In Situ Growth of Cs₃Bi₂Br₉ Quantum Dots on Bi-MOF Nanosheets via Cosharing Bismuth Atoms for CO₂ Capture and Photocatalytic Reduction

Inorganic Chemistry, Год журнала: 2023, Номер 62(5), С. 2289 - 2303

Опубликована: Янв. 24, 2023

Given the global warming caused by excess CO2 accumulation in atmosphere, it is essential to reduce capturing and converting chemical feedstock using solar energy. Herein, a novel Cs3Bi2Br9/bismuth-based metal-organic framework (Bi-MOF) composite was prepared via an situ growth strategy of Cs3Bi2Br9 quantum dots (QDs) on surface Bi-MOF nanosheets through coshared bismuth atoms. The Cs3Bi2Br9/Bi-MOF exhibits bifunctional merits for both high capture effective conversion CO2, among which optimized 3Cs3Bi2Br9/Bi-MOF sample shows CO2-CO yield as 572.24 μmol g-1 h-1 under irradiation 300 W Xe lamp. In addition, good stability after five recycles humid air, photoreduction efficiency does not decrease significantly. mechanistic investigation uncovers that intimate atomic-level contact between atoms only improves dispersion QDs over but also accelerates interfacial charge transfer forming strong bonding linkage, endows with best performance photoreduction. Our new finding bismuth-based framework/lead-free halide perovskite cosharing opens avenue preparation heterojunction potential applications photocatalytic CO2.

Язык: Английский

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Isolated Single-Atom Cobalt in the ZnIn₂S₄ Monolayer with Exposed Zn Sites for CO₂ Photofixation

ACS Catalysis, Год журнала: 2023, Номер 13(12), С. 8317 - 8329

Опубликована: Июнь 7, 2023

Constructing highly active photocatalysts with rich reactive sites for photofixation of CO2 organic compounds implements an environmentally friendly route valorization and carbon neutralization. Herein, we report the isolated cobalt (Co) single-atom (SA)-decorated two-dimensional (2D) single-layer ZnIn2S4 (ZIS) nanosheet composites (Co-sZIS) dual centers Co Zn fixation epoxides under visible light. The unique ensemble Co-sZIS optimizes light harvesting, promotes charge carrier separation, enriches bifunctional efficient adsorption activation reactants CO2. Consequently, exhibits significantly improved CO2-epoxide cycloaddition performance compared to bulk ZIS. In addition, synergetic photoredox manner simultaneously exploiting photogenerated electrons holes efficiently facilitates epoxides, thereby further reducing energy barrier fixation. This work not only provides a paradigm rationally interfacial engineered SA-onto-2D semiconductors but also highlights structure–activity relationship by well-defined in this SA-based hybrid platform.

Язык: Английский

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Halide perovskite quantum dots for photocatalytic CO₂reduction

Journal of Materials Chemistry A, Год журнала: 2023, Номер 11(24), С. 12482 - 12498

Опубликована: Янв. 1, 2023

This review focuses on halide perovskite quantum dots (QDs) for photocatalytic CO 2 reduction, discussing the structures and properties of QDs, mechanism photocatalyst design, challenges directions future research.

Язык: Английский

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Accumulation of Long‐Lived Photogenerated Holes at Indium Single‐Atom Catalysts via Two Coordinate Nitrogen Vacancy Defect Engineering for Enhanced Photocatalytic Oxidation

Advanced Materials, Год журнала: 2024, Номер 36(28)

Опубликована: Май 11, 2024

Visible-light-driven photocatalytic oxidation by photogenerated holes has immense potential for environmental remediation applications. While the electron-mediated photoreduction reactions are often at spotlight, active possess a remarkable capacity that can degrade recalcitrant organic pollutants, resulting in nontoxic byproducts. However, random charge transfer and rapid recombination of electron-hole pairs hinder accumulation long-lived reaction center. Herein, novel method employing defect-engineered indium (In) single-atom photocatalysts with nitrogen vacancy (Nv) defects, dispersed carbon nitride foam (In-Nv-CNF), is reported to overcome these challenges make further advances photocatalysis. This Nv strategy produces extension lifetime an increase concentration In-Nv-CNF. Consequently, optimized In-Nv-CNF demonstrates 50-fold photo-oxidative degradation rate compared pristine CN, effectively breaking down two widely used antibiotics (tetracycline ciprofloxacin) under visible light. The contaminated water treated completely based on growth Escherichia coli. Structural-performance correlations between defect engineering hole established validated through experimental theoretical agreement. work elevate efficiency overall from hole-centric standpoint.

Язык: Английский

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Rational Design of S‐Scheme Heterojunction toward Efficient Photocatalytic Cellulose Reforming for H₂ and Formic Acid in Pure Water

Advanced Materials, Год журнала: 2023, Номер 36(4)

Опубликована: Окт. 9, 2023

Abstract Photocatalytic cellulose reforming usually requires harsh conditions due to its sluggish kinetics. Here, a hollow structural S‐scheme heterojunction of ZnSe and oxygen vacancy enriched TiO 2 , namely, h‐ZnSe/Pt@TiO is designed fabricated, with which the photocatalytic for H formic acid realized in pure water. productivity 1858 372 µmol g −1 h steady evolution 300 are achieved α‐cellulose. Comparable activity can also be using various sources. It experimentally proven that photogenerated charge transfer follows an mechanism, not only promotes separation but preserves higher reductive oxidative abilities respectively. Furthermore, polyhydroxy species produced during degradation favored adsorb on surface, process accounted preservation as major solution‐phase product. In addition, sequential reactions oxidation aldehydes elimination revealed. This work provides strategy sustainably produce hydrogen value‐added chemicals from biomass under most environmentally benign condition, i.e.,

Язык: Английский

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Photo-thermal coupling to enhance CO2 hydrogenation toward CH4 over Ru/MnO/Mn3O4

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

Опубликована: Фев. 6, 2024

Upcycling of CO

Язык: Английский

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Circumventing bottlenecks in H2O2 photosynthesis over carbon nitride with iodine redox chemistry and electric field effects

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

Опубликована: Июнь 3, 2024

Abstract Artificial photosynthesis using carbon nitride (g-C 3 N 4 ) holds a great promise for sustainable and cost-effective H 2 O production, but the high carrier recombination rate impedes its efficiency. To tackle this challenge, we propose an innovative method involving multispecies iodine mediators (I − /I intercalation through pre-photo-oxidation process potassium iodide (suspected deteriorated “KI”) within g-C framework. Moreover, introduce external electric field by incorporating cationic methyl viologen ions to establish auxiliary electron transfer channel. Such unique design drastically improves separation of photo-generated carriers, achieving impressive production 46.40 mmol g −1 h under visible light irradiation, surpassing most visible-light -producing systems. Combining various advanced characterization techniques elucidates inner photocatalytic mechanism, application potential system is validated with simulation scenarios. This work presents significative strategy preparing applying highly efficient -based catalysts in photochemical production.

Язык: Английский

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Lattice Match‐Enabled Covalent Heterointerfaces with Built‐in Electric Field for Efficient Hydrogen Peroxide Photosynthesis

Advanced Materials, Год журнала: 2024, Номер unknown

Опубликована: Окт. 20, 2024

Crafting semiconducting heterojunctions represents an effective route to enhance photocatalysis by improving interfacial charge separation and transport. However, lattice mismatch (δ) between different semiconductors can significantly hinder dynamics. Here, meticulous tailoring is reported create a covalent heterointerface with built-in electric field (BIEF), imparting markedly improved hydrogen peroxide (H

Язык: Английский

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Regulating *COOH intermediate via amino alkylation engineering for exceptionally effective photocatalytic CO2 reduction

Journal of Energy Chemistry, Год журнала: 2024, Номер 92, С. 282 - 291

Опубликована: Янв. 25, 2024

Язык: Английский

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Enabling CsPbBr₃ Perovskites for Photocatalytic CO₂ Methanation by Rationalizing a Z-Scheme Heterojunction with Zinc Phthalocyanine

ACS Materials Letters, Год журнала: 2024, Номер 6(3), С. 999 - 1006

Опубликована: Фев. 16, 2024

Perovskite materials are regarded as promising photocatalysts for light harvesting, yet they exhibit low photocatalytic activity due to serious charge recombination and lack of efficient catalytic sites toward CO2 reduction. Previous studies have employed perovskites reductive sides in a Z-scheme heterojunction suppress recombination, which however still encounter selectivity because the absence specific In this work, we report strategy that enables CsPbBr3 perovskite methanation. The central concept is construction using zinc phthalocyanine (ZnPc) side. enhanced separation CsPbBr3/ZnPc provides catalytically active ZnPc with sufficient energetic electrons As result, achieves up 89% 168 μmol g–1 h–1 CH4 production, well exceeding all reported perovskite-based photocatalysts. This work insights into rational design heterojunctions artificial photosynthesis.

Язык: Английский

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