Skip to main content

Thank you for visiting You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

Electroreduction of nitrogen with almost 100% current-to-ammonia efficiency


In addition to its use in the fertilizer and chemical industries1, ammonia is currently seen as a potential replacement for carbon-based fuels and as a carrier for worldwide transportation of renewable energy2. Implementation of this vision requires transformation of the existing fossil-fuel-based technology for NH3 production3 to a simpler, scale-flexible technology, such as the electrochemical lithium-mediated nitrogen-reduction reaction3,4. This provides a genuine pathway from N2 to ammonia, but it is currently hampered by limited yield rates and low efficiencies4,5,6,7,8,9,10,11,12. Here we investigate the role of the electrolyte in this reaction and present a high-efficiency, robust process that is enabled by compact ionic layering in the electrode–electrolyte interface region. The interface is generated by a high-concentration imide-based lithium-salt electrolyte, providing stabilized ammonia yield rates of 150 ± 20 nmol s−1 cm−2 and a current-to-ammonia efficiency that is close to 100%. The ionic assembly formed at the electrode surface suppresses the electrolyte decomposition and supports stable N2 reduction. Our study highlights the interrelation between the performance of the lithium-mediated nitrogen-reduction reaction and the physicochemical properties of the electrode–electrolyte interface. We anticipate that these findings will guide the development of a robust, high-performance process for sustainable ammonia production.

This is a preview of subscription content, access via your institution

Access options

Rent or buy this article

Get just this article for as long as you need it


Prices may be subject to local taxes which are calculated during checkout

Fig. 1: Electrolyte effects in the Li-NRR.
Fig. 2: Influence of the potential on the composition of the electrode surface during N2 electroreduction mediated by 2 M LiNTf2.
Fig. 3: Li-NRR performance with a bare Ni wire electrode (geometric surface area 0.15 cm2) as a function of time.
Fig. 4: Longer-term Li-NRR performance with isolated Ni electrodes.

Data availability

All data are available in the paper and its Supplementary Information. Source data that support the findings of this study are available from the corresponding authors upon reasonable request.


  1. Fowler, D. et al. The global nitrogen cycle in the twenty-first century. Phil. Trans. R. Soc. B 368, 20130164 (2013).

    Article  Google Scholar 

  2. MacFarlane, D. R. et al. Liquefied sunshine: transforming renewables into fertilizers and energy carriers with electromaterials. Adv. Mater. 32, 1904804 (2020).

    Article  CAS  Google Scholar 

  3. MacFarlane, D. R. et al. A roadmap to the ammonia economy. Joule 4, 1186–1205 (2020).

    Article  CAS  Google Scholar 

  4. Tsuneto, A., Kudo, A. & Sakata, T. Efficient electrochemical reduction of N2 to NH3 catalyzed by lithium. Chem. Lett. 22, 851–854 (1993).

    Article  Google Scholar 

  5. Tsuneto, A., Kudo, A. & Sakata, T. Lithium-mediated electrochemical reduction of high pressure N2 to NH3. J. Electroanal. Chem. 367, 183–188 (1994).

    Article  CAS  Google Scholar 

  6. Andersen, S. Z. et al. A rigorous electrochemical ammonia synthesis protocol with quantitative isotope measurements. Nature 570, 504–508 (2019).

    Article  ADS  CAS  Google Scholar 

  7. Lazouski, N., Chung, M., Williams, K., Gala, M. L. & Manthiram, K. Non-aqueous gas diffusion electrodes for rapid ammonia synthesis from nitrogen and water-splitting-derived hydrogen. Nat. Catal. 3, 463–469 (2020).

    Article  CAS  Google Scholar 

  8. Andersen, S. Z. et al. Increasing stability, efficiency, and fundamental understanding of lithium-mediated electrochemical nitrogen reduction. Energy Environ. Sci. 13, 4291–4300 (2020).

    Article  CAS  Google Scholar 

  9. Cherepanov, P. V., Krebsz, M., Hodgetts, R. Y., Simonov, A. N. & MacFarlane, D. R. Understanding the factors determining the faradaic efficiency and rate of the lithium redox-mediated N2 reduction to ammonia. J. Phys. Chem. C 125, 11402–11410 (2021).

    Article  CAS  Google Scholar 

  10. Suryanto, B. H. et al. Nitrogen reduction to ammonia at high efficiency and rates based on a phosphonium proton shuttle. Science 372, 1187–1191 (2021).

    Article  ADS  CAS  Google Scholar 

  11. Li, K. et al. Increasing current density of Li-mediated ammonia synthesis with high surface area copper electrodes. ACS Energy Lett. 7, 36–41 (2022).

    Article  ADS  CAS  Google Scholar 

  12. Li, K. et al. Enhancement of lithium-mediated ammonia synthesis by addition of oxygen. Science 374, 1593–1597 (2021).

    Article  ADS  CAS  Google Scholar 

  13. Du, H.-L. et al. Is molybdenum disulfide modified with molybdenum metal catalytically active for the nitrogen reduction reaction? J. Electrochem. Soc. 167, 146507 (2020).

    Article  ADS  CAS  Google Scholar 

  14. Choi, J. et al. Identification and elimination of false positives in electrochemical nitrogen reduction studies. Nat. Commun. 11, 5546 (2020).

    Article  ADS  CAS  Google Scholar 

  15. Choi, J. et al. Reassessment of the catalytic activity of bismuth for aqueous nitrogen electroreduction. Nat. Catal. 5, 382–384 (2022).

    Article  CAS  Google Scholar 

  16. Lazouski, N., Schiffer, Z. J., Williams, K. & Manthiram, K. Understanding continuous lithium-mediated electrochemical nitrogen reduction. Joule 3, 1127–1139 (2019).

    Article  CAS  Google Scholar 

  17. Gao, L.-F. et al. Domino effect: gold electrocatalyzing lithium reduction to accelerate nitrogen fixation. Angew. Chem. Int. Ed. 60, 5257–5261 (2021).

    Article  CAS  Google Scholar 

  18. Sonoki, H., Matsui, M. & Imanishi, N. Effect of anion species in early stage of SEI formation process. J. Electrochem. Soc. 166, A3593–A3598 (2019).

    Article  CAS  Google Scholar 

  19. Shadike, Z. et al. Identification of LiH and nanocrystalline LiF in the solid–electrolyte interphase of lithium metal anodes. Nat. Nanotechnol. 16, 549–554 (2021).

    Article  ADS  CAS  Google Scholar 

  20. Wang, L., Uosaki, K. & Noguchi, H. Effect of electrolyte concentration on the solvation structure of gold/LiTFSI–DMSO solution interface. J. Phys. Chem. C 124, 12381–12389 (2020).

    Article  CAS  Google Scholar 

  21. Zhang, W., Zhuang, H. L., Fan, L., Gao, L. & Lu, Y. A “cation-anion regulation” synergistic anode host for dendrite-free lithium metal batteries. Sci. Adv. 4, eaar4410 (2018).

    Article  ADS  Google Scholar 

  22. Tong, J. et al. Insights into the solvation and dynamic behaviors of a lithium salt in organic- and ionic liquid-based electrolytes. Phys. Chem. Chem. Phys. 21, 19216–19225 (2019).

    Article  CAS  Google Scholar 

  23. Younesi, R., Veith, G. M., Johansson, P., Edström, K. & Vegge, T. Lithium salts for advanced lithium batteries: Li–metal, Li–O2, and Li–S. Energy Environ. Sci. 8, 1905–1922 (2015).

    Article  CAS  Google Scholar 

  24. Xue, W. et al. Ultra-high-voltage Ni-rich layered cathodes in practical Li metal batteries enabled by a sulfonamide-based electrolyte. Nat. Energy 6, 495–505 (2021).

    Article  ADS  CAS  Google Scholar 

  25. Qian, J. et al. High rate and stable cycling of lithium metal anode. Nat. Commun. 6, 6362 (2015).

    Article  ADS  CAS  Google Scholar 

  26. Horwitz, G., Rodríguez, C., Factorovich, M. & Corti, H. R. Maximum electrical conductivity of associated lithium salts in solvents for lithium–air batteries. J. Phys. Chem. C 123, 12081–12087 (2019).

    Article  CAS  Google Scholar 

  27. Hodgetts, R. Y. et al. Refining universal procedures for ammonium quantification via rapid 1H NMR analysis for dinitrogen reduction studies. ACS Energy Lett. 5, 736–741 (2020).

    Article  CAS  Google Scholar 

  28. Xu, C. et al. Interface layer formation in solid polymer electrolyte lithium batteries: an XPS study. J. Mater. Chem. A 2, 7256–7264 (2014).

    Article  CAS  Google Scholar 

  29. Takeda, Y., Yamamoto, O. & Imanishi, N. Lithium dendrite formation on a lithium metal anode from liquid, polymer and solid electrolytes. Electrochemistry 84, 210–218 (2016).

    Article  CAS  Google Scholar 

  30. Rakov, D. A. et al. Engineering high-energy-density sodium battery anodes for improved cycling with superconcentrated ionic-liquid electrolytes. Nat. Mater. 19, 1096–1101 (2020).

    Article  ADS  CAS  Google Scholar 

  31. Bard, A. J. & Faulkner, L. R. in Electrochemical Methods: Fundamentals and Applications 2nd edn, Ch. 13 (John Wiley & Sons, 2001).

  32. Nilsson, V., Bernin, D., Brandell, D., Edström, K. & Johansson, P. Interactions and transport in highly concentrated LiTFSI-based electrolytes. ChemPhysChem 21, 1166–1176 (2020).

    Article  CAS  Google Scholar 

  33. Lu, Y. et al. Stable cycling of lithium metal batteries using high transference number electrolytes. Adv. Energy Mater. 5, 1402073 (2015).

    Article  Google Scholar 

  34. Haj Ibrahim, S. et al. Insight into cathode microstructure effect on the performance of molten carbonate fuel cell. J. Power Sources 491, 229562 (2021).

    Article  CAS  Google Scholar 

  35. Hodgetts, R. Y., Du, H.-L., Nguyen, T. D., MacFarlane, D. & Simonov, A. N. Electrocatalytic oxidation of hydrogen as an anode reaction for the Li-mediated N2 reduction to ammonia. ACS Catal. 12, 5231–5246 (2022).

    Article  CAS  Google Scholar 

Download references


We acknowledge funding of this work by the Australian Research Council (Discovery Project DP200101878, Centre of Excellence for Electromaterials Science CE140100012, Future Fellowship to A.N.S. (FT200100317)) and the Australian Renewable Energy Agency (‘Renewable Hydrogen for Export’ project 2018RND/009 DM015); and the Monash Centre for Electron Microscopy, Monash X-ray platform and Monash Analytical platform for providing access to the physical characterization and spectroscopic facilities. We thank Nippon Shokubai for a gift of LiFSI and F. Shanks for his assistance with the Fourier-transform infrared attenuated total reflectance spectroscopic measurements.

Author information

Authors and Affiliations



H.-L.D. conceived and did the electrochemical experiments, viscosity and conductivity measurements and co-wrote the manuscript. M.C. did the XRD and  Fourier-transform infrared attenuated total reflectance spectroscopic analyses, and assisted with monitoring long-term experiments. R.Y.H. contributed to the reproducibility studies and performed the 1H NMR analysis of ammonia. P.V.C. collected and analysed XPS data. C.K.N. did nitrite/nitrate measurements, and the SEM and EDS analyses. K.M. contributed to conductivity measurements and collected the NMR data for the electrolyte stability. D.R.M. and A.N.S. conceived the experiments, directed the project and co-wrote the manuscript.

Corresponding authors

Correspondence to Douglas R. MacFarlane or Alexandr N. Simonov.

Ethics declarations

Competing interests

H.-L.D., D.R.M. and A.N.S. are inventors on an Australian provisional patent application that covers aspects of the work reported here, and which has been licensed to Jupiter Ionics. D.R.M. and A.N.S. have minority equity ownership, as well as management and consulting roles, in Jupiter Ionics.

Peer review

Peer review information

Nature thanks anonymous reviewers for their contribution to the peer review of this work. Peer reviewer reports are available.

Additional information

Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

Supplementary Information

This file contains Supplementary Figs. 1–40, Supplementary Tables 1–18 and references.

Peer Review File

Rights and permissions

Springer Nature or its licensor holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.

Reprints and Permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Du, HL., Chatti, M., Hodgetts, R.Y. et al. Electroreduction of nitrogen with almost 100% current-to-ammonia efficiency. Nature 609, 722–727 (2022).

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI:

This article is cited by


By submitting a comment you agree to abide by our Terms and Community Guidelines. If you find something abusive or that does not comply with our terms or guidelines please flag it as inappropriate.


Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing