Browsing by Author "Cameli, Fabio"
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Item Biphasic Plasma Microreactor for Oxyfunctionalization of Liquid Hydrocarbons(Industrial & Engineering Chemistry Research, 2024-05-22) Nguyen, Darien K.; Cameli, Fabio; Dimitrakellis, Panagiotis; Vlachos, Dionisios G.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.Item Direct Conversion of Ethane to Oxygenates, Ethylene, and Hydrogen in a Noncatalytic Biphasic Plasma Microreactor(ACS Sustainable Chemistry and Engineering, 2023-05-29) Cameli, Fabio; Dimitrakellis, Panagiotis; Vlachos, Dionisios G.We selectively upgrade ethane (C2H6) to ethanol (C2H5OH), methanol (CH3OH), and acetic acid (CH3COOH) in a catalyst-free, continuous, argon/water biphasic plasma microreactor. The water (H2O) evaporates and electron- dissociates into OH· radicals. OH· recombines with alkyl radicals, produced via electron dissociation of ethane, to generate the oxygenates that absorb into H2O. A plasma-assisted path, reminiscent of the low-temperature thermocatalytic ethane steam reforming, leads to significant H2 coproduction. The gaseous stream also comprises CO2 and C2H4. Up to 1.3 and 1 μmol min–1 of liquid C2H5OH and CH3OH are attained, respectively. Compared to CO2-assisted ethane plasma conversion, which produces many oxygenates with low selectivity, the carbon selectivity can range from >70% C2H5OH, CH3OH, and CH3COOH to 60% C2H4. The low carbon footprint, electrified, modular, intensified process using a reactive evaporation and separation plasma could pave the way for the valorization of underutilized shale gas resources in remote areas.Item Microflow chemistry and its electrification for sustainable chemical manufacturing(Chemical Science, 2022-08-06) Chen, Tai-Ying; Wei Hsiao, Yung; Baker-Fales, Montgomery; Cameli, Fabio; Dimitrakellis, Panagiotis; Vlachos, Dionisios G.Sustainability is vital in solving global societal problems. Still, it requires a holistic view by considering renewable energy and carbon sources, recycling waste streams, environmentally friendly resource extraction and handling, and green manufacturing. Flow chemistry at the microscale can enable continuous sustainable manufacturing by opening up new operating windows, precise residence time control, enhanced mixing and transport, improved yield and productivity, and inherent safety. Furthermore, integrating microfluidic systems with alternative energy sources, such as microwaves and plasmas, offers tremendous promise for electrifying and intensifying modular and distributed chemical processing. This review provides an overview of microflow chemistry, electrification, their integration toward sustainable manufacturing, and their application to biomass upgrade (a select number of other processes are also touched upon). Finally, we identify critical areas for future research, such as matching technology to the scale of the application, techno-economic analysis, and life cycle assessment.