Catalysis Today ( IF 5.2 ) Pub Date : 2018-08-17 , DOI: 10.1016/j.cattod.2018.08.003 Siddulu Naidu Talapaneni , Kavitha Ramadass , Sujanya J. Ruban , Mercy Benzigar , Kripal S. Lakhi , Jae-Hun Yang , Ugo Ravon , Khalid Albahily , Ajayan Vinu
A novel highly ordered three dimensional mesoporous graphitic carbon nitride (MGCN-6) with C3N4 stoichiometry having amorphous wall structure, tunable textural parameters with body-centered cubic Ia3d framework has been prepared from 3D mesoporous silica, KIT-6 with adjustable pore diameters as hard templates through a temperature-induced poly condensation followed by the polymerization reaction of cyanamide (CNNH2) precursor. The structure of the resulting mesoporous graphitic carbon nitride materials consists of sheets of three-dimensionally arranged s-heptazine units that are held together by covalent bonds between C and N atoms. The realized MGCN-6 materials have been thoroughly characterized using various techniques such as powder X-ray diffraction (XRD), N2 physisorption, high-resolution transmission electron microscopy (HRTEM), field emission scanning electron microscopy (FESEM), X-ray photoelectron spectroscopy (XPS), UV–vis and Fourier transform infrared (FT-IR) spectroscopy, and elemental analysis. The characterization data reveal that the resultant materials possess a well-defined ordered three-dimensional porous structure with a high surface area and a large pore volume. The catalytic activity of these materials has been tested in the Knoevenagel condensation between benzaldehyde and malononitrile. This catalyst is found to be highly active and shows a high conversion with 100% product selectivity even at room temperature.
中文翻译:
源自KIT-6的具有可调孔径的3D立方介孔C 3 N 4及其在碱催化的Knoevenagel反应中的应用
用3D介孔二氧化硅,孔度可调的KIT-6制备了具有无定形壁结构,体心立方Ia3d骨架可调结构参数的C 3 N 4化学计量的新型高度有序的三维介孔石墨碳氮化物(MGCN-6)。通过温度诱导的缩聚反应,然后进行氰酰胺(CNNH 2)的前体。所得的中孔石墨碳氮化物材料的结构由三维排列的S-庚嗪单元薄片组成,这些薄片通过C和N原子之间的共价键结合在一起。使用各种技术(例如粉末X射线衍射(XRD),N 2物理吸附,高分辨率透射电子显微镜(HRTEM),场发射扫描电子显微镜(FESEM),X射线光电子能谱(XPS),紫外可见和傅里叶变换红外(FT-IR)光谱以及元素分析。表征数据表明,所得材料具有高表面积和大孔体积的明确定义的有序三维多孔结构。这些材料的催化活性已在苯甲醛和丙二腈之间的Knoevenagel缩合反应中进行了测试。发现该催化剂是高活性的,甚至在室温下也显示出高转化率和100%的产物选择性。