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 | |
刊名 | CHINESE JOURNAL OF CHEMICAL ENGINEERING |
2017-12-01 | |
卷号 | 25期号:12页码:1760-1770 |
关键词 | Hexamethylene-1 Thermal Decomposition 6-dicarbamate (Hdc) Hexamethylene-1 Co3o4/zsm-5 6-diisocyanate (Hdi) Heterogeneous Catalyst |
ISSN号 | 1004-9541 |
DOI | 10.1016/j.cjche.2017.03.032 |
文献子类 | Article |
英文摘要 | 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. |
WOS关键词 | PEPTIDE ISOCYANATES ; ZSM-5 ; OXIDATION ; CO-ZSM-5 ; ZEOLITES ; PROPANE ; CH4 |
WOS研究方向 | Engineering |
语种 | 英语 |
WOS记录号 | WOS:000419223300008 |
资助机构 | National Natural Science Foundation of China(21476244 ; 21406245) |
内容类型 | 期刊论文 |
源URL | [http://ir.ipe.ac.cn/handle/122111/23492] |
专题 | 过程工程研究所_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 |
推荐引用方式 GB/T 7714 | 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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