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Updated: Jun 15, 2025
A Protocol for Safe Lithiation Reactions Using Organolithium Reagents
Published on: November 12, 2016
Enhancement of Lithium-Mediated Nitrogen Reduction by Modifying Center Atom of Tetraalkyl-Type Ionic Liquids
Sungbin Yang1, Jinwoo Chu1, Jihye Park2
1Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), Daejeon, 34141, Republic of Korea.
Abstract:
The lithium-mediated nitrogen reduction reaction (Li-NRR) offers a viable alternative to the Haber-Bosch process for ammonia production. However, ethanol, a common proton carrier in Li-NRR, exhibits electrochemical instability, leading to oxidation at the anode or byproduct formation at the cathode. This study replaces alcoholic proton carriers with ionic liquids (ILs), specifically tetrabutylphosphonium chloride (TBPCl) and tetrabutylammonium chloride (TBACl), to examine how the electronegativity differences between the central atom and adjacent carbon of the cation affect catalytic performance. The results show that switching the central atom in tetraalkyl-type ILs markedly enhances performance, specifically resulting in a 1.45-fold increase in Faradaic efficiency (FE) with the transition from phosphonium to ammonium cation of ILs. Additionally, optimal IL concentrations in the electrolyte are identified to maximize ammonia yield. TBACl, in particular, demonstrates enhanced ammonia production and operational stability, achieving an ammonia yield rate of 13.60 nmol/cm2/s, an FE of 39.5 %, and operational stability for over 12 h under conditions of 10 mA/cm2 and 10 atm. This research underscores the potential of precise IL modifications for more efficient and sustainable Li-NRR.
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