Zn-Ca-Al mixed oxide as efficient catalyst for synthesis of propylene carbonate from urea and 1, 2-propylene glycol

doi:10.1016/j.cjche.2016.11.003

›› 2017, Vol. 25 ›› Issue (5): 609-616.DOI: 10.1016/j.cjche.2016.11.003

• Catalysis, Kinetics and Reaction Engineering • 上一篇下一篇

Zn-Ca-Al mixed oxide as efficient catalyst for synthesis of propylene carbonate from urea and 1, 2-propylene glycol

Sen Liu^1,2, Suhong Sun², Xuehui Tian², Peiyong Sun², Shenghong Zhang², Zhilong Yao²

1 College of Chemical Engineering, Sichuan University, Chengdu 610065, China;
2 Beijing Key Laboratory of Enze Biomass Fine Chemicals, College of Chemical Engineering, Beijing Institute of Petrochemical Technology, Beijing 102617, China

收稿日期:2016-08-25 修回日期:2016-11-04 出版日期:2017-05-28 发布日期:2017-07-06
通讯作者: Shenghong Zhang,E-mail address:zshong@bipt.edu.cn
基金资助:
Supported by the Changcheng Scholars Program of Beijing (CIT&TCD 20150316).

Zn-Ca-Al mixed oxide as efficient catalyst for synthesis of propylene carbonate from urea and 1, 2-propylene glycol

Sen Liu^1,2, Suhong Sun², Xuehui Tian², Peiyong Sun², Shenghong Zhang², Zhilong Yao²

1 College of Chemical Engineering, Sichuan University, Chengdu 610065, China;
2 Beijing Key Laboratory of Enze Biomass Fine Chemicals, College of Chemical Engineering, Beijing Institute of Petrochemical Technology, Beijing 102617, China

Received:2016-08-25 Revised:2016-11-04 Online:2017-05-28 Published:2017-07-06
Supported by:
Supported by the Changcheng Scholars Program of Beijing (CIT&TCD 20150316).

摘要/Abstract

摘要： A series of Zn-Ca-Al oxides with different CaO and ZnO contents have been prepared and evaluated in the synthesis of propylene carbonate (PC) from 1,2-propylene glycol (PG) and urea in a batch reactor. The effect of catalyst composition, basicity and reaction process parameters such as temperature, catalyst dose, molar ratio of PG to urea, purge gas flow and reaction time has been studied to find suitable reaction conditions for the PC synthesis. The PC selectivity and yield under the desired conditions could reach 98.4% and 90.8%, respectively. The best performing catalyst also exhibited a good reusability without appreciable loss in the PC selectivity and yield after five consecutive reaction runs. In addition, a stepwise reaction pathway involving a 2-hydroxypropyl carbamate intermediate was proposed for the urea alcoholysis to PC in the presence of Zn-Ca-Al catalysts, according to the time dependences of reaction intermediates and products.

关键词: Propylene carbonate, 1,2-Propylene glycol, Urea, Catalysis, Alcoholysis

Abstract: A series of Zn-Ca-Al oxides with different CaO and ZnO contents have been prepared and evaluated in the synthesis of propylene carbonate (PC) from 1,2-propylene glycol (PG) and urea in a batch reactor. The effect of catalyst composition, basicity and reaction process parameters such as temperature, catalyst dose, molar ratio of PG to urea, purge gas flow and reaction time has been studied to find suitable reaction conditions for the PC synthesis. The PC selectivity and yield under the desired conditions could reach 98.4% and 90.8%, respectively. The best performing catalyst also exhibited a good reusability without appreciable loss in the PC selectivity and yield after five consecutive reaction runs. In addition, a stepwise reaction pathway involving a 2-hydroxypropyl carbamate intermediate was proposed for the urea alcoholysis to PC in the presence of Zn-Ca-Al catalysts, according to the time dependences of reaction intermediates and products.

Key words: Propylene carbonate, 1,2-Propylene glycol, Urea, Catalysis, Alcoholysis

Sen Liu, Suhong Sun, Xuehui Tian, Peiyong Sun, Shenghong Zhang, Zhilong Yao. Zn-Ca-Al mixed oxide as efficient catalyst for synthesis of propylene carbonate from urea and 1, 2-propylene glycol[J]. , 2017, 25(5): 609-616.

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Zn-Ca-Al mixed oxide as efficient catalyst for synthesis of propylene carbonate from urea and 1, 2-propylene glycol

Zn-Ca-Al mixed oxide as efficient catalyst for synthesis of propylene carbonate from urea and 1, 2-propylene glycol

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