TY - JOUR
T1 - Plasma-catalytic ammonia synthesis beyond thermal equilibrium on Ru-based catalysts in non-thermal plasma
AU - Rouwenhorst, Kevin H.R.
AU - Burbach, Hugo G.B.
AU - Vogel, Dave W.
AU - Núñez Paulí, Judit
AU - Geerdink, Bert
AU - Lefferts, Leon
N1 - Funding Information:
This project is co-financed by TKI-Energie from Toeslag voor Topconsortia voor Kennis en Innovatie (TKI) from the Ministry of Economic Affairs and Climate Policy, the Netherlands. The authors acknowledge K. Altena-Schildkamp for N2chemisorption and CO chemisorption measurements. The authors acknowledge T. M. L. Velthuizen for XRF analysis.
Publisher Copyright:
© The Royal Society of Chemistry 2021.
PY - 2021/4/21
Y1 - 2021/4/21
N2 - Recently it was proposed that plasma-catalytic NH3synthesis with excited N2allows for conversions beyond thermal equilibrium. We show that this is indeed possible with experimental data for Ru catalysts at temperatures above 300 °C, resulting in significant thermal activity for NH3synthesis. The resulting NH3concentration is determined by competition between, on the one hand, dissociative adsorption of ground-state N2and adsorption of plasma-generated N radical species with subsequent hydrogenation to NH3, and on the other hand, thermal-catalytic decomposition of NH3. At temperatures below 300 °C, plasma-catalytic ammonia synthesis is attributed to adsorption of N radicals, generated in the plasma, with subsequent hydrogenation to NH3. These findings imply that catalysts with thermal activity are not suitable for plasma catalysis, aiming at conversion beyond equilibrium, as these also catalyze the reverse decomposition reaction.
AB - Recently it was proposed that plasma-catalytic NH3synthesis with excited N2allows for conversions beyond thermal equilibrium. We show that this is indeed possible with experimental data for Ru catalysts at temperatures above 300 °C, resulting in significant thermal activity for NH3synthesis. The resulting NH3concentration is determined by competition between, on the one hand, dissociative adsorption of ground-state N2and adsorption of plasma-generated N radical species with subsequent hydrogenation to NH3, and on the other hand, thermal-catalytic decomposition of NH3. At temperatures below 300 °C, plasma-catalytic ammonia synthesis is attributed to adsorption of N radicals, generated in the plasma, with subsequent hydrogenation to NH3. These findings imply that catalysts with thermal activity are not suitable for plasma catalysis, aiming at conversion beyond equilibrium, as these also catalyze the reverse decomposition reaction.
UR - http://www.scopus.com/inward/record.url?scp=85104968538&partnerID=8YFLogxK
U2 - 10.1039/d0cy02189j
DO - 10.1039/d0cy02189j
M3 - Article
AN - SCOPUS:85104968538
VL - 11
SP - 2834
EP - 2843
JO - Catalysis science & technology
JF - Catalysis science & technology
SN - 2044-4753
IS - 8
ER -