One-step bulk fabrication of a CaO/carbon heterogeneous catalyst from calcium citrate for rapid synthesis of dimethyl carbonate (DMC) by transesterification of ethylene carbonate (EC)

被引:23
作者
Wei, Qiang [1 ,2 ]
Zhang, Gang [1 ,2 ]
Yao, Jie [1 ]
Chen, Xuejun [1 ]
Wang, Gongying [1 ]
Yang, Xiangui [1 ]
机构
[1] Chinese Acad Sci, Chengdu Inst Organ Chem, Chengdu 610041, Sichuan, Peoples R China
[2] Univ Chinese Acad Sci, Natl Engn Lab Far VOCs Pollut Control Mat & Techn, 19A Yuquan Rd, Beijing 100049, Peoples R China
基金
国家重点研发计划;
关键词
Ethylene - Rate constants - Calcium compounds - Reusability - Carbonization - Catalysts - Transesterification - Carbonation;
D O I
10.1039/d0nj06144a
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Dimethyl carbonate (DMC) is well known as an extremely industrially valuable substance. The demand for high-efficiency synthesis of DMC has greatly driven the exploration of novel catalysts and their low-cost preparation methods. Herein, a novel method for the rapid batch preparation of CaO/carbon catalysts using calcium citrate (CaCi) was provided, and these catalysts were used to catalyze the transesterification reaction of methanol and ethylene carbonate (EC) to synthesize DMC and ethylene glycol (EG). Accordingly, the structure and properties of the catalysts were characterized using XRD, FTIR, N-2 adsorption-desorption, TG, TG-IR, CO2-TPD, XPS, SEM, TEM and ICP-OES techniques. Meanwhile, the effect of various process conditions such as carbonization temperature, reaction temperature, reaction time and catalyst amount has been extensively evaluated. Under the optimal process parameters, the conversion of EC and the selectivity of DMC and EG were 81.2, 99.3 and 99.5%, while the turnover number (TON) and turnover frequency (TOF) were 54.1 and 162 h(-1), respectively. Furthermore, kinetic analysis was carried out, and the value of k (reaction rate constant) was approximate to 0.159 mol L-1 min(-1). The reusability was also investigated.
引用
收藏
页码:5540 / 5550
页数:11
相关论文
共 52 条
[1]  
Akhtar K., 2019, J DISPERSION SCI TEC, V41, P1
[2]  
Bei P., 2019, ENVIRON SCI POLLUT R, P26
[3]   Carbon nanotubes supported Cu-Ni bimetallic catalysts and their properties for the direct synthesis of dimethyl carbonate from methanol and carbon dioxide [J].
Bian, Jun ;
Xiao, Min ;
Wang, Shuan-Jin ;
Lu, Yi-Xin ;
Meng, Yue-Zhong .
APPLIED SURFACE SCIENCE, 2009, 255 (16) :7188-7196
[4]  
BRISTOW PA, 1967, TETRAHEDRON LETT, P901
[5]   Thermal degradation characteristics of flame retardant polylactide using TG-IR [J].
Chen, Xilei ;
Zhuo, Jinlong ;
Jiao, Chuanmei .
POLYMER DEGRADATION AND STABILITY, 2012, 97 (11) :2143-2147
[6]   Developments in the production and application of dimethylcarbonate [J].
Delledonne, D ;
Rivetti, F ;
Romano, U .
APPLIED CATALYSIS A-GENERAL, 2001, 221 (1-2) :241-251
[7]   Highly efficient catalyst PdCl2-CuCl2-KOAc/AC@Al2O3 for gas-phase oxidative carbonylation of methanol to dimethyl carbonate: Preparation and reaction mechanism [J].
Ding, Xiaoshu ;
Dong, Xiangmo ;
Kuang, Dongting ;
Wang, Shufang ;
Zhao, Xinqiang ;
Wang, Yanji .
CHEMICAL ENGINEERING JOURNAL, 2014, 240 :221-227
[8]   Catalyst screening for the melt polymerization of isosorbide-based polycarbonate [J].
Eo, Yong Seok ;
Rhee, Hee-Woo ;
Shin, Seunghan .
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY, 2016, 37 :42-46
[9]   Optimization of Catalytic Distillation for the Synthesis of Dimethyl Carbonate by Response Surface Methodology [J].
Feng, Yuchen ;
Guo, Bao ;
Tang, Shixiong ;
Liu, Yida ;
Liu, Jidong ;
Lv, Jianhua .
CHEMISTRYSELECT, 2020, 5 (47) :14955-14965
[10]   Mesoporous carbons synthesized by direct carbonization of citrate salts for use as high-performance capacitors [J].
Ferrero, G. A. ;
Sevilla, M. ;
Fuertes, A. B. .
CARBON, 2015, 88 :239-251