Water Increases the Faradaic Selectivity of Li-Mediated Nitrogen Reduction

被引:34
|
作者
Spry, Matthew [1 ]
Westhead, Olivia [1 ]
Tort, Romain [2 ]
Moss, Benjamin [1 ]
Katayama, Yu [3 ]
Titirici, Maria-Magdalena [2 ]
Stephens, Ifan E. L. [1 ]
Bagger, Alexander [2 ]
机构
[1] Imperial Coll London, Dept Mat, London SW7 2AZ, England
[2] Imperial Coll London, Dept Chem Engn, London SW7 2AZ, England
[3] Osaka Univ, SANKEN Inst Sci & Ind Res, Osaka 5670047, Japan
基金
英国工程与自然科学研究理事会; 欧洲研究理事会; 日本学术振兴会;
关键词
SOLID-ELECTROLYTE INTERPHASE; ELECTROCHEMICAL REDUCTION; AMMONIA-SYNTHESIS; LITHIUM; EFFICIENCY; N2;
D O I
10.1021/acsenergylett.2c02792
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The lithium-mediated system catalyzes nitrogen to ammonia under ambient conditions. Herein we discover that trace amount of water as an electrolyte additive -in contrast to prior reports from the literature-can effect a dramatic improvement in the Faradaic selectivity of N-2 reduction to NH3. We report that an optimal water concentration of 35.9 mM and LiClO4 salt concentration of 0.8 M allows a Faradaic efficiency up to 27.9 +/- 2.5% at ambient pressure. We attribute the increase in Faradaic efficiency to the incorporation of Li2O in the solid electrolyte interphase, as suggested by our X-ray photoelectron spectroscopy measurements. Our results high light the extreme sensitivity of lithium-mediated N-2 reduction to small changes in the experimental conditions.
引用
收藏
页码:1230 / 1235
页数:6
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