Interfacial Chemical Bond and Oxygen Vacancy‐Enhanced In₂O₃/CdSe‐DETA S‐scheme Heterojunction for Photocatalytic CO₂ Conversion

Advanced Functional Materials, Год журнала: 2023, Номер 33(23)

Опубликована: Март 2, 2023

Abstract The S‐scheme heterojunctions have great potential for photocatalytic carbon dioxide reduction due to their unique carrier migration pathways, superior separation efficiencies, and high redox capacities. However, the precise process of oriented powerful electron transport remains a challenge. Herein, an InOCd bond‐modulated heterojunction In 2 O 3 /CdSe‐DETA is synthesized by simple microwave‐assisted hydrothermal method accelerated photogenerated transfer. Meanwhile, oxygen vacancies (Vo) capture effect. Consequently, thanks synergistic effect this In‐Vo‐In‐O‐Cd structural units at interface, electrons are extracted rapidly transferred surface‐active sites, which improves electronic coupling CO . This finding precisely adjusts transfer pathway shortens distance. chemical bond established in heterostructure with (Vo‐In ) provides new insights into reduction.

Язык: Английский

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A S‐Scheme MOF‐on‐MOF Heterostructure

Advanced Functional Materials, Год журнала: 2023, Номер 33(20)

Опубликована: Фев. 20, 2023

Abstract Constructing MOF‐on‐MOF heterojunction with elaborate charge transfer mechanism and interface is a promising strategy for improving the photocatalytic properties of MOFs. Herein, Step‐scheme (S‐scheme) MIL‐125‐NH 2 @CoFe Prussian blue analogue (PBA) reported first time. The heterostructure exhibits sandwich‐like morphology hollow CoFe PBA nanocages selectively assembled on top‐down surfaces nanocakes. Experimental findings theoretical simulation results reveal formation internal electric field via interfacial TiOCo bonds at heterojunction, providing driving force atomic transportation highway accelerating S‐scheme enhancing redox performance. Contributed further by structures increased active site exposure, designed significantly enhanced activity degradation various organic pollutants. This study provides insights toward rational design semiconducting MOF‐based heterojunctions improved properties.

Язык: Английский

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Hierarchically Ordered Macro–Mesoporous Electrocatalyst with Hydrophilic Surface for Efficient Oxygen Reduction Reaction

Advanced Materials, Год журнала: 2023, Номер 35(30)

Опубликована: Апрель 18, 2023

Metal-organic frameworks (MOFs) offer versatile templates/precursors to prepare supported metal catalysts. However, the afforded catalysts usually exhibit microporous structures and unsuitable wettability, which will restrict accessibility of active sites in liquid-phase reactions. Herein, an etching-functionalization strategy is developed for construction a tannic-acid-functionalized MOF with unique hollow-wall 3D-ordered macroporous (H-3DOM) structure. The functional can be further employed as ideal precursor synthesis cobalt on oxygen/nitrogen-co-doped carbon composites H-3DOM structures, hydrophilic surface. structure improve external surface area maximize exposure sites. Moreover, oxygen-containing groups enhance wettability guarantee more electrochemically accessible aqueous electrolyte. Benefitting from these outstanding characteristics, H-3DOM-Co/ONC exhibits high electrocatalytic activity oxygen reduction reaction, superior its counterparts without hierarchically ordered functionalization.

Язык: Английский

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Modulating the Reaction Configuration by Breaking the Structural Symmetry of Active Sites for Efficient Photocatalytic Reduction of Low‐concentration CO₂

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(42)

Опубликована: Авг. 29, 2023

Photocatalytic conversion of low-concentration CO2 is considered as a promising way to simultaneously mitigate the environmental and energy issues. However, weak adsorption tough activation process seriously compromise CO production, due chemical inertness molecule formed fragile metal-C/O bond. Herein, we designed fabricated oxygen vacancy contained Co3 O4 hollow nanoparticles on ordered macroporous N-doped carbon framework (Vo-HCo3 /OMNC) towards photoreduction . In situ spectra ab initio molecular dynamics simulations reveal that constructed able break local structural symmetry Co-O-Co sites. The formation asymmetric active site switches configuration from single-site linear model multiple-sites bending one with highly stable configuration, enhancing binding polarization molecules. As result, Vo-HCo3 /OMNC shows unprecedent activity in photocatalytic (10 % /Ar) under laboratory light source or even natural sunlight, affording syngas yield 337.8 95.2 mmol g-1 h-1 , respectively, an apparent quantum up 4.2 %.

Язык: Английский

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Highly selective photocatalytic CO₂reductionviaa lead-free perovskite/MOF catalyst

Journal of Materials Chemistry A, Год журнала: 2023, Номер 11(8), С. 4020 - 4029

Опубликована: Янв. 1, 2023

A lead-free perovskite/MOF catalyst shows a high CO selectivity of 99.5% for photocatalytic 2 reduction, stemming from efficient charge separation, formation *COOH intermediates, and prompt desorptionof the catalyst.

Язык: Английский

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Construction of Single Ni Atom-Immobilized ZIF-8 with Ordered Hierarchical Pore Structures for Selective CO₂ Photoreduction

ACS Catalysis, Год журнала: 2023, Номер 13(10), С. 6630 - 6640

Опубликована: Май 1, 2023

The rational construction of single-atom-modified porous metal–organic frameworks (MOFs) for efficient CO2 photoconversion is a promising avenue, yet the one that poses significant challenge. In this study, we demonstrate successful Ni single-atom-immobilized ZIF-8 with an ordered hierarchical (macro–micro) pore structure highly photocatalytic reduction to CO. interpenetrated macroporous in microporous built up by employing polystyrene (PS) opal as hard template, while high stability framework achieved through double-solvent-induced crystallization. enables rapid mass transport and strong adsorption CO2, single atoms active sites electron-trapping optimize reaction energy hinder competitive H2 evolution. As result, achieves activity 4.2 mmol g–1 h–1 CO yield electronic selectivity 94%, which shows 47-fold ZIF-8. This work highlights significance constructing MOFs single-atom-active improve photoreduction realizing carbon neutralization.

Язык: Английский

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Manipulating the d-band center enhances photoreduction of CO2 to CO in Zn2GeO4 nanorods

Chemical Engineering Journal, Год журнала: 2023, Номер 468, С. 143569 - 143569

Опубликована: Май 26, 2023

Язык: Английский

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Recent advances in tailoring zeolitic imidazolate frameworks (ZIFs) and their derived materials based on hard template strategy for multifunctional applications

Coordination Chemistry Reviews, Год журнала: 2023, Номер 498, С. 215464 - 215464

Опубликована: Окт. 10, 2023

Язык: Английский

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Solar-Driven Highly Effective Biomass-Derived Alcohols C–C Coupling Integrated with H₂ Production by CdS Quantum Dots Modified Zn₂In₂S₅ Nanosheets

ACS Catalysis, Год журнала: 2024, Номер 14(7), С. 4581 - 4592

Опубликована: Март 12, 2024

The integration of solar-driven H2 evolution with the selective conversion biomass-derived alcohols into value-added chemicals has gained significant attention for full use electrons and holes. We develop a dual-functional photocatalyst highly oxidation Cα–H bond benzyl alcohol to C–C coupled products (hydrobenzoin deoxybenzoin), in cooperation evolution, using point-to-face interface engineering by decorating CdS quantum dots on Zn2In2S5 nanosheets (CdS QDs/Zn2In2S5 NS). NS exhibit high rate 13 mmol g–1 h–1 formation 10.8 96.3% selectivity. Benzyl achieves 91% an 89% yield gram-scale. introduction enhances interfacial contact, facilitating efficient spatial separation photogenerated electron–hole pairs providing active sites evolution. In situ characterization DFT calculation reveal that carbon-centered radical •CH(OH)C6H5, generated abstracting alcohol, is reactive intermediate photocatalytic process.

Язык: Английский

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Asymmetric Atomic Dual‐Sites for Photocatalytic CO₂ Reduction

Advanced Materials, Год журнала: 2024, Номер 36(38)

Опубликована: Июль 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.

Язык: Английский

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