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
相关论文
共 50 条
  • [1] Nonaqueous Li-Mediated Nitrogen Reduction: Taking Control of Potentials
    Tort, Romain
    Westhead, Olivia
    Spry, Matthew
    Davies, Bethan J. V.
    Ryan, Mary P.
    Titirici, Maria-Magdalena
    Stephens, Ifan E. L.
    ACS ENERGY LETTERS, 2023, 8 (02) : 1003 - 1009
  • [2] Enhancing Ammonia Production by Ag Incorporation in Li-Mediated Nitrogen Reduction Reactions
    Jeon, Yeongbae
    Shin, Dongwoo
    Yong, Kijung
    Hwang, Yun Jeong
    ACS ENERGY LETTERS, 2024, 9 (08): : 4147 - 4152
  • [3] Localized High-Concentration Electrolyte in Li-Mediated Nitrogen Reduction for Ammonia Synthesis
    Yun, Hyeju
    Lim, Chaeeun
    Kwon, Minjun
    Lee, Dongmin
    Yun, Yongju
    Seo, Dong-Hwa
    Yong, Kijung
    ADVANCED MATERIALS, 2024,
  • [4] Effect of Sulfur-Derived Solid Electrolyte Interphase on Li-mediated Nitrogen Reduction
    Lim, Chaeeun
    Kim, Dongkyu
    Kim, Mingyun
    Yun, Hyeju
    Shin, Dongwoo
    Hwang, Yun Jeong
    Shin, Hyeyoung
    Yong, Kijung
    ACS ENERGY LETTERS, 2023, 8 (11) : 4875 - 4884
  • [5] Theoretical insight into the mechanism of Li-mediated nitrogen reduction reaction by density functional theory
    Zhang, Ji
    Yu, Aimin
    Li, Dong-sheng
    Sun, Chenghua
    MOLECULAR CATALYSIS, 2024, 569
  • [6] Devices for Li-mediated synthesis
    James Gallagher
    Nature Energy, 2023, 8 : 641 - 641
  • [7] Devices for Li-mediated synthesis
    Gallagher, James
    NATURE ENERGY, 2023, 8 (07) : 641 - 641
  • [8] Li-Mediated Electrochemical Nitrogen Fixation: Key Advances and Future Perspectives
    Ahmed, Muhammad Ibrar
    Assafiri, Aya
    Hibbert, David Brynn
    Zhao, Chuan
    SMALL, 2023, 19 (52)
  • [9] Li-Mediated Electrochemical Nitrogen Fixation: Key Advances and Future Perspectives
    Ahmed, Muhammad Ibrar
    Assafiri, Aya
    Hibbert, David Brynn
    Zhao, Chuan
    SMALL, 2023,
  • [10] Identification, Quantification, and Elimination of NOx and NH3 Impurities for Aqueous and Li-Mediated Nitrogen Reduction Experiments
    Izelaar, Boaz
    Ripepi, Davide
    van Noordenne, Dylan D.
    Jungbacker, Peter
    Kortlever, Ruud
    Mulder, Fokko M.
    ACS ENERGY LETTERS, 2023, 8 (08) : 3614 - 3620