| Autor: |
Olivia Westhead, Matthew Spry, Alexander Bagger, Zonghao Shen, Hossein Yadegari, Silvia Favero, Romain Tort, Maria-Magdalena Titirici, Mary P. Ryan, Rhodri Jervis, Ainara Aguadero, Anna Regoutz, Alexis Grimaud, Ifan E.L. Stephens |
| Rok vydání: |
2022 |
| DOI: |
10.26434/chemrxiv-2022-01g9l |
| Popis: |
Since its verification in just 2019, there have been numerous high-profile papers reporting improved efficiency of the lithium-mediated electrochemical nitrogen reduction system to make ammonia. However, the literature lacks a cohesive investigation systematically linking bulk electrolyte properties to electrochemical performance and Solid Electrolyte Interphase (SEI) properties. In this study, we vary electrolyte salt concentration and observe a transition from an unstable working electrode potential to working electrode potential stability and peak in Faradaic efficiency of 7.8 ± 0.5 % at 0.6 M LiClO4. The behaviour is linked to the formation of Solvent Separated Ion Pairs in the electrolyte through Raman spectroscopy. Time of Flight Secondary Ion Mass Spectrometry and X-Ray Photoelectron Spectroscopy reveal a more inorganic, and therefore more stable, SEI layer with increasing salt concentration. A drop in Faradaic efficiency is seen at concentrations higher than 0.6 M LiClO4, which is attributed to a combination of a loss in nitrogen solubility and diffusivity as well as increased SEI conductivity as measured by Electrochemical Impedance Spectroscopy. |
| Databáze: |
OpenAIRE |
| Externí odkaz: |
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