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
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
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