Title:
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Selective Electrochemical Nitrogen Reduction Driven by Hydrogen Bond Interactions at Metal−Ionic Liquid Interfaces
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Author:
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Ortuño, Manuel A.; Hollóczki, Oldamur; Kirchner, Barbara; López, Núria
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Abstract:
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Increasing the activity of the nitrogen reduction reaction while slowing the
detrimental hydrogen evolution reaction is a key challenge in current electrocatalysis to provide
a sustainable route to ammonia. Recently, nanoparticles in ionic liquid (IL) environments have
been found to boost the selectivity of electrochemical synthesis of ammonia from dinitrogen at
room temperature. Here, we use for the first time a fully atomistic representation of metal−IL
interfaces at the density functional theory level to understand experimental evidence, with
particular focus on the rate and selectivity determining formation of N2H intermediates
compared to hydrogen evolution. We find that decorating the metal surface with fluorinated ILs
creates specific H-bond interactions between Ru−N2H and IL anions, stabilizing this
intermediate and thus driving the selectivity of the electrochemical process. |
Publication date:
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2019-01-15 |
Subject(s):
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54 |
Rights:
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L'accés als continguts d'aquest document queda condicionat a l'acceptació de les condicions d'ús establertes per la següent llicència Creative Commons:http://creativecommons.org/licenses/by-nc-nd/4.0/ |
Pages:
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513 p. |
Document type:
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Article Article - Accepted version |
DOI:
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10.1021/acs.jpcleE.8b03409
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