Selective preparation and reaction kinetics of dimethyl carbonate from alcoholysis of methyl carbamate with methanol over ZnAl-LDO

被引:8
作者
Jia, Bo [1 ]
Sun, Xiaoyu [1 ]
Chen, Ming [1 ]
Jian, Jian [2 ]
You, Kuiyi [2 ]
Luo, He'an [2 ]
Huang, Yangqiang [1 ]
Luo, Xiao [1 ]
Jin, Bo [1 ]
Wang, Nailiang [3 ]
Liang, Zhiwu [1 ]
机构
[1] Hunan Univ, Minist Educ, Engn Res Ctr Adv Catalysis, Coll Chem & Chem Engn, Changsha 410082, Hunan, Peoples R China
[2] Xiangtan Univ, Coll Chem Engn, Xiangtan 411105, Peoples R China
[3] Ningxia Univ, State Key Lab High Efficiency Utilizat Coal & Gre, Yinchuan 750000, Ningxia, Peoples R China
基金
中国国家自然科学基金;
关键词
DIETHYL CARBONATE; MIXED OXIDES; PROPYLENE CARBONATE; CATALYSTS; UREA; MG; ETHANOL; LA; HYDROGENATION; PRECURSORS;
D O I
10.1039/d1re00158b
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
In this paper, an optimal composite metal oxide ZnAl-LDO catalyst, which was prepared from Zn/Al layered double hydroxides (ZnAl-LDHs) as the precursor, has been evaluated for the synthesis of dimethyl carbonate (DMC) by methyl carbamate (MC) alcoholysis. The composite metal oxide achieved a selectivity of 58.26% for DMC production under optimal reaction conditions (the catalyst calcination temperature is 873 K, the molar ratio of methanol to MC is 15, the catalyst weight percentage is 1 wt%, and the reaction temperature and reaction time are 453 K and 10 h). The influence of the structural characteristics of the catalyst on its catalytic performance was investigated by characterizing the catalyst. The kinetic model of the catalytic reaction was established and modified. According to the fitting results, it can be concluded that the reaction process conforms to the Langmuir-Hinshelwood kinetic model, and the kinetic parameters were obtained by the Arrhenius formula (the pre-exponential factor was 1.21 x 10(6) and the activation energy was 56.34 kJ mol1). At the same time, the reaction enthalpy (Delta = 106.203 kJ mol) and Gibbs free energy (Delta) were determined by thermodynamic calculation of the reaction equation.
引用
收藏
页码:1854 / 1868
页数:15
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