Fine-Tuning the Micro-Environment to Optimize the Catalytic Activity of Enzymes Immobilized in Multivariate Metal–Organic Frameworks

Journal of the American Chemical Society, Год журнала: 2021, Номер 143(37), С. 15378 - 15390

Опубликована: Сен. 3, 2021

The artificial engineering of an enzyme's structural conformation to enhance its activity is highly desired and challenging. Anisotropic reticular chemistry, best illustrated in the case multivariate metal–organic frameworks (MTV-MOFs), provides a platform modify MOF's pore inner-surface with functionality variations on optimize interior environment specifically targeted property. In this study, we altered ratio linkers zeolitic imidazolate (ZIFs), subclass MOFs, MTV approach demonstrate strategy that allows us encapsulated enzyme by continuously tuning framework–enzyme interaction through hydrophilicity change pores' microenvironment. To systematically study interaction, developed component-adjustment-ternary plot (CAT) method optimal BCL revealed nonlinear correlation, first incremental then decremental, between hydrophilic linker' ratios MTV-ZIF-8. These findings indicated there spatial arrangement functional groups along three-dimensional space across ZIF-8 crystal unique sequence could structure closed-lid open-lid conformations. changes were confirmed FTIR spectra fluorescence studies. optimized BCL@ZIF-8 not only thermally chemically more stable than free solution, but also doubles catalytic reactivity kinetic resolution reaction 99% ee products.

Язык: Английский

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Atomically unveiling the structure-activity relationship of biomacromolecule-metal-organic frameworks symbiotic crystal

Nature Communications, Год журнала: 2022, Номер 13(1)

Опубликована: Фев. 17, 2022

Abstract Crystallization of biomacromolecules-metal-organic frameworks (BMOFs) allows for orderly assemble symbiotic hybrids with desirable biological and chemical functions in one voxel. The structure-activity relationship this crystal, however, is still blurred. Here, we directly identify the atomic-level structure BMOFs, using integrated differential phase contrast-scanning transmission electron microscopy, cryo-electron microscopy x-ray absorption fine techniques. We discover an obvious difference nanoarchitecture BMOFs under different crystallization pathways that was previously not seen. In addition, find significantly affects bioactivity BMOFs. This work gives important insight into synthesized scenarios, may act as a guide to engineer next-generation materials excellent functions.

Язык: Английский

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Combining a Genetically Engineered Oxidase with Hydrogen‐Bonded Organic Frameworks (HOFs) for Highly Efficient Biocomposites

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(16)

Опубликована: Янв. 17, 2022

Enzymes incorporated into hydrogen-bonded organic frameworks (HOFs) via bottom-up synthesis are promising biocomposites for applications in catalysis and sensing. Here, we explored synthetic incorporation of d-amino acid oxidase (DAAO) with the metal-free tetraamidine/tetracarboxylate-based BioHOF-1 water. N-terminal enzyme fusion positively charged module Z

Язык: Английский

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Encapsulating and stabilizing enzymes using hydrogen-bonded organic frameworks

Nature Protocols, Год журнала: 2023, Номер 18(7), С. 2032 - 2050

Опубликована: Май 17, 2023

Язык: Английский

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Enzyme hybrid nanoflowers and enzyme@metal–organic frameworks composites: fascinating hybrid nanobiocatalysts

Critical Reviews in Biotechnology, Год журнала: 2023, Номер 44(4), С. 674 - 697

Опубликована: Апрель 9, 2023

Hybrid nanomaterials have recently emerged as a new interface of nanobiocatalysis, serving host platform for enzyme immobilization. Enzyme immobilization in inorganic crystal nanoflowers and metal-organic frameworks (MOFs) has sparked the bulk scientific interest due to their superior performances. Many breakthroughs been achieved preparation various types enzyme@MOF enzyme-hybrid nanoflower composites. However, it is unfortunate that there are few reviews literature related composites improved synthesis strategies applications biotechnology. In this review, innovative synthetic discussed. Enzyme@MOF reviewed terms biotechnological potential research directions. We convinced fundamental study application will be understood by reader result work. The summary different improvement also benefit readers provide ideas thoughts future process.

Язык: Английский

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Green synthesis of stable hybrid biocatalyst using a hydrogen-bonded, π-π-stacking supramolecular assembly for electrochemical immunosensor

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Июнь 20, 2023

Abstract Rational integration of native enzymes and nanoscaffold is an efficient means to access robust biocatalyst, yet remains on-going challenges due the trade-off between fragile harsh assembling conditions. Here, we report a supramolecular strategy enabling in situ fusion into porous crystal. A c2-symmetric pyrene tecton with four formic acid arms utilized as building block engineer this hybrid biocatalyst. The decorated afford tectons high dispersibility minute amount organic solvent, permit hydrogen-bonded linkage discrete extended network around enzyme almost solvent-free aqueous solution. This biocatalyst covered by long-range ordered pore channels, which can serve gating sieve catalytic substrate thus enhance biocatalytic selectivity. Given structural integration, biocatalyst-based electrochemical immunosensor developed, pg/mL detection cancer biomarker.

Язык: Английский

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A comprehensive review of recent developments in metal-organic framework/polymer composites and their applications

Surfaces and Interfaces, Год журнала: 2023, Номер 43, С. 103574 - 103574

Опубликована: Ноя. 10, 2023

Язык: Английский

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Microfluidic formulation of anticancer peptide loaded ZIF-8 nanoparticles for the treatment of breast cancer

Journal of Colloid and Interface Science, Год журнала: 2023, Номер 642, С. 810 - 819

Опубликована: Март 30, 2023

Язык: Английский

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Metal–organic framework-engineered enzyme/nanozyme composites: Preparation, functionality, and sensing mechanisms

Chemical Engineering Journal, Год журнала: 2024, Номер 496, С. 153884 - 153884

Опубликована: Июль 9, 2024

Язык: Английский

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Mof-derived hollow-open hierarchically porous carbon spheres for enzyme encapsulation and biocatalysis

Chemical Engineering Journal, Год журнала: 2025, Номер 505, С. 158972 - 158972

Опубликована: Янв. 7, 2025

Язык: Английский

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