Rationally Tailored Mesoporous Hosts for Optimal Protein Encapsulation DOI
Fanrui Sha, Haomiao Xie, Florencia A. Son

и другие.

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(30), С. 16383 - 16390

Опубликована: Июль 18, 2023

Proteins play important roles in the therapeutic, medical diagnostic, and chemical catalysis industries. However, their potential is often limited by fragile dynamic nature outside cellular environments. The encapsulation of proteins solid materials has been widely pursued as a route to enhance stability ease handling. Nevertheless, experimental investigation protein interactions with rationally designed synthetic hosts still represents an area need improvement. In this work, we leveraged tunability crystallinity metal-organic frameworks (MOFs) developed series crystallographically defined varying properties. Through systematic studies, identified dominating mechanisms for host material well-tailored properties effectively encapsulate ubiquitin. Specifically, our mesoporous hosts, found that ubiquitin thermodynamically favored. A more hydrophilic environment favorable electrostatic induces enthalpically favored ubiquitin-MOF interactions, higher pH condition reduces intraparticle diffusion barrier, both leading loading. Our findings provide fundamental understanding host-guest between matrices offer new insights guide design future achieve optimal MOF modification technique used work also demonstrates facile method develop easily customizable encapsulating different surface

Язык: Английский

Stimuli-responsive metal–organic framework nanoparticles for controlled drug delivery and medical applications DOI
Zhixin Zhou, Margarita Vázquez‐González, Itamar Willner

и другие.

Chemical Society Reviews, Год журнала: 2021, Номер 50(7), С. 4541 - 4563

Опубликована: Янв. 1, 2021

Different chemical, physical, and biomarker triggers to unlock the metal–organic framework nanoparticles release drugs loaded in particles will be addressed.

Язык: Английский

Процитировано

237
Confining enzymes in porous organic frameworks: from synthetic strategy and characterization to healthcare applications DOI
Siming Huang, Guosheng Chen, Gangfeng Ouyang

и другие.

Chemical Society Reviews, Год журнала: 2022, Номер 51(15), С. 6824 - 6863

Опубликована: Янв. 1, 2022

This review comprehensively presents the cutting-edge advances of enzyme confinement using different porous organic frameworks.

Язык: Английский

Процитировано

193
Protein-directed, hydrogen-bonded biohybrid framework DOI Creative Commons
Guosheng Chen, Siming Huang,

Yong Shen

и другие.

Chem, Год журнала: 2021, Номер 7(10), С. 2722 - 2742

Опубликована: Авг. 3, 2021

Язык: Английский

Процитировано

124
Fine-Tuning the Micro-Environment to Optimize the Catalytic Activity of Enzymes Immobilized in Multivariate Metal–Organic Frameworks DOI
Yiming Li, Jian Yuan, Hao Ren

и другие.

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

Процитировано

122
Hydrogen-bonded organic framework biomimetic entrapment allowing non-native biocatalytic activity in enzyme DOI Creative Commons
Guosheng Chen,

Linjing Tong,

Siming Huang

и другие.

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

Опубликована: Авг. 16, 2022

Abstract Nature programs the structural folding of an enzyme that allows its on-demand biofunctionality; however, it is still a long-standing challenge to manually modulate enzyme’s conformation. Here, we design exogenous hydrogen-bonded organic framework conformation cytochrome c, and hence allow non-native bioactivity for enzyme. The rigid framework, with net-arranged carboxylate inner cage, in situ installed onto native c. resultant nano-biointerface changes previously not achieved catalase-like species within reported c-porous systems. In addition, preserved can stabilize encapsulated channel-like pores also guarantee free entrance catalytic substrates. This work describes conceptual nanotechnology manoeuvring flexible conformations enzyme, highlights advantages artificial scaffolds activity.

Язык: Английский

Процитировано

118
Green and Scalable Fabrication of High‐Performance Biocatalysts Using Covalent Organic Frameworks as Enzyme Carriers DOI

Yunlong Zheng,

Sainan Zhang,

Jinbiao Guo

и другие.

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(39)

Опубликована: Авг. 2, 2022

Abstract Enzyme immobilization is essential to the commercial viability of various critical large‐scale biocatalytic processes. However, challenges remain for systems, such as difficulties in loading large enzymes, enzyme leaching, and limitations fabrication. Herein, we describe a green scalable strategy prepare high‐performance biocatalysts through situ assembly enzymes with covalent organic frameworks (COFs) under ambient conditions (aqueous solution room temperature). The obtained have exceptional reusability stability serve efficient important industrial reactions that cannot be efficiently catalyzed by free or traditional systems. Notably, this versatile platform applicable COFs enzymes. an aqueous occurred within short timeframe (ca. 10–30 min) could scaled up readily 2.3 g per reaction).

Язык: Английский

Процитировано

114
Enhancing Enzyme Activity by the Modulation of Covalent Interactions in the Confined Channels of Covalent Organic Frameworks DOI

Chunyan Xing,

Pei Mei,

Zhenjie Mu

и другие.

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(21)

Опубликована: Март 10, 2022

Controllable regulations on the enzyme conformation to optimize catalytic performance are highly desired for immobilized biocatalysts yet remain challenging. Covalent organic frameworks (COFs) possess confined channels with finely tunable pore environment, offering a promising platform encapsulation. Herein, we covalently cytochrome c (Cyt c) in size-matched of COFs different contents anchoring site, and significant enhancement stability activity (≈600 % relative compared free enzyme) can be realized by optimizing covalent interactions. Structural analyses Cyt suggest that bonding could induce conformational perturbation resulting more accessible active sites. The effectiveness interaction modulation together tailorable offers promise develop high-performance biocatalysts.

Язык: Английский

Процитировано

87
Design and Advanced Manufacturing of NU‐1000 Metal–Organic Frameworks with Future Perspectives for Environmental and Renewable Energy Applications DOI Creative Commons
Reza Abazari,

Soheila Sanati,

Majed A. Bajaber

и другие.

Small, Год журнала: 2023, Номер 20(15)

Опубликована: Ноя. 23, 2023

Abstract Metal–organic frameworks (MOFs) represent a relatively new family of materials that attract lots attention thanks to their unique features such as hierarchical porosity, active metal centers, versatility linkers/metal nodes, and large surface area. Among the extended list MOFs, Zr‐based‐MOFs demonstrate comparably superior chemical thermal stabilities, making them ideal candidates for energy environmental applications. As Zr‐MOF, NU‐1000 is first synthesized at Northwestern University. A comprehensive review various approaches synthesis MOFs obtaining properties (e.g., diverse morphologies, area, particular pore size distribution) applications in catalysis (electro‐, photo‐catalysis), CO 2 reduction, batteries, hydrogen storage, gas storage/separation, other fields are presented. The further outlines current challenges development derivatives practical applications, revealing areas future investigation.

Язык: Английский

Процитировано

84
Harnessing Self-Repairing and Crystallization Processes for Effective Enzyme Encapsulation in Covalent Organic Frameworks DOI
Yufeng Zhang,

Chunyan Xing,

Zhenjie Mu

и другие.

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(24), С. 13469 - 13475

Опубликована: Июнь 7, 2023

Immobilization of fragile enzymes in crystalline porous materials offers new opportunities to expand the applications biocatalysts. However, limited by pore size and/or harsh synthesis conditions hosts, often suffer from dimension limitation or denaturation during immobilization process. Taking advantage dynamic covalent chemistry feature organic frameworks (COFs), herein, we report a preprotection strategy encapsulate COFs self-repairing and crystallization Enzymes were first loaded low-crystalline polymer networks with mesopores formed at initial growth stage, which could offer effective protection for reaction conditions, subsequently encapsulation proceeded disordered into framework. Impressively, biological activity can be well-maintained after encapsulation, obtained enzyme@COFs also show superior stability. Furthermore, circumvents enzymes, its versatility was verified different sizes surface charges, as well two-enzyme cascade system. This study universal design idea robust supports holds promise developing high-performance immobilized

Язык: Английский

Процитировано

58
Insight into Bioactivity of In‐situ Trapped Enzyme‐Covalent‐Organic Frameworks DOI Creative Commons
Jieying Liang, Juanfang Ruan,

Bosiljka Njegic

и другие.

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(23)

Опубликована: Апрель 6, 2023

Abstract Selecting a suitable support material for enzyme immobilization with excellent biocatalytic activity and stability is critical aspect in the development of functional biosystems. The highly stable metal‐free properties covalent‐organic frameworks (COFs) make them ideal supports immobilization. Herein, we constructed three kinds COFs via biofriendly one‐pot synthetic strategy at room temperature aqueous solution. Among developed (COF‐LZU1, RT‐COF‐1 ACOF‐1), horseradish peroxidase (HRP)‐incorporated COF‐LZU1 found to retain highest activity. Structural analysis reveals that weakest interaction between hydrated COF‐LZU1, an easiest accessibility by substrate, as well optimal conformation together promote bioactivity HRP‐COF‐LZU1. Furthermore, revealed be versatile nanoplatform encapsulating multiple enzymes. also offers superior protection immobilized enzymes under harsh conditions during recycling. comprehensive understanding interfacial interactions COF host guest, substrate diffusion, alteration within matrices represents opportunity design biocatalysts opens broad range applications these nanosystems.

Язык: Английский

Процитировано

50