Lithium-mediated electrochemical nitrogen reduction: Mechanistic insights to enhance performance
Name
1-s2.0-S2589004221010737-main.pdf
Description
Published version
Size
2.4 MB
Format
Unknown
Checksum (MD5)
172c5ae81595dbb696b5c04a762151be
Author(s)
Cai, Xiyang
Fu, Cehuang
Iriawan, Haldrian
Yang, Fan
Wu, Aiming
Luo, Liuxuan
Shen, Shuiyun
Wei, Guanghua
Shao-Horn, Yang
Zhang, Junliang
Date Issued
October 2021
Journal
iScience
Publisher
Elsevier BV
Citation
Cai, Xiyang, Fu, Cehuang, Iriawan, Haldrian, Yang, Fan, Wu, Aiming et al. 2021. "Lithium-mediated electrochemical nitrogen reduction: Mechanistic insights to enhance performance." iScience, 24 (10).
Version
Final published version
Abstract
Green synthesis of ammonia by electrochemical nitrogen reduction reaction (NRR) shows great potential as an alternative to the Haber-Bosch process but is hampered by sluggish production rate and low Faradaic efficiency. Recently, lithium-mediated electrochemical NRR has received renewed attention due to its reproducibility. However, further improvement of the system is restricted by limited recognition of its mechanism. Herein, we demonstrate that lithium-mediated NRR began with electrochemical deposition of lithium, followed by two chemical processes of dinitrogen splitting and protonation to ammonia. Furthermore, we quantified the extent to which the freshly deposited active lithium lost its activity toward NRR due to a parasitic reaction between lithium and electrolyte. A high ammonia yield of 0.410 ± 0.038 μg s-1 cm-2 geo and Faradaic efficiency of 39.5 ± 1.7% were achieved at 20 mA cm-2 geo and 10 mA cm-2 geo, respectively, which can be attributed to fresher lithium obtained at high current density.
MIT Department
Massachusetts Institute of Technology. Department of Materials Science and Engineering
Massachusetts Institute of Technology. Department of Mechanical Engineering
Terms of Use
Creative Commons Attribution 4.0 International license
Persistent DSpace Link
DOI of Published Version
https://doi.org/10.1016/j.isci.2021.103105
