蜜勒胺催化剂的制备及在环碳酸酯合成中的应用研究

Study on the synthesis of melem catalyst and its application in synthesis of cyclic carbonate

摘要: 以纳米二氧化硅 (SiO₂) 为模板，以三聚氰胺为前驱体，采用固相反应法制备一系列介孔蜜勒胺 (melem) 材料。通过调控硬模板剂和前驱体的用量，最终得到一系列高比表面积 (40−92 m²/g) 和孔体积 (0.179−0.407 cm³/g)的介孔 melem材料。将其作为催化剂用于1, 4 -丁二醇二缩水甘油醚 (BDODGE) 与CO₂的环加成反应中，结果表明，随着比表面积增大，催化剂活性相比未加入模板剂的melem样品有了显著提高。三聚氰胺与纳米SiO₂的质量比为2时制备的催化剂，在130 ℃、20 h、2.0 MPa条件下，BDODGE转化率为99.3%，环碳酸酯选择性为99.5%。

Abstract: In this paper, a series of mesoporous melem materials were prepared from melamine by solid-phase reaction using nano-silica (SiO₂) as the template. The mesoporous melem materials with high specific surface area (40−92 m²/g) and pore volume (0.179−0.407 cm³/g) were obtained by adjusting the ratio of SiO₂ template and melamine. The obtained melem was used as catalyst for the cycloaddition reaction between BDODGE and CO₂. The results showed that the catalytic activity was greatly improved with the increase of specific surface area of the catalysts. The catalyst mp-CN-450-2 showed the best performance. After 20 h reaction at 130 ºC, 2.0 MPa, 99.3% of BDODGE conversion and 99.5% of cyclic carbonate selectivity were acquired, respectively.