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

以纳米二氧化硅(SiO_(2))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 m^(2)/g)和孔体积(0.179−0.407 cm^(3)/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CO_(2)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SiO_(2)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%。

In this paper,a series of mesoporous melem materials were prepared from melamine by solid-phase reaction using nano-silica(SiO_(2))as the template.The mesoporous melem materials with high specific surface area(40−92 m^(2)/g)and pore volume(0.179−0.407 cm^(3)/g)were obtained by adjusting the ratio of SiO_(2) template and melamine.The obtained melem was used as catalyst for the cycloaddition reaction between BDODGE and CO_(2).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℃,2.0 MPa,99.3%of BDODGE conversion and 99.5%of cyclic carbonate selectivity were acquired,respectively.