The Effect of Applied Potential on the Li-mediated Nitrogen Reduction Reaction Performance

Boaz Izelaar, Pranav Karanth, Arash Toghraei, Santosh K. Pal, Nandalal Girichandran, Mark Weijers, Ruud W. A. Hendrikx, Fokko M. Mulder and Ruud Kortlever ()
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Boaz Izelaar: Leeghwaterstraat 39, Process and Energy Department, Faculty of Mechanical Engineering, Delft University of Technology
Pranav Karanth: Delft University of Technology, Chemical Engineering Department, Faculty of Applied Sciences
Arash Toghraei: Varennes, Énergie, Matériaux, Télécommunications Research Centre, Institute National de la Recherche Scientifique (INRS), 1650 Bd. Lionel-Boulet
Santosh K. Pal: Delft University of Technology, Chemical Engineering Department, Faculty of Applied Sciences
Nandalal Girichandran: Leeghwaterstraat 39, Process and Energy Department, Faculty of Mechanical Engineering, Delft University of Technology
Mark Weijers: Delft University of Technology, Chemical Engineering Department, Faculty of Applied Sciences
Ruud W. A. Hendrikx: Delft University of Technology, Material Science and Engineering Department, Faculty of Mechanical Engineering
Fokko M. Mulder: Delft University of Technology, Chemical Engineering Department, Faculty of Applied Sciences
Ruud Kortlever: Leeghwaterstraat 39, Process and Energy Department, Faculty of Mechanical Engineering, Delft University of Technology

Nature Communications, 2025, vol. 16, issue 1, 1-14

Abstract: Abstract The Li-mediated nitrogen reduction reaction (Li-NRR) has been proposed as one of the most promising ambient production routes for green ammonia. However, the effect of the applied potential (Ewe) on the reaction performance and the properties of the solid electrolyte interphase (SEI) remain poorly understood. Herein, we combine potential controlled experiments using a reliable LixFePO4 based reference electrode with post-mortem SEI characterization techniques, wherein we observe both an increase in the LiF concentration in the SEI, originating from LiTFSI decomposition, and the Faradaic efficiency (FENH3) with an increasing Ewe. The transition from a predominantly organic SEI at low Ewe (−3.2 VSHE) to a LiF-enriched layer at higher Ewe indicates the existence of kinetic barriers for the SEI formation reactions. Moreover, thicker and denser SEI structures observed at a higher Ewe enhance the Li-NRR by improving the mass transport regulation between reactant species. However, these thicker and denser SEI morphologies lead to current instabilities due to dynamic SEI thickening and breakdown.

Date: 2025
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DOI: 10.1038/s41467-025-65627-w

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