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Post-Synthetic Derivatization of Graphitic Carbon Nitride with Methanesulfonyl Chloride: Synthesis Characterization and Photocatalysis

机译:甲磺酰氯对石墨化氮化碳的后合成衍生反应:合成表征和光催化

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摘要

Bulk graphitic carbon nitride (CN) was synthetized by heating of melamine at 550 °C, and the exfoliated CN (ExCN) was prepared by heating of CN at 500 °C. Sulfur-doped CN was synthesized by heating of thiourea (S-CN) and by a novel procedure based on the post-synthetic derivatization of CN with methanesulfonyl (CH SO ) chloride (Mes-CN and Mes-ExCN). The obtained nanomaterials were investigated by common characterization methods and their photocatalytic activity was tested by means of the decomposition of acetic orange 7 (AO7) under ultraviolet A (UVA) irradiation. The content of sulfur in the modified CN decreased in the sequence of Mes-ExCN > Mes-CN > S-CN. The absorption of light decreased in the opposite manner, but no influence on the band gap energies was observed. The methanesulfonyl (mesyl) groups connected to primary and secondary amine groups were confirmed by high resolution mass spectrometry (HRMS). The photocatalytic activity decreased in the sequence of Mes-ExCN > ExCN > CN ≈ Mes-CN > S-CN. The highest activity of Mes-ExCN and ExCN was explained by the highest amounts of adsorbed Acetic Orange 7 (AO7). In addition, in the case of Mes-ExCN, chloride ions incorporated in the CN lattice enhanced the photocatalytic activity as well.
机译:通过在550℃下加热三聚氰胺来合成块状石墨氮化碳(CN),并且通过在500℃下加热CN来制备剥离的CN(ExCN)。通过加热硫脲(S-CN)并基于基于CN的甲烷磺酰氯(CH SO)的合成后衍生化的新方法(Mes-CN和Mes-ExCN)合成掺杂硫的CN。通过常用的表征方法对所得纳米材料进行了研究,并通过紫外A(UVA)照射下的乙酸橙7(AO7)的分解来测试其光催化活性。修饰的CN中的硫含量按Mes-ExCN> Mes-CN> S-CN的顺序降低。光的吸收以相反的方式降低,但是没有观察到对带隙能量的影响。通过高分辨率质谱(HRMS)证实了与伯胺和仲胺基相连的甲磺酰基(甲磺酰基)。 Mes-ExCN> ExCN> CN≈Mes-CN> S-CN的顺序降低了光催化活性。 Mes-ExCN和ExCN的最高活性由吸附的乙酸橘红7(AO7)的最高含量解释。另外,在Mes-ExCN的情况下,结合在CN晶格中的氯离子也增强了光催化活性。

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