The design of porous microcapsules with selective mass transfer and mechanical robustness for enzyme encapsulation is highly desired for biocatalysis, yet the construction remains challenging. Herein, we report the facile fabrication of porous microcapsules by assembling covalent organic framework (COF) spheres at the interfaces of emulsion droplets followed by interparticle crosslinking. The COF microcapsules could offer an enclosed aqueous environment for enzymes, with size-selective porous shells that allow for the fast diffusion of substrates and products while excluding larger molecules such as protease. Crosslinking of COF spheres not only enhances the structural stability of capsules but also imparts enrichment effects. The enzymes encased in the COF microcapsules show enhanced activity and durability in organic media as verified in both batch reaction and continuous-flow reaction. The COF microcapsules offer a promising platform for the encapsulation of biomacromolecules.

Covalent Organic Framework Based Crosslinked Porous Microcapsules for Enzymatic Catalysis.

Review of covalent organic frameworks for enzyme immobilization: Strategies, applications, and prospects.

A practical electrochemical strategy for direct synthesis of arenesulfonyl fluorides from industrial feedstock nitroarenes is described. Key to success lies in using cheap ionic liquid N-methylimidazolium p-toluenesulfonate ([Mim]PhSO3) as an...

Direct electrochemical synthesis of arenesulfonyl fluorides from nitroarenes: A dramatic ionic liquid effect

Covalent organic frameworks (COFs) have emerged as a new type of crystalline porous polymers of great interest. However, their preparation requires long reaction times. Microwave-assisted synthesis (MAS) offers an interesting approach to increasing the reaction rate of chemical processes. Thus, microwaves can be a key tool for the fast and scalable synthesis of COFs. Since our previous review on the topic, the preparation of COFs with microwaves has been evolving. Herein, we present a compilation of COFs studies and experiments published in the last three years on the synthesis of COFs using microwave-assisted synthesis as a source of energy. The articles include imine, triazine, and other 2D COFs synthesized using MAS. The 3D COFs have also been compiled. The chemical structure of the monomers and the COFs and their main parameters of synthesis and application are summarized for each article.

/pdf/novel-microwave-assisted-synthesis-of-cofs-2020-2022-dqttv8vi.pdf

Novel Microwave-Assisted Synthesis of COFs: 2020–2022

Hypoxia, or low oxygen levels, is a common feature of the tumor microenvironment. It is caused by the aggressive proliferation of cancer cells, which consume more oxygen than healthy cells. Hypoxia not only activates several signaling pathways that promote tumor growth, and metastasis but also increases resistance to conventional cancer treatments. The introduction of covalent organic frameworks (COFs), with their porous structure, high stability, tunable properties, large surface area, and unrivaled biocompatibility, has offered promising prospects for resolving hypoxia-specific challenges. This write-up critically explores the COFs in enhancing oxygen delivery, reactive oxygen species (ROS) generation, optimized drug delivery, and enabling hypoxia-specific imaging. Furthermore, it outlines how COFs facilitate various hypoxia-targeting therapeutic modalities such as chemotherapy, type-I and type-II photodynamic therapy, photothermal therapy, sonodynamic therapy, and immunotherapy. By evaluating the latest research findings and their implications, this review offers insights into the potent role of COFs in curtailing hypoxia and bolstering cancer treatment efficiency. The overarching goal of this assessment is to enrich our understanding of hypoxia-specific cancer therapy strategies, crediting the pivotal role of COFs. It is hoped that this greater comprehension of the abilities and constraints of COFs will pave the way to conceive more potent and targeted therapeutic interventions, thereby enhancing patient outcomes in the complex terrain of cancer therapeutics. 

Covalent organic framework nanoparticles: Overcoming the challenges of hypoxia in cancer therapy

Flow chemistry provides a neo-orientation for the research and development of chemical technology, in which heterogeneous continuous catalysis based on packed beds can realize rapid separation and recycling. However, options for heterogeneous catalysts are still limited. In this work, we gradually grow covalent organic frameworks (COFs, TpBpy) on the surface of a silica gel (SiO2)-supported substrate to obtain a stable copper(I)-chelated high-loading heterogeneous catalyst (SiO2@CuI-TpBpy). SiO2@CuI-TpBpy shows high catalytic activity in three-component Huisgen 1,3-dipolar cycloaddition, giving the corresponding triazoles with excellent yields and reposeful recyclability under batch conditions. The structures of the catalysts remain steady, and the copper contents are basically unchanged after five cycles. Then, the catalysts are successfully applied for three-component heterogeneous catalysis in a one-pot continuous flow to prepare rufinamide in 89% yield for 24 h stably and efficiently with mere traces of copper ions remaining. More importantly, the catalytic system reveals a minuscule effect of catalyst particle size on internal diffusion. This COF encapsulation strategy presents a new possibility for the design of industrial heterogeneous catalysts with high metal loading and low internal diffusion resistance.

Accelerated Diffusion of a Copper(I)-Functionalized COF Packed Bed Reactor for Efficient Continuous Flow Catalysis.

Driven by green and sustainable methodologies for chemical manufacturing, enzymes are forecast to have much to prospect in the coming years due to their high activity and selectivity. However, the fragile active spatial‐conformation of an enzyme is predominantly maintained by weak intermolecular interactions, showing quite sensitive to thermal, pH, and chemical chemoreception. Thus, the low activity and recyclability result from structural instability can hardly meet the prototype of green chemistry in commercial process. Covalent organic frameworks (COFs) are stable extended porous network materials assembled by organic linkers in a moderate way. Due to their pre‐designable structures, an enzyme possesses the access to be immobilized to the interior or surface of COF skeletons via covalent or noncovalent processes, which can afford protection to enzymes in harsh conditions. Moreover, with the improved stability and cyclicity, the formed COF/enzyme biocomposites can facilitate broader horizon. Herein, this review mainly canvasses the advances in the emerging field of COF/enzyme biocomposites, sketching the factors that are critical in building COF/enzyme systems and the applications of registered enzyme host platforms reported in recent years.

Engineering of Covalent Organic Framework‐Based Advanced Platforms for Enzyme Immobilization: Strategies, Research Progress, and Prospects

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Accelerated Diffusion of a Copper(I)-Functionalized COF Packed Bed Reactor for Efficient Continuous Flow Catalysis.

Engineering of Covalent Organic Framework‐Based Advanced Platforms for Enzyme Immobilization: Strategies, Research Progress, and Prospects