Catalysts screening, optimization and mechanism studies of dimethylhexane-1,6-dicarbamate synthesis from 1,6-hexanediamine and dimethyl carbonate over Mn(OAc)(2) catalyst
Zhao, Liyan1,2; He, Peng1; Wang, Liguo1; Ammar, Muhammad1,2; Cao, Yan1; Li, Huiquan1
2017-03-01
发表期刊CATALYSIS TODAY
ISSN0920-5861
卷号281页码:392-401
摘要

The catalytic synthesis of dimethylhexane-1,6-dicarbamate (HDC) from 1,6-hexanediamine (HDA) and dimethyl carbonate (DMC) over a series of homogeneous catalysts (e.g., metallic nitrates and acetates) were investigated. Mn(OAc)(2) was found to be the most effective catalyst for this reaction. Under the optimum reaction conditions (reaction temperature of 363 K, DMC-to-HDA molar ratio of 4:1, catalyst concentration of 7 wt% (based on HDA), and reaction time of 5 h), HDC yield can reach as high as 98.0% with HDA totally converted. Online in-situ Fourier Transform Infrared (FTIR) and Density Functional Theory (DFT) calculations were used together to investigate the interactions between Mn(OAc)(2) and substrates. The results indicated that both of HDA and DMC had interactions with Mn(OAc)(2), but the energy barriers of the transition states (TS) of DMC (DMC-TS) was higher than that of HDA (HDA-TS), which meant that HDA was easier to interact with Mn(OAc)(2) to form new complex than DMC. The whole process can be proposed that, the new species II, which was formed by the interaction of HDA and Mn(OAc)(2), attacked carbonyl carbon of DMC to generate intermediate HMC and finally to HDC. The experimental data and calculation results are in good agreement with each other. (C) 2016 Elsevier B.V. All rights reserved.

关键词Dimethyl Carbonate (Dmc) Mechanism Dimethylhexane-1 Homogeneous Catalyst 6-dicarbamate (Hdc)
文章类型Article
WOS标题词Science & Technology ; Physical Sciences ; Technology
DOI10.1016/j.cattod.2016.02.059
收录类别SCI
语种英语
关键词[WOS]Zinc Acetate ; Polyatomic-molecules ; Diethyl Carbonate ; Transition-states ; Alkyl Carbamate ; Methoxycarbonylation ; 1,6-hexamethylenediamine ; Dicarbamate ; Methanol ; Dioxide
WOS研究方向Chemistry ; Engineering
WOS类目Chemistry, Applied ; Chemistry, Physical ; Engineering, Chemical
WOS记录号WOS:000390623300020
引用统计
文献类型期刊论文
条目标识符http://ir.ipe.ac.cn/handle/122111/21862
专题湿法冶金清洁生产技术国家工程实验室
作者单位1.Chinese Acad Sci, Key Lab Green Proc & Engn, Natl Engn Lab Hydromet Cleaner Prod Technol, Inst Proc Engn, Beijing 100190, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
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Zhao, Liyan,He, Peng,Wang, Liguo,et al. Catalysts screening, optimization and mechanism studies of dimethylhexane-1,6-dicarbamate synthesis from 1,6-hexanediamine and dimethyl carbonate over Mn(OAc)(2) catalyst[J]. CATALYSIS TODAY,2017,281:392-401.
APA Zhao, Liyan,He, Peng,Wang, Liguo,Ammar, Muhammad,Cao, Yan,&Li, Huiquan.(2017).Catalysts screening, optimization and mechanism studies of dimethylhexane-1,6-dicarbamate synthesis from 1,6-hexanediamine and dimethyl carbonate over Mn(OAc)(2) catalyst.CATALYSIS TODAY,281,392-401.
MLA Zhao, Liyan,et al."Catalysts screening, optimization and mechanism studies of dimethylhexane-1,6-dicarbamate synthesis from 1,6-hexanediamine and dimethyl carbonate over Mn(OAc)(2) catalyst".CATALYSIS TODAY 281(2017):392-401.
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