4.6 Article

Understanding the Factors Determining the Faradaic Efficiency and Rate of the Lithium Redox-Mediated N2 Reduction to Ammonia

Journal

JOURNAL OF PHYSICAL CHEMISTRY C
Volume 125, Issue 21, Pages 11402-11410

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.1c02494

Keywords

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Funding

  1. Australian Research Council [DP200101878, FT200100317]
  2. Australian Renewable Energy Agency [2018/RND009 DRM015]
  3. Australian Research Council (Centre of Excellence for Electromaterials Science Grant) [CE140100012]
  4. Australian Research Council [DP200101878, FT200100317] Funding Source: Australian Research Council

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The study investigated the effects of parameters such as electrode potential, convection, N-2 pressure, and water content on the electrochemical production of ammonia. Results showed that a closely linear ammonia yield and approximately constant faradaic efficiency can be maintained during experiments lasting up to 60 hours. Improved control of reaction conditions led to ammonia yield rates above 1 nmol s(-1) cm(-2) and faradaic efficiencies as high as 60%.
The lithium mediated reduction of N-2 is one of the only available approaches to electrochemical ammonia production at significant yields under ambient conditions. However, much remains to be investigated about the various electrochemical processes and side reactions that are involved. Herein, we have examined the effects of parameters including electrode potential, convection, N-2 pressure, and water content to refine and control the process. We demonstrate that a closely linear ammonia yield can be maintained during experiments up to 60 h in length, with approximately constant faradaic efficiency. This steady state operation appears to be preceded by a coating of the electrode surface with the products of the reductive electrolyte decomposition, such as LiF. We demonstrate ammonia yield rates above 1 nmol s(-1) cm(-2) and faradaic efficiencies as high as 60% through the improved control of the reaction conditions.

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