Enhancing H₂O₂ Photocatalytic Production via Increased Triazine Moiety Content in the Skeleton of Covalent Triazine Framework

Photocatalytic hydrogen peroxide (H 2 O 2 ) synthesis offers a promising alternative through direct solar energy utilization. Covalent Triazine Frameworks (CTFs) have emerged as effective photocatalysts due to their structural integrity and nitrogen‐rich composition. However, although it is generally considered that increasing the content of triazine moiety in the skeleton is beneficial for improving photocatalytic reaction efficiency, there is still a lack of more direct experimental evidence. In this study, we present the first design of a unique CTF and achieve precise control over the density of triazine units in the CTF skeleton through rational structural design. Further experiments demonstrate the direct impact of triazine content on H 2 O 2 photosynthesis. Photocatalytic assessments reveal that for this unique structure, CTF‐Th achieves 3.4 times higher than CTF‐T with lower triazine content. This work introduces triazine ring concentration as a critical design parameter and establishes its relationship with photocatalytic performance, providing valuable insights for the rational design of advanced photocatalysts.