Atomic-level design of metalloenzyme-like active pockets in metal–organic frameworks for bioinspired catalysis

Chemical Society Reviews, Год журнала: 2023, Номер 53(1), С. 137 - 162

Опубликована: Ноя. 29, 2023

Natural metalloenzymes with astonishing reaction activity and specificity underpin essential life transformations. Nevertheless, enzymes only operate under mild conditions to keep sophisticated structures active, limiting their potential applications. Artificial that recapitulate the catalytic of can not circumvent enzymatic fragility but also bring versatile functions into practice. Among them, metal-organic frameworks (MOFs) featuring diverse site-isolated metal sites supramolecular have emerged as promising candidates for move toward unparalleled properties behaviour enzymes. In this review, we systematically summarize significant advances in MOF-based metalloenzyme mimics a special emphasis on active pocket engineering at atomic level, including primary secondary coordination spheres. Then, deep understanding mechanisms advanced applications are discussed. Finally, perspective emerging frontier research is provided advance bioinspired catalysis.

Язык: Английский

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Chiral Linker Installation in a Metal–Organic Framework for Enantioselective Luminescent Sensing

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(22), С. 15446 - 15452

Опубликована: Май 22, 2024

Linker installation is a potent strategy for integrating specific properties and functionalities into metal–organic frameworks (MOFs). This method enhances the structural diversity of enables precise construction robust structures, complementing conventional postsynthetic modification approaches, by fully leveraging open metal sites active organic linkers at targeting locations. Herein, we demonstrated an insertion d-camphorate linker flexible Zr-based MOF, PCN-700, through installation. The resultant homochiral MOF not only exhibits remarkable stability but also functions as highly efficient luminescent material enantioselective sensing. Competitive absorption energy/electron transfer processes contribute to sensing performance, while difference in binding affinities dominates enantioselectivity. work presents straightforward route crafting stable MOFs

Язык: Английский

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On–Off Ratiometric Fluorescence Europium(III) Metal–Organic Framework for Quantitative Detection of the Inflammatory Marker Neopterin

Inorganic Chemistry, Год журнала: 2024, Номер 63(10), С. 4697 - 4706

Опубликована: Фев. 26, 2024

Benefiting from the unique photoluminescence behavior of lanthanide(III) ions and organic ligands, a metal-organic framework (Ln-MOF) material can simultaneously demonstrate cations molecules endow its superior applications fluorescence sensing behaviors. Herein, we present europium(III) MOF {[Eu

Язык: Английский

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Bacterial Cellulose–Based MOF Hybrid as a Sensitive Switch Off–On Luminescent Sensor for the Selective Recognition of l-Histidine

Inorganic Chemistry, Год журнала: 2024, Номер 63(7), С. 3560 - 3571

Опубликована: Фев. 8, 2024

In this study, a stable and luminescent UiO-66-NH2 (UN) its derivative Cu2+@UN were prepared utilized successfully as an Off–On sensing platform for effective, selective, well rapid (5 min) detection of l-Histidine (l-His). The UN reveals efficient quenching in the presence Cu2+ ions through photoinduced electron transition (PET) mechanism dynamic process (in range 0.01–1 mM) forming platform. However, due to remarkable affinity between l-His Cu2+, luminescence is recovered indicating Turn-On behavior via quencher detachment (QD). A good linear relationship concentration intensity was observed 0.01–40 μM (R2 = 0.9978) with limit 7 nM sensing. suggested method determination real samples recoveries satisfying consequences. Moreover, result indicates that only induces significant restoration signal significantly greater than other amino acids. Also, portable test paper based on bacterial cellulose (BC) Cu2+@UNBC developed conveniently evaluate effective l-His.

Язык: Английский

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Development of the design and synthesis of metal–organic frameworks (MOFs) – from large scale attempts, functional oriented modifications, to artificial intelligence (AI) predictions

Chemical Society Reviews, Год журнала: 2024, Номер unknown

Опубликована: Ноя. 25, 2024

The design and synthesis of MOFs have evolved from traditional large-scale approaches to function-oriented modifications, recently AI predictions, which save time, reduce costs, enhance the efficiency achieving target functions.

Язык: Английский

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Brain-specific targeted delivery of therapeutic agents using metal–organic framework-based nanomedicine

Coordination Chemistry Reviews, Год журнала: 2024, Номер 514, С. 215926 - 215926

Опубликована: Май 9, 2024

Язык: Английский

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Achieving On–Off Ratiometric Luminescence Dynamics in a Nanoporous Eu(III) Metal–Organic Framework for Neopterin Detection

ACS Applied Nano Materials, Год журнала: 2024, Номер 7(15), С. 17748 - 17758

Опубликована: Июль 30, 2024

Thanks to the superior photoluminescence performance of lanthanide(III) ions sensitized by organic ligands via an "antenna effect" and host–guest interactions between a MOF material targeted analytes, nanoporous can achieve luminescence dynamics through influence thus endowing with ratiometric sensing application. Consequently, 3D Eu(III) based material, {[Eu(BPDC)(μ3–OH)(H2O)]·H2O·DMF}n (Eu-MOF, 2,2′-bipyridine-4,4′-dicarboxylic acid = H2BPDC), assembled H2BPDC ligand Eu3+ for achieving on–off inflammatory marker neopterin (Neo) detection, has been fabricated. The Eu-MOF is consist 1D Eu(μ3–OH) chains, which could further be connected deprotonated build framework, showing nanosized aperture ca. 12.6 Å × along a-direction. titration experiments demonstrate that exhibit simultaneous behavior Neo, regulating interactions. More importantly, visible color change observation from red bluish violet naked eyes in response concentrations Neo indicator facile achieved luminescent test strips portable hydrogels. A combination competitive absorption contribute confirmed UV–vis spectral overlap experiment density functional theory calculations.

Язык: Английский

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Sequential Linker Installation in Metal–Organic Frameworks

Accounts of Chemical Research, Год журнала: 2024, Номер 57(21), С. 3217 - 3226

Опубликована: Окт. 16, 2024

ConspectusMetal–organic frameworks (MOFs) represent a sophisticated blend of inorganic and organic components, promoting the development coordination chemistry greatly offering versatile platform for tailored functionalities. By combining various metal nodes, linkers, functional guests, MOFs provide numerous pathways their design, synthesis, customization. Among these, sequential linker installation (SLI) stands out as novel crucial strategy, enabling precise integration desired properties functions at atomic scale. SLI enhances structural diversity stability while facilitating meticulous construction robust by leveraging open sites linkers targeted locations. Compared to direct synthesis MOFs, postsynthetic modification methods allow regulation structures corresponding properties. While unlike conventional methods, requires careful selection framework design ensure positioning installation, which gives rise well-designed ordered positions installed confirmed directly X-ray diffraction technology.Recent advancements in MOF have led creation increasingly flexible matrix structures, particularly due diverse connection modes multicore clusters, especially Zr6 cluster. The spatial hindrance certain ligands has resulted formation unsaturated clusters missing pockets. Examples these advanced include PCN-606, PCN-608, PCN-609, PCN-700, PCN-808, feature specific flexibility conducive SLI. Strategically positioned within serve predetermined anchor points molecules, frameworks' can accommodate molecules varying sizes extent, enlarging scopes application greatly. This groups enables enhanced applications, such adsorption, catalysis, recognition.In this Account, we delve into intricate process designing synthesizing with appropriate missing-linker pockets aforementioned applications. We discuss used insert them MOFs. Additionally, explore functionalities resulting focusing on adsorptive, catalytic, recognition performance. Furthermore, insights future trajectory complemented our recent works. Account not only reviews evolution method but also underscores its practical applications across domains, paving rational pathway multifunctional through method.

Язык: Английский

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Designing homochiral metal-organic frameworks with ultrahigh surface areas and stability for practical applications

Science Bulletin, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

Язык: Английский

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Indirect Construction of Chiral Metal–Organic Frameworks for Enantioselective Luminescence Sensing

Accounts of Chemical Research, Год журнала: 2025, Номер unknown

Опубликована: Фев. 2, 2025

ConspectusChiral metal-organic frameworks (MOFs) are promising candidates as luminescent sensing materials for chiral species, which essential components in modern industries, pharmaceuticals, and biological processes. The discrimination of enantiomers with highly similar physical chemical properties is crucial because they often present concurrently the same system but may feature distinct effects on living matters. While rapid precise capabilities MOFs outshine traditional detection methods species daily life, production, natural environment, it requires well-matched electronic structures between species. Yet, conventional strategies to construct immensely challenging due crystallization difficulties based low-symmetric building blocks.Recent advancements MOF chemistry have led novel pathways synthesizing enantioselective sensing. Compared direct synthesis using optically pure ligands, usually complex costly, indirect has garnered significant attention reduced costs, simplified synthesis, enhanced material stability, broad application scope. In past few years, our group developed guest ion exchange, coordination modification, defect engineering indirectly MOFs. exchange cost-effective introducing ions into pores can be applied only charged frameworks. addition, also faces limitations availability tendency toward chirality loss during process. Besides, compared modification maintain stability stronger bonds. Still, accessible open metal sites that bind disordered dangling molecules, complicating structural determination. Therefore, specific such linker installation dual-end been afford well-defined crystal structures. all aforementioned decrease MOFs' pore sizes a certain degree, we further approach enlarge size introduce center simultaneously. Such competitive strategy facile low-cost expanded many well-known stable MOFs.In this Account, delve intricate evolution constructing tailored applications. We provide detailed analysis progression innovation within field, tracing development MOF-based luminescence sensors. By systematically reviewing various synthetic approaches, work highlights their respective strengths limitations. Beyond state art, Account offers forward-looking insights aiming inspire design next-generation These advanced hold promise versatile impactful applications across beyond.

Язык: Английский

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