Brandon Kamiyama, Mohammad Ali Eslamisaray, Emily Gillmore, R. Mohan Sankaran
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Influence of Gaseous Oxygen Species on Liquid-Phase, Fixed Nitrogen Products in Aqueous Plasma-Based Electrochemical Processes
Electrified, small-scale, remote approaches are needed as an alternative to conventional centralized methods for nitrogen fixation in order to reduce our reliance on fossil fuels and ensure global food security. Plasma-based electrolytic processes offer a promising solution by directly reacting molecular nitrogen and water under mild conditions. However, the complex non-equilibrium chemistry results in a diverse range of gas-phase and liquid-phase reactions, which impacts selectivity toward desired products. In this study, we investigate the influence of feed gas composition, specifically the presence of molecular oxygen at minute quantities, on the liquid-phase nitrogen products. Specifically, oxygen gas concentrations as low as 0.1% in the gas feed are found to substantially affect the selectivity towards ammonium ions. We additionally show that the total gas flow rate has an indiscriminate effect on both ammonium and nitrate/nitrite ion yields because of the presence of water vapor. By carefully controlling these process parameters, a production rate for ammonium ions exceeding 1 mg/h with a molar selectivity of ~ 14 is achieved. Our results highlight the importance of gas-phase chemistry in plasma-based electrolytic nitrogen fixation.
期刊介绍：
Publishing original papers on fundamental and applied research in plasma chemistry and plasma processing, the scope of this journal includes processing plasmas ranging from non-thermal plasmas to thermal plasmas, and fundamental plasma studies as well as studies of specific plasma applications. Such applications include but are not limited to plasma catalysis, environmental processing including treatment of liquids and gases, biological applications of plasmas including plasma medicine and agriculture, surface modification and deposition, powder and nanostructure synthesis, energy applications including plasma combustion and reforming, resource recovery, coupling of plasmas and electrochemistry, and plasma etching. Studies of chemical kinetics in plasmas, and the interactions of plasmas with surfaces are also solicited. It is essential that submissions include substantial consideration of the role of the plasma, for example, the relevant plasma chemistry, plasma physics or plasma–surface interactions; manuscripts that consider solely the properties of materials or substances processed using a plasma are not within the journal’s scope.
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