负载型KI催化甘油与CO2合成甘油碳酸酯

doi:10.16085/j.issn.1000-6613.2015.02.016

化工进展 ›› 2015, Vol. 34 ›› Issue (02): 402-406,412.DOI: 10.16085/j.issn.1000-6613.2015.02.016

负载型KI催化甘油与CO₂合成甘油碳酸酯

王富丽¹, 黄世勇¹, 余青云², 黄媚¹, 孙果宋¹

1. 广西壮族自治区化工研究院, 广西南宁 530006;
2. 广西大学化学化工学院, 广西南宁 530004

收稿日期:2014-05-16 修回日期:2014-09-21 出版日期:2015-02-05 发布日期:2015-02-05
通讯作者: 黄世勇,博士,高级工程师。E-mail:shiyonghuang@163.com
作者简介:王富丽(1976-),女,硕士,工程师,研究方向为绿色化学
基金资助:
广西自然科学基金项目(2011GXNSFA018053)

Synthesis of glycerol carbonate from glycerol and CO₂ by supported KI catalysts

WANG Fuli¹, HUANG Shiyong¹, YU Qingyun², HUANG Mei¹, SUN Guosong¹

1. Guangxi Research Institute of Chemical Industry, Nanning 530006, Guangxi, China;
2. School of Chemistry and Chemical Engineering, Guangxi University, Nanning 530004, Guangxi, China

Received:2014-05-16 Revised:2014-09-21 Online:2015-02-05 Published:2015-02-05

摘要/Abstract

摘要： 添加不同组分对氧化铝载体进行调变改性,再以改性氧化铝为载体,负载KI制备了一系列负载型催化剂KI/Al₂O₃-MgO、KI/Al₂O₃-ZnO、KI/Al₂O₃-TiO₂和KI/Al₂O₃-ZrO₂,并通过CO₂、环氧丙烷和甘油合成甘油碳酸酯反应评价其催化活性,发现KI/Al₂O₃-MgO具有最高的活性。由不同载体的CO₂-TPD分析可以发现,载体表面少量碱性位的存在有利于反应进行。实验研究了不同负载量KI/Al₂O₃-MgO的活性及稳定性,发现KI负载量为1.5mmol/g较为适宜。同时,实验又通过N₂吸附/脱附(BET)、X射线衍射(XRD)等手段对不同负载量的KI/Al₂O₃-MgO进行了表征,进一步说明了负载量过多会导致KI晶粒团聚,并阻塞载体孔道。优化了反应条件,在最佳条件下(环氧丙烷0.3mol,甘油0.1mol,反应温度130℃,反应时间2h,反应压力6.0MPa),甘油的转化率为65.5%,甘油碳酸酯的产率为60.8%。

关键词: 甘油, 二氧化碳, 催化, 甘油碳酸酯, 多相反应

Abstract: Different components were chosen to modify alumina and then KI was loaded on the surface of modified alumina,and a series of supported KI catalysts were prepared,such as KI/Al₂O₃-MgO,KI/Al₂O₃-ZnO,KI/Al₂O₃-TiO₂ and KI/Al₂O₃-ZrO₂. The catalytic activities were evaluated by the reaction of CO₂,propylene epoxide and glycerol to synthesize glycerol carbonate and KI/Al₂O₃-MgO was found to be the best one. Through CO₂-TPD of diffirent supports,it could be found that a few basic positions on the surface of supports were favorable to the reaction. The catalytic activity and stability of KI/Al₂O₃-MgO with different loading amounts were investigated and the optimal loading amount of KI was 1.5mmol/g. At the same time,KI/Al₂O₃-MgO was characterized by N₂ adsorption/desorption (BET) and X ray diffraction (XRD). Overfull loading amount could lead to agglomeration of KI crystals and blockage of support pores. Reaction conditions were optimized. Under the optimal conditions (propylene oxide 0.3mol,glycerol 0.1mol,reaction temperature 130℃,reaction time 2h,and reaction pressure 6.0MPa),conversion of glycerol was 65.5% and yield of glycerol carbonate was 60.8%.

Key words: glycerol, carbon dioxide, catalysis, glycerol carbonate, multiphase reaction

中图分类号:

TQ426.8

王富丽, 黄世勇, 余青云, 黄媚, 孙果宋. 负载型KI催化甘油与CO₂合成甘油碳酸酯[J]. 化工进展, 2015, 34(02): 402-406,412.

WANG Fuli, HUANG Shiyong, YU Qingyun, HUANG Mei, SUN Guosong. Synthesis of glycerol carbonate from glycerol and CO₂ by supported KI catalysts[J]. Chemical Industry and Engineering Progree, 2015, 34(02): 402-406,412.

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负载型KI催化甘油与CO₂合成甘油碳酸酯

Synthesis of glycerol carbonate from glycerol and CO₂ by supported KI catalysts

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