Introducing Hydrogen-Bonding Microenvironment in Close Proximity to Single-Atom Sites for Boosting Photocatalytic Hydrogen Production

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(29), С. 20391 - 20400

Опубликована: Июль 10, 2024

Inspired by enzymatic catalysis, it is crucial to construct hydrogen-bonding-rich microenvironment around catalytic sites; unfortunately, its precise construction and understanding how the distance between such sites affects catalysis remain significantly challenging. In this work, a series of metal-organic framework (MOF)-based single-atom Ru

Язык: Английский

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MOF-Based Electrocatalysts: An Overview from the Perspective of Structural Design

Chemical Reviews, Год журнала: 2025, Номер unknown

Опубликована: Фев. 18, 2025

The electrocatalytic technique, as an efficient energy storage and conversion technology, has attracted significant attention to address exhaustion environmental pollution. Usually, the activity selectivity of reactions are largely dominated by dynamic process occurring on electrocatalysts. Therefore, high-performance electrocatalysts, which can dominate pathway barrier reactions, great significance for advancement technique. Metal-organic frameworks (MOFs), emerging crystalline porous materials, present structural component advantages including well-defined structure, high surface area, large porosity, diverse components, easy tailorability, demonstrating fantastic potential precise fabrication In this Review, strategies in electrocatalysts based MOF-related materials specifically introduced from aspects catalytic site design microenvironment modulation around sites. Furthermore, representative progress achieved various applications employing MOF-based is systematically summarized, with special emphasis MOFs performance optimization. Finally, remaining challenges future perspectives further highlighted.

Язык: Английский

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Modification engineering over single-atom catalysts for efficient heterogeneous photocatalysis

Coordination Chemistry Reviews, Год журнала: 2025, Номер 529, С. 216468 - 216468

Опубликована: Янв. 21, 2025

Язык: Английский

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Recent Progress and Perspectives on Metal–Organic Framework-Based Electrode Materials for Metal-Ion Batteries and Supercapacitors

Energy & Fuels, Год журнала: 2024, Номер 38(15), С. 13796 - 13818

Опубликована: Июль 11, 2024

Язык: Английский

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Design principle and synthetic strategy for metal-organic framework composites

Composites Communications, Год журнала: 2024, Номер 48, С. 101933 - 101933

Опубликована: Май 9, 2024

Язык: Английский

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Reticular Materials for Photocatalysis

Advanced Materials, Год журнала: 2024, Номер unknown

Опубликована: Ноя. 27, 2024

Abstract Photocatalysis leverages solar energy to overcome the thermodynamic barrier, enabling efficient chemical reactions under mild conditions. It can greatly reduce reliance on traditional sources and has attracted significant research interest. Reticular materials, including metal‐organic frameworks (MOFs) covalent organic (COFs), represent a class of crystalline materials constructed from molecular building blocks linked by coordination bonds, respectively. function as heterogeneous catalysts, combining well‐defined structures high tailorability akin homogeneous catalysts. In this review, regulation light absorption, charge separation, surface in photocatalytic process through precise molecular‐level design based features reticular is elaborated. Notably, for MOFsmicroenvironment modulation around catalytic sites affects performance delved, with emphasis their unique dynamic flexible microenvironments. For COFs, inherent excitonic effects due fully nature discussed highlight strategies regulate charge‐ and/or energy‐transfer‐mediated photocatalysis. Finally, current challenges future directions field, aiming provide comprehensive understanding how be optimized enhanced photocatalysis discussed.

Язык: Английский

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Incorporation of Pd Single‐atom Sites in Perovskite with an Excellent Selectivity toward Photocatalytic Semihydrogenation of Alkynes

Angewandte Chemie International Edition, Год журнала: 2024, Номер unknown

Опубликована: Июль 27, 2024

Abstract Semihydrogenation is a crucial industrial process. Noble metals such as Pd have been extensively studied in semihydrogenation reactions, owing to their unique catalytic activity toward hydrogen activation. However, the overhydrogenation of alkenes alkanes often happens due rather strong adsorption on active phases. Herein, we demonstrate that incorporation phases single‐atom sites perovskite lattices SrTiO 3 can greatly alternate electronic structure and coordination environment facilitate desorption than further hydrogenation. Furthermore, incorporated be well stabilized without sintering by host–guest interaction with during activation H species hydrogenation reactions. As result, (Pd‐SrTiO ) exhibits an excellent time‐independent selectivity (>99.9 %) robust durability for photocatalytic phenylacetylene styrene. This strategy based will broad implications development high‐performance photocatalysts selective

Язык: Английский

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Fabrication of TiO₂/MOF Type II Heterojunction by Growth of TiO₂ on Cr-Based MOF for Enhanced Photocatalytic Hydrogen Production

Crystal Growth & Design, Год журнала: 2025, Номер unknown

Опубликована: Фев. 5, 2025

MOF-based heterojunctions can significantly enhance the efficiency of photocatalytic hydrogen production; however, construction efficient remains a formidable challenge. In this study, we successfully developed series Type II by growing TiO2 on Cr-based MOF, thereby regulating generation, separation, and transportation photogenerated charge carriers to improve evolution performance. Among these, 23%TiO2/MIL-101(Cr) photocatalyst exhibited highest production activity, achieving 884.01 μmol g–1 in just 5 h, which is 6.8 6.0 times that pure MIL-101(Cr) TiO2, respectively. Additionally, demonstrated excellent cyclic stability. Tiny particles were proven mainly deposited surface N2 sorption isotherm analyses, transmission electron microscopy (TEM), high-resolution TEM, high-angle annular dark field scanning microscopy, etc. Characterization techniques such as situ XPS confirmed formation TiO2/MIL-101(Cr) heterostructure. Band structure analysis indicates meets thermodynamic requirements for production. Furthermore, transient photocurrent measurements, electrochemical impedance analysis, photoluminescence reveal possesses superior capabilities carrier transport, resulting from kinetic perspective. This research offers valuable insights into preparation development photocatalysts

Язык: Английский

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Enhanced Selectivity of Photocatalytic CO₂ Reduction to Formate via Tailoring the Metal Site

ACS Catalysis, Год журнала: 2025, Номер unknown, С. 3000 - 3007

Опубликована: Фев. 5, 2025

Язык: Английский

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Location‐Specific Microenvironment Modulation Around Single‐Atom Metal Sites in Metal‐Organic Frameworks for Boosting Catalysis

Angewandte Chemie, Год журнала: 2024, Номер unknown

Опубликована: Ноя. 7, 2024

Abstract Despite coordination environment of catalytic metal sites has been recognized to be great importance in single‐atom catalysts (SACs), a significant challenge remains the understanding how location‐specific microenvironment higher sphere influences their catalysis. Herein, series Cu‐based SACs, namely Cu 1 /UiO‐66‐X (X=‐NO 2 , ‐H, and ‐NH ), are successfully constructed by anchoring single atoms onto Zr‐oxo clusters metal–organic frameworks (MOFs), i.e., UiO‐66‐X. The ‐X functional groups dangling on MOF linkers could regarded as remote regulate electronic properties atoms. Remarkably, they exhibit differences catalysis toward hydroboration alkynes. activity follows order /UiO‐66‐NO > /UiO‐66 /UiO‐66‐NH under identical reaction conditions, where showcases phenylacetylene conversion 92 %, ~3.5 times efficiency than that . Experimental calculation results jointly support structure is modulated microenvironment, thereby regulating product desorption promoting

Язык: Английский

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