What question did this study set out to answer?

The aim is to improve the efficiency of H2O2 synthesis using tailored interlayer interactions in g-C3N4 nanosheets.

April 3, 2026Catalysts0 citationsOpen Access

Tailoring Interlayer Interactions to Construct Ultrathin g-C3N4 Nanosheets for Efficient H2O2 Photosynthesis

LYLiantao YangKunming University of Science and Technology YLYuanzhe LiKunming University of Science and Technology BZBin ZhangKunming University of Science and Technology

Puntos clave

The aim is to improve the efficiency of H2O2 synthesis using tailored interlayer interactions in g-C3N4 nanosheets.
Developed ultrathin g-C3N4 nanosheets through topology-directed strategy.
Measured photocatalytic performance of the nanosheets under visible light.
Conducted water contact angle, FTIR, and EPR spectroscopy for characterization.
Assessed charge transfer dynamics using Kelvin probe force microscopy (KPFM).
Achieved an H2O2 production rate of 1.34 mmol g−1 h−1, 2.48 times higher than bulk g-C3N4.
Engineered nanosheets showed improved hydrophilicity, enhancing mass transfer.
Optimized adsorption configuration of *OOH intermediate led to increased •O2− and •OH radical generation.
Induced robust internal electric field reduced charge recombination and extended exciton lifetime by a factor of 1.249.

Resumen

Photocatalytic H2O2 synthesis emerges as a promising green substitute for the energy-intensive anthraquinone process, yet its efficiency is limited by rapid charge recombination and limited surface active sites in bulk polymeric semiconductors. Herein, we report a topology-directed strategy to tailor the interlayer interactions of graphitic carbon nitride (g-C3N4), yielding ultrathin nanosheets with optimized electronic structures. The resulting catalyst exhibits an exceptional H2O2 production rate of 1.34 mmol g−1 h−1 under visible light, surpassing bulk g-C3N4 by a factor of 2.48. Water contact angle measurements confirm the superior hydrophilicity of the engineered nanosheets, facilitating interfacial mass transfer, while in situ FTIR and EPR spectroscopies unravel that the abundant exposed active sites optimize the adsorption configuration of the key *OOH intermediate and promote the generation of •O2− and •OH radicals. Regarding charge transfer dynamics, in situ EPR trapping experiments and Kelvin probe force microscopy (KPFM) reveal that the attenuated interlayer coupling induces a robust internal electric field, effectively suppressing carrier recombination and prolonging the exciton lifetime by a factor of 1.249. This work establishes a quantitative structure–activity relationship between interlayer engineering and exciton dynamics, offering a reliable protocol for the rational design of high-performance molecular photocatalysts.

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