A DFT study on the insertion of CO2 into styrene oxide catalyzed by 1-butyl-3-methyl-Imidazolium bromide ionic liquid

作者：Marmitt Sandro; Goncalves Paulo F B^*

来源：Journal of Computational Chemistry, 2015, 36(17): 1322-1333.

DOI：10.1002/jcc.23930

• density functional theory
• cycloaddition reaction
• CO2
• reactive indices
• noncovalent interactions

Green systems able to capture or fix CO2 are becoming more important specially to reduce environmental impacts. In this work, the mechanism of insertion of CO2 into styrene oxide (STYO) both in the absence and presence of the catalyst 1-butyl-3-methyl-imidazolium bromide (BMIm Br) was investigated through calculations based on density functional theory in the B97X-D level. Two different routes were considered and it was shown they are energetically available and compete against each other. For both routes, the rate-determinant step is the ring opening of STYO resulting from the nucleophilic attack of the Br- on the C atom from STYO and is associated mainly to the participation of the cation and the anion from the catalyst in the reaction. Reactive indices and noncovalent interaction analysis were used as a tool to investigate this reason. This work allowed a better comprehension of the underlying mechanism and the supplied data provide valuable support for the design of new more efficient ionic liquid catalyst.

• 出版日期2015-6-30