Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)
Publication date: 18th July 2023
Electrochemical ammonia synthesis under ambient conditions is a promising sustainable alternative to the highly carbon-intensive Haber-Bosch process. The lithium-mediated system is to date the only rigorously verified method of reducing dinitrogen, though its mechanism is not yet understood. have proposed that electrodeposited metallic lithium cleaves the dinitrogen triple bond; others that metallic Li or a LiH/Li3N layer provides a catalytic surface for direct protonation. None are yet supported by spectroscopic evidence
Several reports now suggest that engineering of the Solid Electrolyte Interphase (SEI) on the working electrode, like those formed on lithium-ion battery anodes, is the key to efficient nitrogen reduction[1]–[4], by controlling the transport rates of N2, Li+ and H2, thus suppressing excess Li plating and H2 evolution. In previous work, we demonstrated a dramatic improvement in Faradaic efficiency in LiClO4-containing electrolytes with small additions of water and linked this to enhanced Li2O formation in the SEI[5].
In this work, we investigate two key processes using in situ infrared spectroscopy. Firstly, the formations of key SEI species in different electrolyte formulations, and the potentials at which these reactions occur. We find that the lithium ethoxide content of the SEI depends strongly on the water concentration of the electrolyte and propose a mechanism for Li2O formation and ethanol regeneration in the presence of water. Secondly, we exploit the surface-enhancement effect to probe adsorbed intermediates on the working electrode. By detecting key NH intermediates, we can identify the mechanism of nitrogen reduction and inform the design of novel electrocatalysts.
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