Overcoming ammonia synthesis scaling relations with plasma-enabled catalysis

Title
Overcoming ammonia synthesis scaling relations with plasma-enabled catalysis
Authors
김종식Prateek MehtaPatrick BarbounFrancisco A. HerreraPaul RumbachDavid B. GoJason C. HicksWilliam F. Schneider
Issue Date
2018-04
Publisher
Nature catalysis
Citation
VOL 1, NO 4-275
Abstract
Correlations between the energies of elementary steps limit the rates of thermally catalysed reactions at surfaces. Here, we show how these limitations can be circumvented in ammonia synthesis by coupling catalysts to a non-thermal plasma. We postulate that plasma-induced vibrational excitations in N2 decrease dissociation barriers without influencing subsequent reaction steps. We develop a density-functional-theory-based microkinetic model to incorporate this effect, and parameterize the model using N2 vibrational excitations observed in a dielectric-barrier-discharge plasma. We predict plasma enhancement to be particularly great on metals that bind nitrogen too weakly to be active thermally. Ammonia synthesis rates observed in a dielectric-barrier-discharge plasma reactor are consistent with predicted enhancements and predicted changes in the optimal metal catalyst. The results provide guidance for optimizing catalysts for application with plasmas.
URI
http://pubs.kist.re.kr/handle/201004/67527
ISSN
2520-1158
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