g−1 h−1 achieved. This study provides new insights into fixation.

Language: Английский

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Construction of COF/COF Organic S‐Scheme Heterostructure for Enhanced Overall Water Splitting

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 18, 2024

Covalent organic frameworks (COFs) as a new type of photocatalysts have shown unique advantages in visible-light-driven hydrogen evolution, while the reported overall water-splitting systems are still very rare among various COF-based photocatalysts. Herein, two COFs integrated to construct S-scheme heterojunction for improved water splitting. In this system, TpBpy-COF and COF-316 serve H

Language: Английский

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Nanoarchitectonics of S‐Scheme Heterojunction Photocatalysts: A Nanohouse Design Improves Photocatalytic Nitrate Reduction to Ammonia Performance

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(38)

Published: June 25, 2024

Photocatalytic nitrate reduction reaction (NitRR) is a promising route for environment remediation and sustainable ammonia synthesis. To design efficient photocatalysts, the recently emerged nanoarchitectonics approach holds great promise. Here, we report nanohouse-like S-scheme heterjunction photocatalyst with high photocatalytic NitRR performance. The nano-house has floor of plate-like metal organic framework-based (NH

Language: Английский

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Boosted photocatalytic hydrogen evolution of S-scheme N-doped CeO2-δ@ZnIn2S4 heterostructure photocatalyst

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 669, P. 430 - 443

Published: May 1, 2024

Language: Английский

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Synergistic electric fields induced by unilateral doping modulation for enhanced organic pollutant degradation and sterilization

Applied Surface Science, Journal Year: 2025, Volume and Issue: unknown, P. 162711 - 162711

Published: Feb. 1, 2025

Language: Английский

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