Selective preparation and reaction kinetics of dimethyl carbonate from alcoholysis of methyl carbamate with methanol over ZnAl-LDO
- 9 July 2021
- journal article
- research article
- Published by Royal Society of Chemistry (RSC) in Reaction Chemistry & Engineering
- Vol. 6 (10), 1854-1868
- https://doi.org/10.1039/d1re00158b
Abstract
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 × 106 and the activation energy was 56.34 kJ mol−1). At the same time, the reaction enthalpy (ΔrH0 m = 106.203 kJ mol−1) and Gibbs free energy (ΔrG0 m = 59.389 kJ mol−1) were determined by thermodynamic calculation of the reaction equation.Keywords
Funding Information
- National Natural Science Foundation of China (21536003, 21776065, 21808049)
- Natural Science Foundation of Hunan Province (2019JJ20006)
This publication has 46 references indexed in Scilit:
- Synthesis of Dimethyl Carbonate from Methyl Carbamate and Methanol Using a Fixed‐Bed ReactorChemical Engineering & Technology, 2012
- Synthesis of dimethyl carbonate from urea and methanol over ZnO(X)–CeO2(1−X) catalysts prepared by a sol–gel methodJournal of Industrial and Engineering Chemistry, 2012
- Kinetics of dimethyl carbonate synthesis from methanol and carbon dioxide over ZrO2–MgO catalyst in the presence of butylene oxide as additiveApplied Catalysis A: General, 2011
- Zn,Al hydrotalcites calcined at different temperatures: Preparation, characterization and photocatalytic activity in gas–solid regimeJournal of Molecular Catalysis A: Chemical, 2011
- Hydrogenation of Ethyl Acetate to Ethanol over Ni-Based Catalysts Obtained from Ni/Al Hydrotalcite-Like CompoundsMolecules, 2010
- Zn/Fe mixed oxide: Heterogeneous catalyst for the synthesis of dimethyl carbonate from methyl carbamate and methanolCatalysis Communications, 2010
- High-Yield Synthesis of Dimethyl Carbonate from Urea and Methanol Using a Catalytic Distillation ProcessIndustrial & Engineering Chemistry Research, 2007
- Synthesis of dimethyl carbonate from urea and methanol catalyzed by the metallic compounds at atmospheric pressureCatalysis Communications, 2006
- Synthesis of Dimethyl Carbonate from Urea and Methanol over ZnOIndustrial & Engineering Chemistry Research, 2005
- Heterogeneous basic catalysts as alternatives to homogeneous catalysts: reactivity of Mg/Al mixed oxides in the alkylation of m-cresol with methanolCatalysis Today, 2002