TY - JOUR
T1 - Electrosynthesis of ammonia with high selectivity and high rates via engineering of the solid-electrolyte interphase
AU - Li, Shaofeng
AU - Zhou, Yuanyuan
AU - Li, Katja
AU - Saccoccio, Mattia
AU - Sažinas, Rokas
AU - Andersen, Suzanne Z.
AU - Pedersen, Jakob B.
AU - Fu, Xianbiao
AU - Shadravan, Vahid
AU - Chakraborty, Debasish
AU - Kibsgaard, Jakob
AU - Vesborg, Peter C.K.
AU - Nørskov, Jens K.
AU - Chorkendorff, Ib
N1 - Publisher Copyright:
© 2022 The Author(s)
PY - 2022
Y1 - 2022
N2 - 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.
AB - 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.
U2 - 10.1016/j.joule.2022.07.009
DO - 10.1016/j.joule.2022.07.009
M3 - Journal article
C2 - 36188748
AN - SCOPUS:85138153666
SN - 2542-4785
VL - 6
SP - 2083
EP - 2101
JO - Joule
JF - Joule
IS - 9
ER -