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  Kinetics of NH3 desorption and diffusion on Pt: Implications for the Ostwald process

Borodin, D., Rahinov, I., Galparsoro, O., Fingerhut, J., Schwarzer, M., Golibrzuch, K., et al. (2021). Kinetics of NH3 desorption and diffusion on Pt: Implications for the Ostwald process. Journal of the American Chemical Society, 143(43), 18305-18316. doi:10.1021/jacs.1c09269.

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Datensatz-Permalink: https://hdl.handle.net/21.11116/0000-000A-67A1-C Versions-Permalink: https://hdl.handle.net/21.11116/0000-000A-67A4-9
Genre: Zeitschriftenartikel

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 Urheber:
Borodin, D.1, Autor           
Rahinov, I., Autor
Galparsoro, O., Autor           
Fingerhut, J., Autor
Schwarzer, M., Autor
Golibrzuch, K.2, Autor           
Skoulatakis, G.3, Autor           
Auerbach, D. J.2, Autor           
Kandratsenka, A.3, Autor           
Kitsopoulos, T. N.2, Autor           
Wodtke, A. M.2, Autor           
Affiliations:
1Department of Dynamics at Surfaces, MPI for Biophysical Chemistry, Max Planck Society, ou_persistent22              
2Department of Dynamics at Surfaces, MPI for biophysical chemistry, Max Planck Society, ou_578600              
3Department of Dynamics at Surfaces, MPI for Biophysical Chemistry, Max Planck Society, ou_578600              

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Schlagwörter: -
 Zusammenfassung: ABSTRACT: We report accurate time-resolved measurements of
NH3 desorption from Pt(111) and Pt(332) and use these results to
determine elementary rate constants for desorption from steps,
from (111) terrace sites and for diffusion on (111) terraces.
Modeling the extracted rate constants with transition state theory,
we find that conventional models for partition functions, which
rely on uncoupled degrees of freedom (DOFs), are not able to
reproduce the experimental observations. The results can be
reproduced using a more sophisticated partition function, which
couples DOFs that are most sensitive to NH3 translation parallel to
the surface; this approach yields accurate values for the NH3
binding energy to Pt(111) (1.13 ± 0.02 eV) and the diffusion
barrier (0.71 ± 0.04 eV). In addition, we determine NH3’s binding
energy preference for steps over terraces on Pt (0.23 ± 0.03 eV). The ratio of the diffusion barrier to desorption energy is ∼0.65, in
violation of the so-called 12% rule. Using our derived diffusion/desorption rates, we explain why established rate models of the
Ostwald process incorrectly predict low selectivity and yields of NO under typical reactor operating conditions. Our results suggest
that mean-field kinetics models have limited applicability for modeling the Ostwald process.

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Sprache(n): eng - English
 Datum: 2021-09-012021-10-212021-11-03
 Publikationsstatus: Erschienen
 Seiten: -
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: DOI: 10.1021/jacs.1c09269
 Art des Abschluß: -

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Projektinformation

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Projektname : PSBICH 3219 (KID)
Grant ID : -
Förderprogramm : Horizon 2020 (H2020)
Förderorganisation : European Commission (EC)
Projektname : BENCh gradute school
Grant ID : -
Förderprogramm : DFG (389479699/GRK2455)
Förderorganisation : Deutsche Forschungsgemeinschaft
Projektname : -
Grant ID : -
Förderprogramm : ISF 2187/19
Förderorganisation : Israel Science Foundation (ISF)
Projektname : -
Grant ID : -
Förderprogramm : Grant 31044
Förderorganisation : Open University of Israel Research Authority
Projektname : -
Grant ID : -
Förderprogramm : Grant PID2019-107396GB-I00/AEI/10.13039/501100011033
Förderorganisation : Spanish Ministerio de Ciercia e Innovacion

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Titel: Journal of the American Chemical Society
  Andere :
Genre der Quelle: Zeitschrift
 Urheber:
Affiliations:
Ort, Verlag, Ausgabe: -
Seiten: - Band / Heft: 143 (43) Artikelnummer: - Start- / Endseite: 18305 - 18316 Identifikator: -