Molecular Benzene‐Heptazine Junction Over Carbon Nitride Frameworks for Dual‐Pathway Photosynthesis of Hydrogen Peroxide

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Abstract
Tailoring polymeric carbon nitride (CN) to simultaneously broaden its light absorption range and improve charge carrier mobility remains a key challenge for photocatalytic H 2 O 2 production. The molecular junction strategy has been proven to be an effective approach to address the aforementioned challenges. In this work, we developed a molecular junction through controlled thermal ring‐opening isomerization of benzoguanamine, thereby creating a well‐defined C‐C‐bridged benzene‐heptazine molecular junction. Experimental and theoretical studies reveal that: (1) Benzene functionalization extends the π‐conjugation, enabling n→π* transitions for broad‐spectrum absorption; (2) The donor‐acceptor structure enhances self‐polarization effects, strengthening the built‐in electric field for efficient charge separation; (3) The unique molecular architecture overcomes traditional kinetic limitations, enabling a dual‐channel H 2 O 2 synthesis mechanism. The optimized catalyst achieves remarkable production rates of 5222 µmol∙g − 1 ∙h − 1 in isopropanol/water and 1587 µmol∙g −1 ∙h −1 in pure water, representing 13.1‐fold and 32.4‐fold improvements over pristine CN, respectively. This work advances molecular‐scale design of photocatalysts and offers new strategies for artificial photosynthesis.
Funding Information
  • Natural Science Foundation of Jiangsu Province (BK20240332)
  • National Natural Science Foundation of China (22578376)
  • National Natural Science Foundation of China (52570130)

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