Article, 2024

Long-term continuous ammonia electrosynthesis

Nature, ISSN 0028-0836, 1476-4687, Volume 629, 8010, Pages 92-97, 10.1038/s41586-024-07276-5

Contributors

Li, Shaofeng 0000-0002-9500-2636 [1] Zhou, Yuanyuan [1] Fu, Xianbiao 0000-0001-5172-3354 [1] Pedersen, Jakob Bruun 0000-0002-4825-3221 [1] Saccoccio, Mattia 0000-0002-5365-3158 [1] Andersen, Suzanne Zamany 0000-0003-2681-7978 [1] Enemark-Rasmussen, Kasper 0000-0001-7455-7512 [1] Kempen, Paul Joseph 0000-0003-2179-2257 [1] Damsgaard, Christian Danvad 0000-0002-3117-8616 [1] Xu, Aoni 0000-0001-5114-8740 [1] Sažinas, Rokas 0000-0002-4422-890X [1] Mygind, Jon Bjarke Valbaek 0000-0003-2032-4152 [1] Deissler, Niklas Henrik 0000-0001-9117-5030 [1] Kibsgaard, Jakob 0000-0002-9219-816X [1] Vesborg, Peter Christian Kjærgaard 0000-0002-3761-4212 [1] Nørskov, Jens Kehlet 0000-0002-4427-7728 (Corresponding author) [1] Chorkendorff, I B 0000-0003-2738-0325 (Corresponding author) [1]

Affiliations

  1. [1] Technical University of Denmark
  2. [NORA names: DTU Technical University of Denmark; University; Denmark; Europe, EU; Nordic; OECD]

Abstract

Ammonia is crucial as a fertilizer and in the chemical industry and is considered to be a carbon-free fuel1. Ammonia electrosynthesis from nitrogen under ambient conditions offers an attractive alternative to the Haber–Bosch process2,3, and lithium-mediated nitrogen reduction represents a promising approach to continuous-flow ammonia electrosynthesis, coupling nitrogen reduction with hydrogen oxidation4. However, tetrahydrofuran, which is commonly used as a solvent, impedes long-term ammonia production owing to polymerization and volatility problems. Here we show that a chain-ether-based electrolyte enables long-term continuous ammonia synthesis. We find that a chain-ether-based solvent exhibits non-polymerization properties and a high boiling point (162 °C) and forms a compact solid-electrolyte interphase layer on the gas diffusion electrode, facilitating ammonia release in the gas phase and ensuring electrolyte stability. We demonstrate 300 h of continuous operation in a flow electrolyser with a 25 cm2 electrode at 1 bar pressure and room temperature, and achieve a current-to-ammonia efficiency of 64 ± 1% with a gas-phase ammonia content of approximately 98%. Our results highlight the crucial role of the solvent in long-term continuous ammonia synthesis.

Keywords

Haber-Bosch, alternative, ambient conditions, ammonia, ammonia content, ammonia electrosynthesis, ammonia production, ammonia release, ammonia synthesis, chemical, chemical industry, conditions, content, continuous operation, coupling, diffusion electrode, efficiency, electrode, electrolyser, electrolyte, electrolyte stability, electrosynthesis, fertility, flow, gas, gas diffusion electrode, gas phase, hydrogen, industry, interphase layer, layer, nitrogen, nitrogen reduction, operation, phase, polymerization, problem, production, properties, reduction, release, results, room, room temperature, solid electrolyte interphase layer, solvent, stability, synthesis, temperature, tetrahydrofuran, volatility, volatility problem

Funders

  • European Research Council
  • Danish National Research Foundation
  • Innovation Fund Denmark
  • European Commission
  • The Velux Foundations

Data Provider: Digital Science