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.

Developing efficient and durable electrocatalysts is key to optimizing the electrocatalytic hydrogen evolution reaction (HER), currently one of the cleanest and most sustainable routes for producing hydrogen. Here, a unique and efficient approach to fabricate and embed uniformly dispersed Ir nanoparticles in a 3D cage‐like organic network (CON) structure is reported. These uniformly trapped Ir nanoparticles within the 3D CON (Ir@CON) effectively catalyze the HER process. The Ir@CON electrocatalyst exhibits high turnover frequencies of 0.66 and 0.20 H2 s−1 at 25 mV and small overpotentials of 13.6 and 13.5 mV while generating a current density of 10 mA cm−2 in 0.5 m H2SO4 and 1.0 m KOH aqueous solutions, respectively, as compared to commercial Pt/C (18 and 23 mV) and Ir/C (20.7 and 28.3 mV). More importantly, the catalyst shows superior stability in both acidic and alkaline media. These results highlight a potentially powerful approach for the design and synthesis of efficient and durable electrocatalysts for HER.

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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.

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