Biphasic Plasma Microreactor for Oxyfunctionalization of Liquid Hydrocarbons
Date
2024-05-22
Authors
Nguyen, Darien K.
Cameli, Fabio
Dimitrakellis, Panagiotis
Vlachos, Dionisios G.
Journal Title
Journal ISSN
Volume Title
Publisher
Industrial & Engineering Chemistry Research
Abstract
Oxyfunctionalization of linear alkanes is important but challenging to achieve. Herein, we demonstrate a biphasic gas–liquid modular plasma microreactor utilizing Ar/O2 gas to selectively oxidize liquid n-dodecane (C12) in an electrified, catalyst-free fashion. C12 secondary alcohols and ketones are the major products, with selectivities of 45–60% and a maximum yield of 23%. Fine-tuning gas and liquid flow rates enhance the plasma–liquid interfacial area, leading to a conversion of >50%. Difunctional and oligomerized oxygenates, alongside lighter hydrocarbons stemming from carbon–carbon cleavage, form at higher conversions. The energy efficiency (0.189 μmol/J) of the modular microreactor is the highest reported among plasma systems. Alkane conversion can be further improved by increasing the length of the plasma region while maintaining excellent energy efficiencies. Similarly, sequential processing/recirculation can enhance the extent of the reaction. This system is also amenable to treating mixtures of liquid n-alkanes, where smaller hydrocarbons are oxidized preferentially to a certain extent. The vapor pressure and liquid temperature are the key parameters. The chemistry occurs primarily in the gas phase for the lighter hydrocarbons and switches to interfacial reactions for the larger ones.
Description
This document is the Accepted Manuscript version of a Published Work that appeared in final form in Industrial & Engineering Chemistry Research, copyright © 2024 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.iecr.4c00605. This article will be embargoed until 05/22/2025.
Keywords
non-thermal plasma, microreactor, functionalization, liquid alkane
Citation
Nguyen, Darien K., Fabio Cameli, Panagiotis Dimitrakellis, and Dionisios G. Vlachos. “Biphasic Plasma Microreactor for Oxyfunctionalization of Liquid Hydrocarbons.” Industrial & Engineering Chemistry Research 63, no. 20 (May 22, 2024): 9008–17. https://doi.org/10.1021/acs.iecr.4c00605.