Boron-carbon-nitrogen-containing heterogeneous catalysts for base-catalyzed reaction
Boron-carbon-nitrogen-containing heterogeneous catalysts for base-catalyzed reaction
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DOI：
10.1016/j.apsusc.2021.149841
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发表时间：
2021-05-01
影响因子：
6.7
通讯作者：
Sato, Kazuyoshi
中科院分区：
文献类型：
--
作者：
Horimoto, Takeru;Kannari, Naokatsu;Sato, Kazuyoshi
为了推进绿色化学，进一步开发非均相碱催化剂而不是均相催化剂是必不可少的。在这项研究中，硼-碳-氮（BCN）的含材料的制备和用作非均相催化剂的碱催化反应。通过在不同温度（600、800和1000 ℃）和BCl 3浓度（0.1、0.5和1.0%）下热处理聚丙烯腈来制备BCN材料，以控制BCN材料的组成。采用X射线衍射仪、傅里叶变换红外光谱仪、X射线光电子能谱仪和N2吸附-脱附仪对样品进行了表征。我们使用苯甲醛与氰基乙酸乙酯的Knoevenagel反应生成氰基肉桂酸乙酯（ECC）来评价样品的催化活性。通过在制备过程中引入较高浓度的BCl 3，获得了较高的表面硼和氮组成，这提高了ECC产率。此外，B-N-C型氮的表面比率与ECC产量相关。Knoevenagel反应的循环测试表明，BCN材料随着运行次数的增加而逐渐失活，这归因于B-N位点的水解。
To advance green chemistry, further development of heterogeneous base catalysts rather than homogeneous catalysts is essential. In this study, boron-carbon-nitrogen (BCN)-containing materials were prepared and used as heterogeneous catalysts for a base-catalyzed reaction. The BCN materials were prepared by heat treatment of polyacrylonitrile at various temperatures (600, 800, and 1000 C) and BCl3 concentrations (0.1, 0.5, and 1.0%) to control the composition of the BCN materials. The prepared samples were characterized by X-ray diffractometry, Fourier-transform infrared spectroscopy, X-ray photoelectron spectroscopy, and N2 adsorption-desorption measurement. We evaluated the catalytic activity of the samples using the Knoevenagel reaction of benzaldehyde with ethyl cyanoacetate to produce ethyl cyanocinnamate (ECC). Higher surface compositions of boron and nitrogen were obtained by introducing higher concentrations of BCl3 in the preparation process, which increased the ECC yield. Furthermore, the surface ratio of B-N-C-type nitrogen correlated with the ECC yield. The recycling test of the Knoevenagel reaction indicated that the BCN material gradually deactivated with increasing the number of runs, which is attributed to hydrolysis of the B-N site.