Rational copolymerization strategy engineered C self-doped g-C3N4 for efficient and robust solar photocatalytic H2 evolution
2021
Liu, Enli | Lin, Xue | Hong, Yuanzhi | Yang, Lan | Luo, Bifu | Shi, Weilong | Shi, Junyou
Graphitic carbon nitride (g-C₃N₄) with unique physicochemical features has garnered much attention in artificial photosynthesis, yet the photoactivity of pristine g-C₃N₄ (PCN) is severely restricted because of its rapid charge recombination rate and narrow visible-light absorption. To this end, for the first time, here we reported a rational one-step copolymerization strategy for the fabrication of carbon self-doped g-C₃N₄ (CCN) by using melamine and chitosan as the starting materials. Experimental results indicated that the bridged N atoms were substituted by C atoms in the g-C₃N₄ matrix, resulting in the formation of delocalized big π bonds, thereby the obviously increased the electrical conductivity, remarkably extended the visible-light absorption region, and significantly improved the mobility of photoinduced electron-hole pairs. Consequently, the as-engineered CCN with abundant mesopores structure showed a dramatically boosting photocatalytic H₂-evolved activity (1224 μmol g⁻¹ h⁻¹), 4.5-folds than PCN powders. Eventually, the resulting CCN exhibited an extremely long-term durable stability after storing in reaction solution for 90 days. Our work will bring about potential application in designing of high-performance g-C₃N₄ photocatalyst for renewable solar-to-H₂ conversion.
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