Synthesis of propylene carbonate from urea and 1,2-propylene glycol over MnO2/γ-Al2O3 catalyst modified by NaOH

doi:10.3969/j.issn.0438-1157.2014.11.017

CIESC Journal ›› 2014, Vol. 65 ›› Issue (11): 4333-4339.DOI: 10.3969/j.issn.0438-1157.2014.11.017

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Synthesis of propylene carbonate from urea and 1,2-propylene glycol over MnO₂/γ-Al₂O₃ catalyst modified by NaOH

DU Zhiping, LIN Zhikun, CHEN Fangsheng, HU Xingxing, DING Yigang, CHI Ru'an, WU Yuanxin

Key Laboratory for Green Chemical Process of Ministry of Education, Hubei Novel Reactor and Green Chemical Technology Key Laboratory, Wuhan Institute of Technology, Wuhan 430074, Hubei, China

Received:2014-03-04 Revised:2014-04-30 Online:2014-11-05 Published:2014-11-05
Supported by:
supported by the National Natural Science Foundation of China (21276201) and the Collaborative Innovation Project of Hubei Province (010846).

NaOH改性MnO₂/γ-Al₂O₃催化尿素醇解合成碳酸丙烯酯

杜治平, 林志坤, 陈方胜, 胡星星, 丁一刚, 池汝安, 吴元欣

武汉工程大学绿色化工过程教育部重点实验室, 湖北省新型反应器与绿色化学工艺重点实验室, 湖北武汉 430074

通讯作者: 杜治平
基金资助:
国家自然科学基金项目(21276201);湖北省协同创新项目(010846).

Abstract

Abstract: MnO₂/γ-Al₂O₃ catalyst was prepared by ultrasonic impregnation and modified by alkali or salt. The modified MnO₂/γ-Al₂O₃ was characterized by X-ray diffraction (XRD), temperature-programmed desorption of CO₂(CO₂-TPD). Catalytic performances were investigated in urea alcoholysis to propylene carbonate (PC). The activity of MnO₂/γ-Al₂O₃ catalyst modified by NaOH was the best. At the same time, calcination temperature, calcination time and amount of NaOH affected the quantity and intensity of basic activity centers on the surface of the modified catalyst. The increase of moderately basic activity center was the main reason for the catalyst activity improvement after modification. When the MnO₂/γ-Al₂O₃ catalyst was modified by 10% NaOH, and calcined at 400℃ for 2 h, the quantity of moderately basic activity center on the surface was the most, which led to the highest activity. Yield and selectivity of PC were up to 86.9% and 91.8%, respectively.

Key words: propylene carbonate, urea, catalysis, alumina, surface, modified

摘要： 采用超声浸渍法制备了MnO₂/γ-Al₂O₃催化剂,并用碱和盐对其进行了改性.采用X射线衍射仪(XRD)、CO₂-TPD对改性后的MnO₂/γ-Al₂O₃催化剂进行了表征,研究了改性后催化剂在尿素醇解合成碳酸丙烯酯(PC)反应中的催化性能.研究结果表明,NaOH改性MnO₂/γ-Al₂O₃催化剂具有最好的催化性能;同时催化剂的焙烧时间、焙烧温度以及NaOH改性量影响催化剂表面碱性活性中心的数量和强度,其中中强碱的增加是改性后催化剂活性提高的主要原因.在NaOH用量为MnO₂质量的10%,400℃焙烧2h后,改性MnO₂/γ-Al₂O₃催化剂表面的中强碱量最大,催化活性最高,PC收率与选择性分别达86.9%、91.8%.

关键词: 碳酸丙烯酯, 尿素, 催化, 氧化铝, 表面, 改性

CLC Number:

DU Zhiping, LIN Zhikun, CHEN Fangsheng, HU Xingxing, DING Yigang, CHI Ru'an, WU Yuanxin. Synthesis of propylene carbonate from urea and 1,2-propylene glycol over MnO₂/γ-Al₂O₃ catalyst modified by NaOH[J]. CIESC Journal, 2014, 65(11): 4333-4339.

杜治平, 林志坤, 陈方胜, 胡星星, 丁一刚, 池汝安, 吴元欣. NaOH改性MnO₂/γ-Al₂O₃催化尿素醇解合成碳酸丙烯酯[J]. 化工学报, 2014, 65(11): 4333-4339.

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Synthesis of propylene carbonate from urea and 1,2-propylene glycol over MnO₂/γ-Al₂O₃ catalyst modified by NaOH

NaOH改性MnO₂/γ-Al₂O₃催化尿素醇解合成碳酸丙烯酯

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