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

被引:7
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
相关论文
共 46 条
  • [1] Synthesis of diethyl carbonate from ethyl carbamate and ethanol over ZnO-PbO catalyst
    An, Hualiang
    Zhao, Xinqiang
    Guo, Lian
    Jia, Chunyao
    Yuan, Baoguo
    Wang, Yanji
    [J]. APPLIED CATALYSIS A-GENERAL, 2012, 433 : 229 - 235
  • [2] Heterogeneous basic catalysts as alternatives to homogeneous catalysts:: reactivity of Mg/Al mixed oxides in the alkylation of m-cresol with methanol
    Bolognini, M
    Cavani, F
    Scagliarini, D
    Flego, C
    Perego, C
    Saba, M
    [J]. CATALYSIS TODAY, 2002, 75 (1-4) : 103 - 111
  • [3] Zn,Al hydrotalcites calcined at different temperatures: Preparation, characterization and photocatalytic activity in gas-solid regime
    Carriazo, D.
    del Arco, M.
    Garcia-Lopez, E.
    Marci, G.
    Martin, C.
    Palmisano, L.
    Rives, V.
    [J]. JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2011, 342-43 : 83 - 90
  • [4] Heterogeneously catalyzed persulfate by CuMgFe layered double oxide for the degradation of phenol
    Chen, Yun
    Yan, Jingchun
    Ouyang, Da
    Qian, Linbo
    Han, Lu
    Chen, Mengfang
    [J]. APPLIED CATALYSIS A-GENERAL, 2017, 538 : 19 - 26
  • [5] Experimental and computational VUV photoabsorption study of dimethyl carbonate: A green solvent
    Das, Asim Kumar
    Krishnakumar, Sunanda
    Rajasekhar, B. N.
    [J]. JOURNAL OF QUANTITATIVE SPECTROSCOPY & RADIATIVE TRANSFER, 2018, 217 : 116 - 125
  • [6] Developments in the production and application of dimethylcarbonate
    Delledonne, D
    Rivetti, F
    Romano, U
    [J]. APPLIED CATALYSIS A-GENERAL, 2001, 221 (1-2) : 241 - 251
  • [7] Dhana L.D., 2019, CATAL COMMUN, V122, P1, DOI [10.1016/j.catcom.2019.01.005, DOI 10.1016/J.CATCOM.2019.01.005]
  • [8] Structure and surface and catalytic properties of Mg-Al basic oxides
    Di Cosimo, JI
    Diez, VK
    Xu, M
    Iglesia, E
    Apesteguia, CR
    [J]. JOURNAL OF CATALYSIS, 1998, 178 (02) : 499 - 510
  • [9] Kinetics of dimethyl carbonate synthesis from methanol and carbon dioxide over ZrO2-MgO catalyst in the presence of butylene oxide as additive
    Eta, Valerie
    Maki-Arvela, Paivi
    Warna, Johan
    Salmi, Tapio
    Mikkola, Jyri-Pekka
    Murzin, Dmitry Yu.
    [J]. APPLIED CATALYSIS A-GENERAL, 2011, 404 (1-2) : 39 - 46
  • [10] Role of Lewis and Bronsted Acid Sites in the Dehydration of Glycerol over Niobia
    Foo, Guo Shiou
    Wei, Daniel
    Sholl, David S.
    Sievers, Carsten
    [J]. ACS CATALYSIS, 2014, 4 (09): : 3180 - 3192