Enzyme‐Engineered Metal‐Organic Frameworks for the Construction of Organophosphorus Pesticide Biosensor DOI
Hongxia Li, Qi Lu,

Junxiao Shi

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 34(6)

Published: Oct. 29, 2023

Abstract Rational immobilization of fragile enzymes on a scaffold is an efficient protocol to achieve robust biocatalyst, yet the construction remains challenging due trade‐off between enzyme activity and framework environment. Herein, enzyme‐engineered assembly strategy enabling in situ fusion acetylcholinesterase (AChE) into Zn‐based metal‐organic frameworks (Zn‐MOF‐74) during rapid nucleation crystal defect growth process, demonstrated. The Zn‐MOF‐74 composites can offer hydrophilic microenvironment for maintaining biological state AChE, with flower‐like porous structure that allows boosting mass transfer process substrates products. Impressively, apparent AChE be well maintained 90% after encapsulation, AChE@Zn‐MOF‐74 produced excellent stability inhospitable environments. Given structural integration, AChE@Zn‐MOF‐74‐based biosensor constructed sensitive detection chlorpyrifos (organophosphorus pesticides) limit 1.0 ng mL −1 , monitoring pesticide degradation extent water body. This study anticipated valuable insight understanding structure‐activity relationship enzyme@MOF encourage applications biosensors precision agriculture.

Language: Английский

Bioinspired Framework Catalysts: From Enzyme Immobilization to Biomimetic Catalysis DOI Creative Commons
Kunyu Wang, Jiaqi Zhang, Yu‐Chuan Hsu

et al.

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(9), P. 5347 - 5420

Published: April 12, 2023

Enzymatic catalysis has fueled considerable interest from chemists due to its high efficiency and selectivity. However, the structural complexity vulnerability hamper application potentials of enzymes. Driven by practical demand for chemical conversion, there is a long-sought quest bioinspired catalysts reproducing even surpassing functions natural As nanoporous materials with surface areas crystallinity, metal-organic frameworks (MOFs) represent an exquisite case how enzymes their active sites are integrated into porous solids, affording heterogeneous superior stability customizable structures. In this review, we comprehensively summarize advances MOFs catalysis, discuss design principle various MOF-based catalysts, such as MOF-enzyme composites embedded sites, explore utility these in different reactions. The advantages enzyme mimetics also highlighted, including confinement, templating effects, functionality, comparison homogeneous supramolecular catalysts. A perspective provided potential solutions addressing current challenges MOF catalysis.

Language: Английский

Citations

186

Aggregation behaviour of pyrene-based luminescent materials, from molecular design and optical properties to application DOI
Xing Feng, Xiaohui Wang, Carl Redshaw

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(19), P. 6715 - 6753

Published: Jan. 1, 2023

This review not only highlights the progress of emission and electronic behaviour new pyrene-based luminescence molecules in aggregated state, but also provides a perspective for understanding mechanism optoelectronic properties pyrenes.

Language: Английский

Citations

156

Encapsulating and stabilizing enzymes using hydrogen-bonded organic frameworks DOI
Guosheng Chen, Siming Huang, Xiaomin Ma

et al.

Nature Protocols, Journal Year: 2023, Volume and Issue: 18(7), P. 2032 - 2050

Published: May 17, 2023

Language: Английский

Citations

62

Hydrogen-bonded organic frameworks: new horizons in biomedical applications DOI

Dongqin Yu,

Haochen Zhang, Jinsong Ren

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(21), P. 7504 - 7523

Published: Jan. 1, 2023

Hydrogen-bonded organic frameworks (HOFs) are an emerging attractive class of highly crystalline porous materials characterized by significant biocompatibility, rich chemical functionalities and well-defined porosity. The unique advantages including metal-free nature reversible binding manner significantly distinguish HOFs from other in the biotechnology biomedical field. However, relevant HOF studies still remain their infancy despite promising remarkable results that have been presented recent years. Due to intricate dynamic physiological conditions, major challenge lies stability structural diversity vivo. In this Tutorial Review, we summarize common building blocks for construction HOF-based functional biomaterials latest developments biological Moreover, highlight current challenges regarding functionalization along with corresponding potential solutions. This Review will a profound effect future years on design applications biomaterials.

Language: Английский

Citations

62

Atomic-level design of metalloenzyme-like active pockets in metal–organic frameworks for bioinspired catalysis DOI
Weiqing Xu, Yu Wu, Wenling Gu

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 53(1), P. 137 - 162

Published: Nov. 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.

Language: Английский

Citations

61

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

Chunyan Xing,

Zhenjie Mu

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(24), P. 13469 - 13475

Published: June 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

Language: Английский

Citations

58

Enzyme immobilization on covalent organic framework supports DOI
Qianqian Zhu,

Yunlong Zheng,

Zhenjie Zhang

et al.

Nature Protocols, Journal Year: 2023, Volume and Issue: 18(10), P. 3080 - 3125

Published: Sept. 6, 2023

Language: Английский

Citations

52

Green synthesis of stable hybrid biocatalyst using a hydrogen-bonded, π-π-stacking supramolecular assembly for electrochemical immunosensor DOI Creative Commons
Wei Huang, Haitao Yuan, Hongling Yang

et al.

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: June 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.

Language: Английский

Citations

50

Two-Site Enhanced Porphyrinic Metal–Organic Framework Nanozymes and Nano-/Bioenzyme Confined Catalysis for Colorimetric/Chemiluminescent Dual-Mode Visual Biosensing DOI
Huining Chai, Yujie Li, Kun Yu

et al.

Analytical Chemistry, Journal Year: 2023, Volume and Issue: 95(44), P. 16383 - 16391

Published: Oct. 26, 2023

The rational design of efficient nanozymes and the immobilization enzymes are great significance for construction high-performance biosensors based on nano-/bioenzyme catalytic systems. Herein, a novel V-TCPP(Fe) metal-organic framework nanozyme with two-dimensional nanosheet morphology is rationally designed by using V2CTx MXene as metal source iron tetrakis(4-carboxyphenyl)porphine (FeTCPP) ligand an organic linker. It exhibits enhanced peroxidase- catalase-like activities luminol-H2O2 chemiluminescent (CL) behavior. Based experimental theoretical results, these excellent enzyme-like derived from two-site synergistic effect between V nodes FeTCPP ligands in V-TCPP(Fe). Furthermore, confined system developed zeolitic imidazole (ZIF) coencapsulation bioenzyme. Using acetylcholinesterase (AChE) model, our constructed V-TCPP(Fe)/AChE@ZIF was successfully used colorimetric/CL dual-mode visual biosensing organophosphorus pesticides. This work expected to provide new insights into systems, encouraging applications catalysis biosensing.

Language: Английский

Citations

46

Metal–organic framework-engineered enzyme/nanozyme composites: Preparation, functionality, and sensing mechanisms DOI
Yujie Li, Huining Chai,

Zhishuang Yuan

et al.

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 496, P. 153884 - 153884

Published: July 9, 2024

Language: Английский

Citations

28