Deactivation mechanism of beta-zeolite catalyst for synthesis of cumene by benzene alkylation with isopropanol

doi:10.1016/j.cjche.2016.11.001

›› 2017, Vol. 25 ›› Issue (9): 1195-1201.DOI: 10.1016/j.cjche.2016.11.001

• Catalysis, kinetics and reaction engineering • 上一篇下一篇

Deactivation mechanism of beta-zeolite catalyst for synthesis of cumene by benzene alkylation with isopropanol

Yefei Liu¹, Yang Zou¹, Hong Jiang¹, Huanxin Gao², Rizhi Chen¹

1 State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, China;
2 SINOPEC Shanghai Research Institute of Petrochemical Technology, Shanghai 201208, China

收稿日期:2016-07-21 修回日期:2016-11-09 出版日期:2017-09-28 发布日期:2017-10-11
通讯作者: Rizhi Chen,E-mail:rizhichen@njtech.edu.cn
基金资助:
Supports by the National Key Research and Development Plan (2016YFB0301503), the Jiangsu Natural Science Foundation for Distinguished Young Scholars (BK20150044), the National Natural Science Foundation of China (91534110, 21606124), the Natural Science Foundation of the Higher Education Institutions of Jiangsu Province (14KJB530004), the Foundation from State Key Laboratory of Materials-Oriented Chemical Engineering (ZK201402, ZK201407), and the Technology Innovation Foundation for Science and Technology Enterprises in Jiangsu Province (BC2015008).

Deactivation mechanism of beta-zeolite catalyst for synthesis of cumene by benzene alkylation with isopropanol

Yefei Liu¹, Yang Zou¹, Hong Jiang¹, Huanxin Gao², Rizhi Chen¹

1 State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, China;
2 SINOPEC Shanghai Research Institute of Petrochemical Technology, Shanghai 201208, China

Received:2016-07-21 Revised:2016-11-09 Online:2017-09-28 Published:2017-10-11
Supported by:
Supports by the National Key Research and Development Plan (2016YFB0301503), the Jiangsu Natural Science Foundation for Distinguished Young Scholars (BK20150044), the National Natural Science Foundation of China (91534110, 21606124), the Natural Science Foundation of the Higher Education Institutions of Jiangsu Province (14KJB530004), the Foundation from State Key Laboratory of Materials-Oriented Chemical Engineering (ZK201402, ZK201407), and the Technology Innovation Foundation for Science and Technology Enterprises in Jiangsu Province (BC2015008).

摘要/Abstract

摘要： The alkylation of benzene with isopropanol over beta-zeolite is a more cost-effective solution to cumene production. During the benzene alkylation cycles, the cumene selectivity slowly increased, while the benzene conversion presented the sharp decrease due to catalyst deactivation. The deactivation mechanism of betazeolite catalyst was investigated by characterizing the fresh and used catalysts. The XRD, SEM and TEM results show that the crystalline and particle size of the beta-zeolite catalyst almost remained stable during the alkylation cycles. The drop in catalytic activity and benzene conversion could be explained by the TG, BET, NH₃-TPD and GC-MS results. The organic matters mainly consisted of ethylbenzene, p-xylene and 1-ethyl-3-(1-methyl) benzene produced in the benzene alkylation deposited in the catalyst, which strongly reduced the specific surface area of beta-zeolite catalyst. Moreover, during the reaction cycles, the amount of acidity also significantly decreased. As a result, the catalyst deactivation occurred. To maintain the catalytic performance, the catalyst regeneration was carried out by using ethanol rinse and calcination. The deactivated catalyst could be effectively regenerated by the calcination method and the good catalytic performance was obtained.

关键词: Cumene, Benzene, Isopropanol, Alkylation, Beta-zeolite, Catalyst deactivation

Abstract: The alkylation of benzene with isopropanol over beta-zeolite is a more cost-effective solution to cumene production. During the benzene alkylation cycles, the cumene selectivity slowly increased, while the benzene conversion presented the sharp decrease due to catalyst deactivation. The deactivation mechanism of betazeolite catalyst was investigated by characterizing the fresh and used catalysts. The XRD, SEM and TEM results show that the crystalline and particle size of the beta-zeolite catalyst almost remained stable during the alkylation cycles. The drop in catalytic activity and benzene conversion could be explained by the TG, BET, NH₃-TPD and GC-MS results. The organic matters mainly consisted of ethylbenzene, p-xylene and 1-ethyl-3-(1-methyl) benzene produced in the benzene alkylation deposited in the catalyst, which strongly reduced the specific surface area of beta-zeolite catalyst. Moreover, during the reaction cycles, the amount of acidity also significantly decreased. As a result, the catalyst deactivation occurred. To maintain the catalytic performance, the catalyst regeneration was carried out by using ethanol rinse and calcination. The deactivated catalyst could be effectively regenerated by the calcination method and the good catalytic performance was obtained.

Key words: Cumene, Benzene, Isopropanol, Alkylation, Beta-zeolite, Catalyst deactivation

Yefei Liu, Yang Zou, Hong Jiang, Huanxin Gao, Rizhi Chen. Deactivation mechanism of beta-zeolite catalyst for synthesis of cumene by benzene alkylation with isopropanol[J]. , 2017, 25(9): 1195-1201.

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Deactivation mechanism of beta-zeolite catalyst for synthesis of cumene by benzene alkylation with isopropanol

Deactivation mechanism of beta-zeolite catalyst for synthesis of cumene by benzene alkylation with isopropanol

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