CO2 reduction in aqueous-ionic liquid solution in microscale-based corona reactor Public Deposited

CO₂ reduction in aqueous-ionic liquid solution in microscale-based corona reactor

http://ir.library.oregonstate.edu/concern/graduate_thesis_or_dissertations/pv63g2564

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  • Global warming problem is becoming an increasingly important environmental concern and CO₂ is considered as the major cause of global warming. Among various methods of CO₂ utilization, conversion of CO₂ to value added chemical products is the most attractive. In this study, a microscale-based corona reactor is introduced for reduction of CO₂. Two kinds of solvent were used in this study for absorbing CO₂: DI-water and ionic liquid 1-butyl-3-methylimidazolium tetrafluoroborate ([BMIM][BF4]). The latter one has a much higher solubility of CO₂. After saturated with CO₂, solution was introduced into the microreactor built around the concept of corona discharge. The corona was created through a significant potential difference between two graphite electrodes. The current that passed through two electrodes acted as a catalytic agent for the reduction of CO₂. The experiments were conducted at room temperature and at steady state. The ranges of the operating conditions were: mean residence time 5 to 100 (sec), thickness of spacer 200 and 500 (μm), and voltage applied across the reactor 20 and 22.5 (V). Reactions happened in the bulk of the reactor and five main products were detected at the outlet stream: i) formic acid (HCOOH), ii) formaldehyde (HCHO), iii) methanol (CH₃OH), iv) methane (CH₄) and v) hydrogen (H₂). Among these compounds, formic acid, formaldehyde and methanol are intermediate products. The conversion of CO₂ in aqueous solution can reach as high as 94.8% at mean residence time of 100 sec. Although in ionic liquid solution the conversion of CO₂ is much lower (19.3% at mean residence time of 100 sec), consumption of CO₂ in ionic liquid is 6-7 times larger than that in water when generating same volume of products. A mathematical model reflecting geometry and flow conditions inside the microreactor was developed to simulate the process of CO₂ reduction. The model was solved numerically using COMSOL Multiphysics software package. The simulated results were optimized to fit the experimental data using COMSOL-Matlab LiveLink software package. Primary reaction rate constants for CO₂ reduction were predicted. The mathematical model was found to explain the experimental data pretty well.
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