Long-term continuous ammonia electrosynthesis

Shaofeng Li, Yuanyuan Zhou, Xianbiao Fu, Jakob B. Pedersen, Mattia Saccoccio, Suzanne Z. Andersen, Kasper Enemark-Rasmussen, Paul J. Kempen, Christian Danvad Damsgaard, Aoni Xu, Rokas Sažinas, Jon Bjarke Valbæk Mygind, Niklas H. Deissler, Jakob Kibsgaard, Peter C. K. Vesborg, Jens K. Nørskov () and Ib Chorkendorff ()
Additional contact information
Shaofeng Li: Technical University of Denmark
Yuanyuan Zhou: Technical University of Denmark
Xianbiao Fu: Technical University of Denmark
Jakob B. Pedersen: Technical University of Denmark
Mattia Saccoccio: Technical University of Denmark
Suzanne Z. Andersen: Technical University of Denmark
Kasper Enemark-Rasmussen: Technical University of Denmark
Paul J. Kempen: Technical University of Denmark
Christian Danvad Damsgaard: Technical University of Denmark
Aoni Xu: Technical University of Denmark
Rokas Sažinas: Technical University of Denmark
Jon Bjarke Valbæk Mygind: Technical University of Denmark
Niklas H. Deissler: Technical University of Denmark
Jakob Kibsgaard: Technical University of Denmark
Peter C. K. Vesborg: Technical University of Denmark
Jens K. Nørskov: Technical University of Denmark
Ib Chorkendorff: Technical University of Denmark

Nature, 2024, vol. 629, issue 8010, 92-97

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41586-024-07276-5

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