Dual molecules engineered carbon nitride for achieving outstanding photocatalytic H2O2 production

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Molecular engineering of carbon nitride (CN) was considered as a suitable and compelling strategy to overcome the intrinsic imperfections and enhance photocatalytic H2O2 production. However, the photocatalytic H2O2 production of conventional single molecular engineering is still unsatisfactory, and the comprehension of photogenerated carrier migration and separation is still indistinct. Herein, dual molecules were engineered on CN molecular skeleton for achieving an outstanding photocatalytic rate of H2O2 production. The photocatalytic H2O2 production rate of the dual molecules engineered CN was up to 3320 μmol g−1 h−1, which was approximately 25 times than that of the pristine CN. After the dual-molecular engineering, pyrimidine and cyano group were co-grafted. Synchronously, K ion and Na ion were co-embedded near the interlamination of CN layers. The synergistic effect of the dual molecules in CN not only restrained photogenerated carrier recombination and broadened visible light response by modulating the intrinsic energy band structure, but also enhanced the capture of the photogenerated electrons and accelerated the migration of proton. Hence, the photocatalytic 2e- oxygen reduction reaction, the rate-determining step, was significantly strengthened. Additionally, caused by the positive valence band potential, the H2O oxidation reaction became an indispensable role in photocatalytic H2O2 production. This work provided a viable route to modulate the molecular skeleton of organic semiconductors and presented a promising strategy to obtain high-efficient photocatalytic H2O2 production.