Facile synthesis of few-layer-thick carbon nitride nanosheets by liquid ammonia-assisted lithiation method and their photocatalytic redox properties

Abstract

High-quality few-layer-thick graphitic carbon nitride (g-C₃N₄) nanosheets (NSs) were fabricated by a simple, highly efficient, and rapid method namely, liquid ammonia (LA)-assisted lithiation. Li intercalation occurred in less than half an hour, importantly, the degree of Li intercalation was indicated by the color change of LA solution from deep blue to colorless. The obtained products were carefully investigated by field-emission transmission electron microscopy, field-emission scanning electron microscopy, atomic force microscopy, X-ray powder diffraction, X-ray photoelectron spectroscopy, Raman scattering spectrometry, UV-visible absorption spectrometry, photoluminescence, soft X-ray absorption and nonresonant soft X-ray emission spectroscopy, and X-ray absorption near-edge structure analyses. Because of the lack of high-temperature or high-energy treatment, high-yield few-layer-thick g-C₃N₄ NSs were produced with trace O₂ impurity. Interestingly, while maintaining the similar crystal structure and chemical stoichiometric ratio relative to the parent bulk materials, the surface structure, electronic and optical properties were significantly varied. Moreover, compared to the bulk counterparts, the as-prepared g-C₃N₄ NSs show clearly enhanced photocatalytic redox activity with respect to both photocatalytic H₂ evolution and hydroxyl radical generation. LA-assisted lithiation is a general method and could be easily extended to exfoliate diverse other layered materials such as molybdenum and tungsten sulfides.