Department of Chemistry, University of Toronto , 80 Saint George Street, Toronto, Ontario M5S 3H6, Canada.
J Am Chem Soc. 2014 Mar 12;136(10):3875-80. doi: 10.1021/ja411601a. Epub 2014 Mar 3.
Frustrated Lewis pairs (FLPs) comprising sterically hindered Lewis acids and bases offer the capability to reversibly capture CO2 under mild reaction conditions. The determination of equilibrium constants and thermodynamic properties of these reactions should enable assessment of the efficiency of a particular FLP system for CO2 sequestration and provide insights for design of new, efficient formulations of FLP catalysts for CO2 capture. We have developed a microfluidic approach to studies of FLP-CO2 reactions, which provides their thermodynamic characterization that is not accessible otherwise. The approach enables the determination of the equilibrium reaction constants at different temperatures, the enthalpy, the entropy, and the Gibbs energy of these reactions, as well as the enhancement factor. The microfluidic methodology has been validated by applying it to the well-characterized reaction of CO2 with a secondary amine. The microfluidic approach can be applied for fundamental thermodynamic studies of other gas-liquid reactions.
受阻路易斯对（FLP）由空间位阻路易斯酸和碱组成，能够在温和的反应条件下可逆地捕获 CO2。这些反应的平衡常数和热力学性质的确定，应该能够评估特定 FLP 系统对 CO2 封存的效率，并为设计用于 CO2 捕获的新型高效 FLP 催化剂提供思路。我们已经开发了一种微流控方法来研究 FLP-CO2 反应，该方法提供了其他方法无法获得的热力学特征。该方法能够确定不同温度下的平衡反应常数、这些反应的焓、熵和吉布斯自由能，以及增强因子。该微流控方法已经通过应用于 CO2 与仲胺的特征反应得到了验证。该微流控方法可应用于其他气液反应的基础热力学研究。
