TY - JOUR
T1 - Low temperature ammonia synthesis by surface protonics over metal supported catalysts
AU - Sekine, Yasushi
N1 - Publisher Copyright:
© 2023 The Royal Society of Chemistry.
PY - 2022/11/29
Y1 - 2022/11/29
N2 - Low-temperature ammonia synthesis by applying an electric field to a solid heterogeneous catalyst was investigated to realize an on-demand, on-site catalytic process for converting distributed renewable energy into ammonia. By applying an electric field to the catalyst, even at low temperatures, the reaction proceeds efficiently by an “associative mechanism” in which proton-conducting species on the support surface promote the formation of N2Had intermediates through surface protonics. Kinetics, isotope exchange, infrared spectroscopy, X-ray spectroscopy, and AC impedance analysis were performed to clarify the effect of metal and catalyst support structure on the reaction, and an evaluation method for the surface protonics of the support was established to analyze the reaction mechanism, and further analysis using computational chemistry was also conducted. The elementary step determining catalytic activity changed from N2 dissociation to N2H formation, and this difference resulted in high activity for ammonia synthesis at low temperatures even when using base metal catalysts such as Fe and Ni.
AB - Low-temperature ammonia synthesis by applying an electric field to a solid heterogeneous catalyst was investigated to realize an on-demand, on-site catalytic process for converting distributed renewable energy into ammonia. By applying an electric field to the catalyst, even at low temperatures, the reaction proceeds efficiently by an “associative mechanism” in which proton-conducting species on the support surface promote the formation of N2Had intermediates through surface protonics. Kinetics, isotope exchange, infrared spectroscopy, X-ray spectroscopy, and AC impedance analysis were performed to clarify the effect of metal and catalyst support structure on the reaction, and an evaluation method for the surface protonics of the support was established to analyze the reaction mechanism, and further analysis using computational chemistry was also conducted. The elementary step determining catalytic activity changed from N2 dissociation to N2H formation, and this difference resulted in high activity for ammonia synthesis at low temperatures even when using base metal catalysts such as Fe and Ni.
UR - http://www.scopus.com/inward/record.url?scp=85152116937&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85152116937&partnerID=8YFLogxK
U2 - 10.1039/d2fd00146b
DO - 10.1039/d2fd00146b
M3 - Article
C2 - 37017083
AN - SCOPUS:85152116937
SN - 1359-6640
VL - 243
SP - 179
EP - 197
JO - Faraday Discussions
JF - Faraday Discussions
ER -