Journal article
Electrosynthesis of ammonia with high selectivity and high rates via engineering of the solid-electrolyte interphase
Department of Physics, Technical University of Denmark1
Surface Physics and Catalysis, Department of Physics, Technical University of Denmark2
Catalysis Theory Center, Department of Physics, Technical University of Denmark3
VISION – Center for Visualizing Catalytic Processes, Centers, Technical University of Denmark4
Ammonia is a large-scale commodity essential to fertilizer production, but the Haber-Bosch process leads to massive emissions of carbon dioxide. Electrochemical ammonia synthesis is an attractive alternative pathway, but the process is still limited by low ammonia production rate and faradaic efficiency.
Herein, guided by our theoretical model, we present a highly efficient lithium-mediated process enabled by using different lithium salts, leading to the formation of a uniform solid-electrolyte interphase (SEI) layer on a porous copper electrode. The uniform lithium-fluoride-enriched SEI layer provides an ammonia production rate of 2.5 ± 0.1 μmol s−1 cmgeo−2 at a current density of −1 A cmgeo−2 with 71% ± 3% faradaic efficiency under 20 bar nitrogen.
Experimental X-ray analysis reveals that the lithium tetrafluoroborate electrolyte induces the formation of a compact and uniform SEI layer, which facilitates homogeneous lithium plating, suppresses the undesired hydrogen evolution as well as electrolyte decomposition, and enhances the nitrogen reduction.
Language: | English |
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Year: | 2022 |
Pages: | 2083-2101 |
ISSN: | 25424351 and 25424785 |
Types: | Journal article |
DOI: | 10.1016/j.joule.2022.07.009 |
ORCIDs: | Li, Katja , Saccoccio, Mattia , Sažinas, Rokas , Andersen, Suzanne Z. , Pedersen, Jakob B. , Shadravan, Vahid , Chakraborty, Debasish , Kibsgaard, Jakob , Vesborg, Peter C.K. , Nørskov, Jens K. and Chorkendorff, Ib |