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A series of triarylboron‐based graphdiyne analogues (TAB‐GDYs) with tunable pore size were prepared through copper mediated coupling reaction. The elemental composition, chemical bond, morphology of TAB‐GDYs were well characterized. The crystallinity was confirmed by selected area electron diffraction (SAED) and stacking modes were studied in combination with high resolution transmission electron microscope (HRTEM) and structure simulation. The absorption and desorption isotherm revealed relatively high specific surface area of these TAB‐GDYs up to 788 m2 g−1 for TMTAB‐GDY, which decreased as pore size enlarged. TAB‐GDYs exhibit certain selectivity for CO2/N2 (21.9), CO2/CH4 (5.3), CO2/H2 (41.8) and C2H2/CO2 (2.3). This work has developed a series of boron containing two‐dimensional frameworks with clear structures and good stability, and their tunable pore sizes have laid the foundation for future applications in the gas separation field. [ABSTRACT FROM AUTHOR]

The synthesis of fully conjugated sp2‐carbon covalent organic frameworks (COF) is extremely challenging given the difficulty of the formation of very stable carbon‐carbon double bonds (‐C=C‐). Here, we report the successful preparation of a 2D COF (TP‐COF) based on triazine as central planar units bridged by sp2‐carbon linkers through the ‐C=C‐ condensation reaction. High‐resolution‐transmission electron microscopy (HRTEM) clearly confirmed the tessellated hexagonal pore structure with a pore center‐to‐center distance of 2 nm. Powder X‐ray diffraction (PXRD) together with structural simulations revealed an AA stacking mode of the obtained layered structure. TP‐COF turned out to be an excellent semiconductor material with a LUMO energy of −3.23 eV and a band gap of 2.36 eV. Excitingly, this novel sp2‐carbon conjugated TP‐COF exhibited unprecedented coenzyme regeneration efficiency and can significantly boost the coenzyme‐assisted synthesis of l‐glutamate to a record‐breaking 97 % yield within 12 minutes. Art imitates life: A 2D conjugated covalent organic framework (COF) based on triazine as a central planar unit bridged by sp2‐carbon linkers was constructed through the ‐C=C‐ condensation reaction. The COF can be used as an artificial photosystem I and shows an excellent coenzyme‐regeneration efficiency. [ABSTRACT FROM AUTHOR]