Multicomponent, Multicavity Metallacages That Contain Different Binding Sites for Allosteric Recognition

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(23), С. 15787 - 15795

Опубликована: Май 13, 2024

The encapsulation of different guest molecules by their recognition domains proteins leads to selective binding, catalysis, and transportation. Synthetic hosts capable selectively binding guests in cavities mimic the function are highly desirable but challenging. Here, we report three ladder-shaped, triple-cavity metallacages prepared multicomponent coordination-driven self-assembly. Interestingly, porphyrin-based metallacage is heteroleptic fullerenes (C60 or C70) coronene using its cavities, allowing distinct allosteric upon addition C60 C70. Owing affinities one molecule central cavity two units side while encapsulating C70 cavity. rational design multicavity assemblies that enable will guide further advanced supramolecular constructs with tunable properties.

Язык: Английский

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Chemo-Selective Transformation of Anthracene Derivative within Water-Soluble Coordination Cages Having Different Cavities

Inorganic Chemistry, Год журнала: 2025, Номер unknown

Опубликована: Март 12, 2025

Coordination cages with specific properties and functionalities are utilized as reaction vessels for the desired chemical transformation of substrates. The symmetry inherent cavity coordination can influence host–guest interactions outcome in their confined space. However, impact cage shape on different transformations remains unclear. In this chapter, we report chemo-selective anthracene derivative using three geometrically distinct Pd6 (CC2, CC3, CC4). Photoirradiation 9-bromoanthracene (G3) distorted double-square (CC2) yields anthracene-9,10-dione, while known (CC3) forms a [4 + 4] cycloaddition product. same bowl-shaped (CC4) resulted oxidized Through combination experimental computational studies, demonstrate that size significantly pathways encapsulated derivative, leading to chemo-selectivity. Furthermore, observe encapsulation cavities (CC2 CC4) leads significant enhancement rate photooxidation G3. This work underscores versatility water-soluble synthetic chemistry, offering interesting avenues transformation.

Язык: Английский

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Confining polyoxometalates in porphyrin-based porous cationic polymer toward boosting visible-light-driven synthesis of sulfoxides and detoxification of mustard gas simulants

Journal of Catalysis, Год журнала: 2024, Номер 436, С. 115627 - 115627

Опубликована: Июль 1, 2024

Язык: Английский

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Sustainable scalable solid-state synthesis of highly efficient synergetic 2D/0D micro/nanostructured g-C3N4/CdS photocatalysts for hydrogen production and water purification

Sustainable materials and technologies, Год журнала: 2024, Номер 41, С. e01063 - e01063

Опубликована: Июль 27, 2024

Язык: Английский

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Selective heterogeneous photocatalytic activation for toluene oxidation: recent advances, challenges and perspective

Chemical Synthesis, Год журнала: 2025, Номер 5(1)

Опубликована: Фев. 8, 2025

The conversion of toluene into high-value products without generating undesired CO2 remains a critical challenge. Selective oxidation under visible light irradiation has emerged as promising solution. This review offers comprehensive interpretation photocatalytic transformations in heterogeneous oxidation. We start by outlining the basic mechanism C–H bond activation and provide an overview reactive oxygen species (ROS) within systems. Subsequently, we summary strategies that have been developed to enhance selectivity system. Following this, advanced characterization techniques density functional theory (DFT) calculations are discussed for understanding structure-performance relationship photocatalysts mechanisms underlying processes. Finally, put forward detailed discussion current challenges potential directions future research, with aim offering valuable insights this emerging field. believe will not only spark greater creativity optimizing but also offer designing other

Язык: Английский

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Low-Voltage Electrooxidation of Benzyl Alcohol to Benzoic Acid Enhanced by PtZn-ZnO_x Interface

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Март 11, 2025

The electrocatalytic oxidation of benzyl alcohol to benzoic acid is a process that often requires high voltage, leading increased energy consumption, side reactions (oxygen evolution reaction (OER)), and catalyst degradation. Herein, our study introduces novel approach. We demonstrate PtZn-ZnOx featuring PtZn intermetallic structure with abundant interfaces on the surface allows for an impressive selectivity 99.5% at low potential 0.725 V (vs reversible hydrogen electrode, RHE), which 0.6 lower than most reported studies. This testament efficiency catalyst, as it significantly reduces occurrence reactions, more efficient sustainable process. experimental density functional theory calculations demonstrated adsorption Ph–CH2OH Ph–CHO generation electrophilic OH* were promoted due unsaturated coordination Zn atom in interfaces. Furthermore, potential-determining step coupling was barrier interface, improved catalytic activity selectivity. outlines approach designing highly electrocatalysts high-efficiency valorization voltages.

Язык: Английский

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Metal‐Organic Frameworks (MOFs) and Metal‐Organic Cages (MOCs) for Photocatalytic Hydrogen Production

Chemistry - A European Journal, Год журнала: 2024, Номер 30(43)

Опубликована: Май 29, 2024

Abstract Metal‐organic frameworks (MOFs) and metal‐organic cages (MOCs) have garnered significant attention as promising photocatalysts due to their tunable chemical structures integrated multifunctionality. To increase the photocatalytic efficiency, strategies like ligand functionalization, introducing additional catalytic sites, doping or encapsulating photosensitizers been explored for both MOFs MOCs. This concept review focuses on recent advancements in utilizing MOCs hydrogen production, highlighting unique characteristics respective mechanisms this field. Moreover, it outlines current challenges prospects faced by MOCs, offering an outlook future domain.

Язык: Английский

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Tetraphenylethene-Based Molecular Cage with Coenzyme FAD: Conformationally Isomeric Complexation toward Photocatalysis-Assisted Photodynamic Therapy

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(45), С. 30933 - 30946

Опубликована: Окт. 21, 2024

Flavin adenine dinucleotide (FAD), serving as a light-absorbing coenzyme factor, can undergo conformationally isomeric complexation within different enzymes to form various enzyme-coenzyme complexes, which exhibit photocatalytic functions that play crucial role in physiological processes. Constructing an artificial photofunctional system using FAD or its derivatives not only develop biocompatible systems with excellent activities but also further enhance our understanding of the biological systems. Here, we demonstrate supramolecular approach for constructing enzyme-coenzyme-type host-guest complex photoinduced catalytic function water. First, have designed and synthesized water-soluble tetraphenylethene (TPE)-based octacationic molecular cage (

Язык: Английский

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High-order layered self-assembled multicavity metal–-organic capsules and anti-cooperative host–multi-guest chemistry

Chemical Science, Год журнала: 2024, Номер 15(23), С. 8913 - 8921

Опубликована: Янв. 1, 2024

The construction and application of metal-organic cages with accessible internal cavities have witnessed rapid development, however, the precise synthesis complex capsules multiple achievement multi-guest encapsulation, further in-depth comprehension host-multi-guest recognition remain a great challenge. Just like building LEGO blocks, herein, we constructed series high-order layered architectures generation n (n = 1/2/3/4 is also number cavities) by multi-component coordination-driven self-assembly using porphyrin-containing tetrapodal ligands (like plates), parallel-podal clamps) metal ions nodes). Importantly, these assembled structures possessed different numbers rigid separate formed overlapped porphyrin planes specific gaps. host-guest experiments convincing characterization proved that G2-G4 could serve as host to achieve unprecedentedly encapsulate up four C60 molecules. More interestingly, revealed negative cooperation behavior in process recognition, which provides new platform study complicated interaction field supramolecular chemistry.

Язык: Английский

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Design and synthesis of metal–organic cycles/cages (MOCs) and their applications

APL Materials, Год журнала: 2024, Номер 12(7)

Опубликована: Июль 1, 2024

Metal–organic cycles/cages (MOCs) are a class of nanoscale molecular entities that possess distinct shapes and sizes designed synthesized through the predictable integration organic inorganic ligands. The diverse functionalities MOCs render them valuable in fields biology, chemistry, materials. First, cavity renders suitable for host–guest interactions, which subsequently employed to induce conformational changes, this approach is particularly advantageous catalysis, sensing, controlled loading release. Furthermore, MOC- polymer-based aggregates can be applied biomedical research cascaded light-harvesting systems. Benefiting from high specific surface area, initial exploration MOC-based hierarchical assemblies indicates their potential applications biomedicine catalysis. microsheets centimeter films used dual-mode catalysis novel wound dressing nonhealing wounds. In addition, design synthesis with different various strategies discussed. We summarized latest progress past 5 years Review.

Язык: Английский

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