A microfluidic relative permittivity sensor for feedback control of carbon dioxide expanded liquid flows

Abstract

Binary CO2-alcohol mixtures, such as CO2-expanded liquids (CXLs), are promising green solvents for reaching higher performance in flow chemistry and separation processing. However, their compressibility and high working pressure makes handling challenging. These mixtures allow for a tuneable polarity but, to do so, requires precise flow control. Here, a high-pressure tolerant microfluidic system containing a relative permittivity sensor and a mixing chip is used to actively regulate the relative permittivity of these fluids and indirectly—composition. The sensor is a fluid-filled plate capacitor created using embedded 3D-structured thin films and has a linearity of 0.9999, a sensitivity of 4.88 pF per unit of relative permittivity, and a precision within 0.6% for a sampling volume of 0.3 μL. Composition and relative permittivity of CO2-ethanol mixtures were measured at 82 bar and 21 °C during flow. By flow and dielectric models, this relationship was found to be described by the pure components and a quadratic mixing rule with an interaction parameter, kij, of -0.63 ± 0.02. Microflows with a relative permittivity of 1.7–21.4 were generated, and using the models, this was found to correspond to compositions of 6–90 mol % ethanol in CO2. With the sensor, a closed loop control system was realised and CO2-ethanol flows were tuned to setpoints of the relative permittivity in 30 s.