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Uracil-Doped Graphitic Carbon Nitride for Enhanced Photocatalytic Performance

机译:尿嘧啶掺杂的石墨氮化物,用于增强光催化性能

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摘要

g-C_(3)N_(4) is a visible-light photocatalyst with a suitable band gap and good stability. Moreover, g-C_(3)N_(4) is considered to be earth-abundant, which makes it an appealing photocatalyst. However, due to its small specific surface area, low utilization of visible light, and high photogenerated electron–hole pair recombination rate, the photocatalytic activity of g-C_(3)N_(4) remains unsatisfactory. In this work, a highly efficient nonmetallic photocatalyst, i.e ., g-C_(3)N_(4) doped with uracil (denoted U-C_(3)N_(4)) was successfully developed. Based on the various characterizations and calculations, it is shown that the triazine group in g-C_(3)N_(4) is replaced with the diazine group in uracil. This occurrence leads to the formation of a new electron-transfer pathway between triazine groups, which can promote the separation of photogenerated electrons and holes. Concurrently, due to the ultrathin structure of the as-prepared U-C_(3)N_(4), the material possessed a larger specific surface area than pristine g-C_(3)N_(4), which can provide more active sites. Furthermore, the transfer pathway between the electron and hole was also shortened, and the recombination of the electron and hole was inhibited. According to the results, an optimal hydrogen evolution rate of 31.7 mol h~(–1) g~(–1) was achieved by U-C_(3)N_(4), which is 5.1 times higher as compared to that achieved by pristine g-C_(3)N_(4) (6.26 mol h~(–1) g~(–1)). For the photocatalytic degradation of rhodamine B, the reaction rate constant of U-C_(3)N_(4) (11.3 × 10~(–2) min~(–1)) is about 5.5 times that of g-C_(3)N_(4) (2.07 × 10~(–2) min~(–1)). Furthermore, the uracil-doped catalyst was also able to demonstrate good stability after five successive runs.
机译:g-C_3)N_4是一种具有合适带隙和良好稳定性的可见光光催化剂。此外,g-C_3)N_4被认为富含地球,这使其成为一种诱人的光催化剂。然而,由于其比表面积小、可见光利用率低、光生电子-空穴对复合率高,g-C_3)N_4的光催化活性仍然不令人满意。在这项工作中,一种高效的非金属光催化剂。,成功地研制了尿嘧啶掺杂的g-C_3)N_4(表示为U-C_3)N_4)。基于各种表征和计算,表明g-C_3)N_4中的三嗪基被尿嘧啶中的二嗪基取代。这种现象导致三嗪基团之间形成新的电子转移途径,从而促进光生电子和空穴的分离。同时,由于所制备的U-C_3)N_4的超薄结构,该材料比原始的g-C_3)N_4具有更大的比表面积,从而可以提供更多的活性位点。此外,电子与空穴之间的转移路径也被缩短,电子与空穴的复合受到抑制。结果表明,U-C_3)N_4的最佳析氢速率为31.7mol h~(-1)g~(-1),是原始g-C_3)N_4(6.26mol h~(-1)g~(-1))的5.1倍。对于罗丹明B的光催化降解,U-C_3)N_4(11.3×10~(-2)min~(-1))的反应速率常数约为g-C_3)N_4(2.07×10~(-2)min~(-1))的5.5倍。此外,在连续五次运行后,掺杂尿嘧啶的催化剂也能够表现出良好的稳定性。

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