Covalent Organic Frameworks for the Purification of Recombinant Enzymes and Heterogeneous Biocatalysis

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 146(1), P. 858 - 867

Published: Dec. 30, 2023

Recombinant enzymes have gained prominence due to their diverse functionalities and specificity are often a greener alternative in biocatalysis. This context makes purifying recombinant from host cells other impurities crucial. The primary goal is isolate the pure enzyme of interest ensure its stability under ambient conditions. Covalent organic frameworks (COFs), renowned for well-ordered structure permeability, offer promising approach histidine-tagged (His-tagged) enzymes. Furthermore, immobilizing within COFs represents growing field heterogeneous In this study, we developed flow-based technology utilizing nickel-infused covalent framework (Ni-TpBpy COF) combine two distinct processes: purification His-tagged immobilization simultaneously. Our work primarily focuses on three β-glucosidase, cellobiohydrolase, endoglucanase as well proteins with varying molecular weights, namely, green fluorescent protein (27 kDa) BG Rho (88 kDa). We employed Ni-TpBpy column matrix showcase versatility our system. Additionally, successfully obtained COF immobilized enzymes, which can serve catalyst hydrolysis p-nitrophenyl-β-d-glucopyranoside carboxymethylcellulose. These demonstrated catalytic activity comparable that free counterparts, added advantages recyclability enhanced conditions an extended period, ranging 60 90 days. contrasts do not maintain effectively over time.

Language: Английский

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Enzyme Immobilization using Covalent Organic Frameworks: From Synthetic Strategy to COFs Functional Role

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(31), P. 40371 - 40390

Published: July 29, 2024

Enzymes, a class of biocatalysts, exhibit remarkable catalytic efficiency, specificity, and selectivity, governing many reactions that are essential for various cascades within living cells. The immobilization structurally flexible enzymes on appropriate supports holds significant importance in facilitating biomimetic transformations extracellular environments. Covalent organic frameworks (COFs) have emerged as ideal candidates enzyme due to high surface tunability, diverse chemical/structural designs, exceptional stability, metal-free nature. Various techniques been proposed fabricate COF-enzyme biocomposites, offering enhancements activity reusability COF-immobilized well new insights into developing advanced enzyme-based applications. In this review, we provide comprehensive overview state-of-the-art strategies immobilizing COFs by focusing their applicability versatility. These systematically summarized compared categorizing them postsynthesis situ immobilization, where respective strengths limitations thoroughly discussed. Combined with an critical emerging applications, further elucidate the multifaceted roles subsequent highlighting biofunctionality achievable through COFs.

Language: Английский

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Enhancing the Crystallinity of Keto‐enamine‐Linked Covalent Organic Frameworks through an in situ Protection‐Deprotection Strategy

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(13)

Published: Feb. 7, 2024

β-Keto-enamine-linked 2D covalent organic frameworks (COFs) have emerged as highly robust materials, showing significant potential for practical applications. However, the exclusive reliance on 1,3,5-triformylphloroglucinol (Tp aldehyde) in design of such COFs often results production non-porous amorphous polymers when combined with certain amine building blocks. Attempts to adjust crystallinity and porosity by a modulator approach are inefficient because Tp aldehyde readily forms stable β-keto-enamine-linked monomers/oligomers various aromatic amines through an irreversible keto-enol tautomerization process. Our research employed unique protection-deprotection strategy enhance squaramide-based COFs. Advanced solid-state NMR studies, including 1D

Language: Английский

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Enhancing photocatalytic performance of covalent organic frameworks via ionic polarization

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Nov. 6, 2024

Covalent organic frameworks have emerged as a thriving family in the realm of photocatalysis recently, yet with concerns about their high exciton dissociation energy and sluggish charge transfer. Herein, strategy to enhance built-in electric field series β-keto-enamine-based covalent by ionic polarization method is proposed. The achieved through distinctive post-synthetic quaternization reaction which can endow separated centers comprising cationic skeleton iodide counter-anions. stronger generated between framework anions promotes transfer efficiency. Moreover, introduced not only serve lowered H* formation barrier, but also act electron extractant suppressing recombination electron-hole pairs. Therefore, photocatalytic performance shows notable improvement, among CH3I-TpPa-1 deliver an H2 production rate up 9.21 mmol g−1 h−1 without any co-catalysts, representing 42-fold increase compared TpPa-1, being comparable or possibly exceeding current photocatalysts addition Pt co-catalysts. (COFs) show great promise are limited slow Here, authors report COFs via polarization, resulting hydrogen evolution g-¹ h-¹

Language: Английский

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Frontiers in design and applications of biomacromolecule@COFs composites

Coordination Chemistry Reviews, Journal Year: 2024, Volume and Issue: 515, P. 215965 - 215965

Published: May 23, 2024

Language: Английский

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Nanostructurally Engineering Covalent Organic Frameworks for Boosting CO₂ Photoreduction

Small, Journal Year: 2023, Volume and Issue: 20(15)

Published: Nov. 27, 2023

Abstract Herein, a series of imine‐linked covalent organic frameworks (COFs) are developed with advanced ordered mesoporous hollow spherical nanomorphology and ultra‐large mesopores (4.6 nm in size), named OMHS‐COF‐M (M = H, Co, Ni). The is revealed to be formed via an Ostwald ripening mechanism based on one‐step self‐templated strategy. Encouraged by its unique structural features outstanding photoelectrical property, the OMHS‐COF‐Co material applied as photocatalyst for CO 2 ‐to‐CO reduction. Remarkably, it delivers impressive production rate high 15 874 µmol g −1 h , large selectivity 92.4%, preeminent cycling stability. From in/ex situ experiments density functional theory (DFT) calculations, excellent photoreduction performance ascribed desirable cooperation host abundant isolated Co active sites, enhancing activation, improving electron transfer kinetics well reducing energy barriers intermediates *COOH generation desorption.

Language: Английский

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Metal−Organic Framework‐Induced Rh Monocoodination on Diphosphine Ligand Enables Catalytic Hydroformylation of Aliphatic Olefins at Room Temperature and Pressure

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: July 11, 2024

Abstract Persistent challenges in hydroformylation of olefins include controlling regioselectivity, particularly for short aliphatic and conducting reactions under ambient conditions. We report here the synthesis monophosphine–Rh complexes on a typical chelated diphosphine ligand mediated by Zr‐MOF through isolating pair phosphorus atoms. demonstrate that single‐crystal X‐ray diffraction can elucidate structural transformation Rh catalyst during olefin hydroformylation, providing valuable information active site reconstruction catalysis. The Rh‐MOF demonstrates excellent catalytic recyclable performance with linear to branched ratios up 99 : 1. Due framework‘s capacity adsorb concentrate gases, occur room temperature pressure, eliminating need high pressures typically required homogeneous systems. This study show Zr–MOF be unique platform synthesizing unusual species cannot exist solutions meaningful chemical transformations pertaining metal‐based

Language: Английский

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Covalent Organic Frameworks as Potential Drug Carriers and Chemotherapeutic Agents for Ovarian Cancers

ACS Biomaterials Science & Engineering, Journal Year: 2024, Volume and Issue: 10(7), P. 4227 - 4236

Published: June 7, 2024

Anticancer drugs are often associated with limitations such as poor stability in aqueous solutions, limited cell membrane permeability, nonspecific targeting, and irregular drug release when taken orally. One possible solution to these problems is the use of nanocarriers molecules, particularly those targeting ability, stimuli-responsive properties, high loading capacity. These can improve stability, increase cellular uptake, allow specific cancer cells, provide controlled release. While improving therapeutic efficacy drugs, contemporary researchers also aim reduce their side effects, that patients offered a more effective targeted treatment strategy. Herein, set nine porous covalent organic frameworks (COFs) were tested delivery nanocarriers. Among these, paclitaxel loaded COF-3 was most against proliferation ovarian cells. This study highlights emerging potential COFs field delivery. Due biocompatibility, viable substrate for release, making them attractive candidates systems. work demonstrates efficient agents, thereby opening up new opportunities sarcoma therapy.

Language: Английский

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Covalent Organic Frameworks: Cutting‐Edge Materials for Carbon Dioxide Capture and Water Harvesting from Air

Chemistry - A European Journal, Journal Year: 2023, Volume and Issue: 30(6)

Published: Dec. 11, 2023

Abstract The implacable rise of carbon dioxide (CO 2 ) concentration in the atmosphere and acute water stress are one central challenges our time. Present‐day chemistry is strongly inclined towards more sustainable solutions. Covalent organic frameworks (COFs), attributable to their structural designability with atomic precision, functionalizable chemical environment robust extended architectures, have demonstrated promising performances CO trapping harvesting from air. In this Review, we discuss major developments field as well sketch out opportunities shortcomings that remain over large‐scale COF synthesis, device engineering, long‐term performance real environments.

Language: Английский

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Responsive Multi‐Arm PEG‐Modified COF Nanocomposites: Dynamic Photothermal, pH/ROS Dual‐Responsive, Targeted Carriers for Rheumatoid Arthritis Treatment

Advanced Healthcare Materials, Journal Year: 2024, Volume and Issue: unknown

Published: June 17, 2024

Rheumatoid arthritis (RA) is a chronic immune disease characterized by the infiltration of cells and proliferation fibroblast-like synoviocytes (FLS) at joint site, leading to inflammation destruction. However, available treatment options targeting both inflammatory proliferative FLS are limited. Herein, this work presents three covalent organic frameworks (COFs) photothermal composite systems modified with multi-armed polyethylene glycols (PEG) for RA. These exhibit dual response under low pH high reactive oxygen species (ROS) conditions site inflammation, specific focus on delivering protein drug ribonuclease A (RNase A). Notably, molecular docking studies reveal interaction between RNase NF-κB p65 protein, Western blotting confirm its inhibitory effect activity. In vitro in vivo experiments verify significant reduction swelling deformities adjuvant-induced (AIA) rats after delivered PEG-modified COF ligands, restoring morphology normal. findings underscore promising therapeutic potential COFs RA, highlighting their unique capabilities addressing aspects expanding scope biomedical applications COFs.

Language: Английский

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