A highly nitrogen-deficient g-C3N4 (AH-CN) nanosheets material was successfully prepared by acetaldehyde assisted hydrothermal route. The as-prepared AH-CN material was analyzed by a series of X-ray powder diffraction (XRD), N2 physical adsorption-desorption, scanning electron microscope (SEM), Transmission electron microscope (TEM), Energy disperse spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), photoluminescence (PL), Fourier transform infrared spectroscopy (FT-IR), UV–vis diffuse reflectance spectra (UV-Vis DRS), elemental analysis (EA), electron paramagnetic resonance (EPR) and photoelectric test. Compared with H-CN (g-C3N4 treated by hydrothermal without acetaldehyde), the high nitrogen vacancy was produced over AH-CN(g-C3N4 treated in acetaldehyde assisted hydrothermal condition).The bandgap of AH-CN decreases and its light absorption was largely improved in UV and visible light region. Moreover, low recombination rate of photogenerated carriers and possesses a relatively negative conduction band potential over AH-CN, which contributes to its strong photocatalytic reduction ability. Under simulated sunlight illumination, and the photocatalytic performance for H2O2 production and Cr(VI) reduction of the AH-CN material was evaluated. The highest H2O2 yield of 670 μM was obtained over 50AH-CN, which was 2.6 times of that of g-CN. In removal of Cr(VI) via reduction and the removal rate for Cr(VI) over 50AH-CN reaches 56% which is about 5.6 times of the g-CN.

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