There have been extensive efforts to synthesize crystalline covalent triazine-based frameworks (CTFs) for practical applications and to realize their potential. The phosphorus pentoxide (P O )-catalyzed direct condensation of aromatic amide instead of aromatic nitrile to form triazine rings. P O -catalyzed condensation was applied on terephthalamide to construct a covalent triazine-based framework (pCTF-1). This approach yielded highly crystalline pCTF-1 with high specific surface area (2034.1 m g ). At low pressure, the pCTF-1 showed high CO (21.9 wt % at 273 K) and H (1.75 wt % at 77 K) uptake capacities. The direct formation of a triazine-based COF was also confirmed by model reactions, with the P O -catalyzed condensation reaction of both benzamide and benzonitrile to form 1,3,5-triphenyl-2,4,6-triazine in high yield.

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Recently, studies of 2D organic layered materials with unique electronic properties have generated considerable interest in the research community. However, the development of organic materials with functional electrical transport properties is still needed. Here, a 2D fused aromatic network (FAN) structure with a C5N basal plane stoichiometry is designed and synthesized, and thin films are cast from C5N solution onto silicon dioxide substrates. Then field‐effect transistors are fabricated using C5N thin flakes as the active layer in a bottom‐gate top‐contact configuration to characterize their electrical properties. The C5N thin flakes, isolated by polydimethylsiloxane stamping, exhibit ambipolar charge transport and extraordinarily high electron (996 cm2 V−1 s−1) and hole (501 cm2 V−1 s−1) mobilities, surpassing the performance of most pristine organic materials without doping. These results demonstrate their vast potential for applications in thin‐film optoelectronic devices.

Planar two-dimensional (2D) layered materials such as graphene, metal-organic frameworks, and covalent-organic frameworks are attracting enormous interest in the scientific community because of their unique properties and potential applications. One common feature of these materials is that their building blocks (monomers) are flat and lie in planar 2D structures, with interlayer π-π stacking, parallel to the stacking direction. Due to layer-to-layer confinement, their segmental motion is very restricted, which affects their sorption/desorption kinetics when used as sorbent materials. Here, to minimize this confinement, a vertical 2D layered material was designed and synthesized, with a robust fused aromatic ladder (FAL) structure. Because of its unique structural nature, the vertical 2D layered FAL structure has excellent gas uptake performance under both low and high pressures, and also a high iodine (I 2) uptake capacity with unusually fast kinetics, the fastest among reported porous organic materials to date.

There have been extensive efforts to synthesize crystalline covalent triazine‐based frameworks (CTFs) for practical applications and to realize their potential. The phosphorus pentoxide (P2O5)‐catalyzed direct condensation of aromatic amide instead of aromatic nitrile to form triazine rings. P2O5‐catalyzed condensation was applied on terephthalamide to construct a covalent triazine‐based framework (pCTF‐1). This approach yielded highly crystalline pCTF‐1 with high specific surface area (2034.1 m2 g−1). At low pressure, the pCTF‐1 showed high CO2 (21.9 wt % at 273 K) and H2 (1.75 wt % at 77 K) uptake capacities. The direct formation of a triazine‐based COF was also confirmed by model reactions, with the P2O5‐catalyzed condensation reaction of both benzamide and benzonitrile to form 1,3,5‐triphenyl‐2,4,6‐triazine in high yield.