Three-Dimensional Tetrathiafulvalene-Based covalent organic frameworks for efficient photocatalytic nitrogen fixation
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Tetrathiafulvalene
Covalent organic framework
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Abstract Covalent organic frameworks (COF) with periodic porous structures and tunable functionalities are a new class of crystalline polymers connected via strong covalent bonds. Constructing COF materials with high stability and porosity is attracting and essential for COFs’ further functional exploration. In this work, two new covalent organic frameworks (TTA‐TMTA‐COF and TTA‐FMTA‐COF) with high surface area, large pore volume, and excellent chemical stability toward harsh conditions are designed and synthesized by integrating the methoxy functional groups into the networks. Both two COFs are further employed for iodine removal since radioactive iodine in nuclear waste has seriously threatened the natural environment and human health. TTA‐TMTA‐COF and TTA‐FMTA‐COF can capture 3.21 and 5.07 g g −1 iodine, respectively. Notably, the iodine capture capacity for iodine of TTA‐FMTA‐COF does not show any decline after being recycled five times. These results demonstrate both COFs possess ultrahigh capacity and excellent recyclability.
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A heterostructured covalent organic framework (COF) membrane is synthesized via in situ linker exchange. Narrowed pores can be formed at the interface between two types of COFs by adjusting the linker exchange duration. The resultant COF membrane demonstrates a high rejection rate toward Na2SO4 of up to 97%.
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Covalent organic framework
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A hydrophilic covalent organic framework (BTA-BDSA-COF) was successfully erected by introducing multi-sulfonated groups into a covalent framework structure and it can be easily applied to capture the cationic dye in real water samples.
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Cationic polymerization
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A novel covalent organic framework (COF) based on terphenyldiboronic acid exhibiting open pores of about 4.1 nm is presented. The pore walls of the COF could be functionalized with a fluorescent dye.
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For the first time, covalent organic frameworks (COF-TpPa and COF-TpPaC) are selected to combine with the BiVO4 photoanode through a covalent bond. The heterojunction and covalent connection of COFs and BiVO4 can promote the separation of carriers, and the -CH3 on the benzene ring in COF-TpPaC as an electron donor group can increase the carrier concentration of the photoanode. As a result, the TpPaC/BiVO4 photoanode shows the best performance. This covalent hybridization strategy opens a new insight into the development of COF-modified photoanodes.
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Covalent organic frameworks (COF) are porous crystalline polymers connected by covalent bonds. Due to their inherent high specific surface area, tunable pore size, and good stability, they have attracted extensive attention from researchers. In recent years, COF membrane materials developed rapidly, and a large amount of research work has been presented on the preparation methods, properties, and applications of COF membranes. This review focuses on the research on independent/pure continuous COF membranes. First, based on the membrane formation mechanism, COF membrane preparation methods are categorized into two main groups: bottom-up and top-down. Four methods are presented, namely, solvothermal, interfacial polymerization, steam-assisted conversion, and layer by layer. Then, the aperture, hydrophilicity/hydrophobicity and surface charge properties of COF membranes are summarized and outlined. According to the application directions of gas separation, water treatment, organic solvent nanofiltration, pervaporation and energy, the latest research results of COF membranes are presented. Finally, the challenges and future directions of COF membranes are summarized and an outlook provided. It is hoped that this work will inspire and motivate researchers in related fields.
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Abstract Redox‐active tetrathiafulvalene (TTF)‐based covalent organic frameworks (COFs) exhibit distinctive electrochemical and photoelectrical properties, but their prevalent two‐dimensional (2D) structure with densely packed TTF moieties limits the accessibility of redox center and constrains their potential applications. To overcome this challenge, an 8‐connected TTF linker (TTF‐8CHO) is designed as a new building block for the construction of three‐dimensional (3D) COFs. This approach led to the successful synthesis of a 3D COF with the bcu topology, designated as TTF‐8CHO‐COF. In comparison to its 2D counterpart employing a 4‐connected TTF linker, the 3D COF design enhances access to redox sites, facilitating controlled oxidation by I 2 or Au 3+ to tune physical properties. When irradiated with a 0.7 W cm −2 808 nm laser, the oxidized 3D COF samples (@TTF‐8CHO‐COF and Au NPs@TTF‐8CHO‐COF) demonstrated rapid temperature increases of 239.3 and 146.1 °C, respectively, which surpassed those of pristine 3D COF (65.6 °C) and the 2D COF counterpart (6.4 °C increment after I 2 treatment). Furthermore, the oxidation of the 3D COF heightened its photoelectrical responsiveness under 808 nm laser irradiation. This augmentation in photothermal and photoelectrical response can be attributed to the higher concentration of TTF ·+ radicals generated through the oxidation of well‐exposed TTF moieties.
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We propose a dynamic covalent chemistry (DCC)-induced linker exchange strategy for the structural transformation between covalent organic frameworks (COFs) and cages for the first time. Studies have shown that the COF-to-cage and cage-to-COF transformations were realized by using borate bonds and imine bonds, respectively, as linkages. Self-sorting experiments suggested that borate cages and imine COFs are thermodynamic minimum compounds. This research builds a bridge between discrete and polymeric organic scaffolds and broadens the knowledge of chemistry and materials for porous materials science.
Dynamic Covalent Chemistry
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