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An efficient green route for hexamethylene-1,6-diisocyanate synthesis by thermal decomposition of hexamethylene-1,6-dicarbamate over Co3O4/ZSM-5 catalyst: An indirect utilization of CO2
Ammar, Muhammad1,2; Cao, Yan1; He, Peng1; Wang, Liguo1; Chen, Jiaqiang1; Li, Huiquan1; Cao, Y
2017-12-01
发表期刊CHINESE JOURNAL OF CHEMICAL ENGINEERING
ISSN1004-9541
卷号25期号:12页码:1760-1770
摘要

The utilization of CO2 as raw material for chemical synthesis has the potential for substantial economic and green benefits. Thermal decomposition of hexamethylene-1,6-dicarbamate (HDC) is a promising approach for indirect utilization of CO2 to produce hexamethylene-1,6-diisocyanate (HDI). In this work, a green route was developed for the synthesis of HDI by thermal decomposition of HDC over Co3O4/ZSM-5 catalyst, using chlorobenzene as low boiling point solvent. Different metal oxide supported catalysts were prepared by incipient wetness impregnation (IWI), PEG-additive (PEG) and deposition precipitation with ammonia evaporation (DP) methods. Their catalytic performances for the thermal decomposition of HDC were tested. The catalyst screening results showed that Co3O4/ZSM-5(25) catalysts prepared by different methods showed different performances in the order of Co3O4/ZSM-5(25(PEG)) > Co3O4/ZSM-5(25(IWI)) > Co3O4/ZSM-5(25(DP)). The physicochemical properties of Co3O4/ZSM-5(25) catalyst were characterized by XRD, FTIR, N-2 adsorption-desorption measurements, NH3-TPD and XPS. The superior catalytic performance of Co3O4/ZSM-5(25(PEG)) catalyst was attributed to its relative surface content of Co3+, surface lattice oxygen content and total acidity. Under the optimized reaction conditions: 6.5% HDC concentration in chlorobenzene, 1 wt% Co3O4/ZSM-5(25(PEG)) catalyst, 250 degrees C temperature, 2.5 h time, 800 ml . min(-1) nitrogen flow rate and 1.0 MPa pressure, the HDC conversion and HDI yield could reach 100% and 92.8% respectively. The Co3O4/ZSM-5(25(PEG)) catalyst could be facilely separated from the reaction mixture, and reused without degradation in catalytic performance. Furthermore, a possible reaction mechanism was proposed based on the physicochemical properties of the Co3O4/ZSM-5(25) catalysts. (C) 2017 The Chemical Industry and Engineering Society of China, and Chemical Industry Press. All rights reserved.

关键词Hexamethylene-1 Thermal Decomposition 6-dicarbamate (Hdc) Hexamethylene-1 Co3o4/zsm-5 6-diisocyanate (Hdi) Heterogeneous Catalyst
文章类型Article
WOS标题词Science & Technology ; Technology
DOI10.1016/j.cjche.2017.03.032
收录类别SCI
语种英语
关键词[WOS]PEPTIDE ISOCYANATES ; ZSM-5 ; OXIDATION ; CO-ZSM-5 ; ZEOLITES ; PROPANE ; CH4
WOS研究方向Engineering
WOS类目Engineering, Chemical
项目资助者National Natural Science Foundation of China(21476244 ; 21406245)
WOS记录号WOS:000419223300008
引用统计
文献类型期刊论文
条目标识符http://ir.ipe.ac.cn/handle/122111/23492
专题研究所(批量导入)
通讯作者Cao, Y
作者单位1.Chinese Acad Sci, Inst Proc Engn, Key Lab Green Proc & Engn, Natl Engn Lab Hydromet Cleaner Prod Technol, Beijing 100190, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
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Ammar, Muhammad,Cao, Yan,He, Peng,et al. An efficient green route for hexamethylene-1,6-diisocyanate synthesis by thermal decomposition of hexamethylene-1,6-dicarbamate over Co3O4/ZSM-5 catalyst: An indirect utilization of CO2[J]. CHINESE JOURNAL OF CHEMICAL ENGINEERING,2017,25(12):1760-1770.
APA Ammar, Muhammad.,Cao, Yan.,He, Peng.,Wang, Liguo.,Chen, Jiaqiang.,...&Cao, Y.(2017).An efficient green route for hexamethylene-1,6-diisocyanate synthesis by thermal decomposition of hexamethylene-1,6-dicarbamate over Co3O4/ZSM-5 catalyst: An indirect utilization of CO2.CHINESE JOURNAL OF CHEMICAL ENGINEERING,25(12),1760-1770.
MLA Ammar, Muhammad,et al."An efficient green route for hexamethylene-1,6-diisocyanate synthesis by thermal decomposition of hexamethylene-1,6-dicarbamate over Co3O4/ZSM-5 catalyst: An indirect utilization of CO2".CHINESE JOURNAL OF CHEMICAL ENGINEERING 25.12(2017):1760-1770.
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