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Facile alkali-assisted synthesis of g-C3N4 materials and their high-performance catalytic application in solvent-free cycloaddition of CO2 to epoxides

机译:容易碱辅助合成G-C3N4材料及其在无溶剂环形加成二氧化碳至环氧化物中的高性能催化应用

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A series of graphitic carbon nitride materials were synthesized using guanidine hydrochloride (GndCl) as a precursor with the aid of alkali treatment. The introduction of alkali successfully enabled GndCl to be transformed into g-C _(3) N _(4) at much lower calcination temperatures (450–475 °C). The g-C _(3) N _(4) samples synthesized under various conditions have been characterized by several techniques including XRD, FT-IR, UV-vis, ~(13) C NMR, and XPS spectroscopy. The results confirmed that the alkali could effectively accelerate further condensation of melem-like fragments to g-C _(3) N _(4) . Meanwhile, a possible mechanism of alkali-assisted synthesis of g-C _(3) N _(4) from GndCl has been proposed. In solvent-free catalytic cycloaddition of CO _(2) to propylene oxide to propylene carbonate (PC), g-C _(3) N _(4) -NaOH and g-C _(3) N _(4) -KOH materials demonstrated high and stable catalytic performances, affording PC yields of ca. 90% under optimized reaction conditions. Moreover, the activities were superior to those obtained over g-C _(3) N _(4) prepared without alkali treatment. In addition, the catalytic activity along with preparation method for the present g-C _(3) N _(4) has also been compared with other reported g-C _(3) N _(4) -based catalysts.
机译:借助于碱处理,使用盐酸胍(GNDCl)作为前体合成一系列石墨碳氮化物材料。在煅烧温度下(450-475°C),将碱的引入成功使GNDCL转化为G-C _(3)N _(4)。在各种条件下合成的G-C _(3)N _(4)样品的特征在于包括XRD,FT-IR,UV-VI,〜(13)C NMR和XPS光谱的若干技术。结果证实,碱可以有效地加速梅尔米片段的进一步冷凝至G-C _(3)N _(4)。同时,提出了来自GNDCl的G-C _(3)N _(4)的碱辅助合成的可能机制。在无溶剂催化环加成的CO _(2)中加环碳酸亚丙酯(PC),GC _(3)N _(4)-NNAOH和GC _(3)N _(4)-KOH材料证明高且稳定的催化性能,得到CA的PC产量。优化反应条件下90%。此外,该活性优于在没有碱处理的情况下通过G-C _(3)N _(4)上获得的那些。另外,还将催化活性与本发明的G-C _(3)N _(4)的制备方法一起与其他报道的G-C _(3)N _(4)的催化剂进行比较。

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