Facile Synthesis of Silicon-Based Materials Modified Using Zinc(II) 2-Bromoacetic as Heterogeneous Catalyst for the Fixation of CO2 into Cyclic Carbonates

被引:2
|
作者
Yang, Chaokun [1 ]
Ma, Xiangning [2 ]
Li, Meng [3 ]
Yang, Tuantuan [1 ]
Zhao, Xin [1 ]
机构
[1] Civil Aviat Flight Univ China, Discipline Construct Off, Guanghan 618307, Peoples R China
[2] Shandong Univ, Marine Coll, Weihai 264209, Peoples R China
[3] Civil Aviat Flight Univ China, Coll Aviat Engn, Guanghan 618307, Peoples R China
关键词
CO2; cyclic carbonate; epoxides; silicon-based; KI; PERIODIC MESOPOROUS ORGANOSILICA; COVALENT ORGANIC FRAMEWORK; IN-SITU GENERATION; IONIC LIQUIDS; CHEMICAL FIXATION; CYCLOADDITION REACTION; EFFICIENT CATALYST; COUPLING REACTION; PROPYLENE-OXIDE; DIOXIDE;
D O I
10.3390/catal13071116
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Much effort has been devoted to the development of efficient heterogeneous catalysts for the conversion of carbon dioxide (CO2) into high-value chemicals. Generally, the cycloaddition of CO2 to epoxides is considered a green and atom-economic reaction for the production of cyclic carbonates. Based on this, three kinds of silicon-based catalysts modified using zinc(II) 2-bromoacetic (Si-ZnBA-n, n = 1, 2, 3) were facilely synthesized and employed for the chemical fixation of CO2 to epoxides with the use of potassium iodide (KI). A series of characterization techniques were used to characterize the textual structures and physicochemical properties of Si-ZnBA-n. The synergistic effects of Zn, -NH2, -OH and the nucleophilic group guaranteed the catalytic activity of Si-ZnBA-n. Si-ZnBA-1 exhibited the best catalytic activity among Si-ZnBA-n because Si-ZnBA-1 possessed the highest Zn content. Additionally, the effects of the reaction conditions (temperature, pressure, time and catalyst loadings) were also discussed. The propylene carbonate (PC) yield could reach 97% under 130 & DEG;C, 2 MPa, for 5 h without the employment of organic solvent, and its selectivity was 99%. In addition, the recycling property of Si-ZnBA-1/KI was also investigated, and the catalytic system exhibited good cycle performance. Meanwhile, the catalyst showed outstanding versatility for CO2 application to various epoxides, and a possibly synergistic reaction mechanism was proposed. Finally, a dynamic model was developed to discuss the activation energy of the CO2 cycloaddition reaction over the Si-ZnBA-1 catalyst.
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页数:17
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