Repository logo

Infoscience

  • English
  • French
Log In
Logo EPFL, École polytechnique fédérale de Lausanne

Infoscience

  • English
  • French
Log In
  1. Home
  2. Academic and Research Output
  3. Preprints and Working Papers
  4. Disentangling Site-Selective Redox Couples for N2O Activation on Fe-Exchanged SSZ-13 Using Modulated Excitation Operando EPR spectroscopy
 
preprint

Disentangling Site-Selective Redox Couples for N2O Activation on Fe-Exchanged SSZ-13 Using Modulated Excitation Operando EPR spectroscopy

Fischer, Jörg W. A.
•
Cano-Blanco, Daniel C.  
•
Karas, Hugo
Show more
August 25, 2025

Iron-exchanged zeolites are promising materials for mitigating N2O emissions and converting methane into methanol. Here, we present site-specific kinetic analysis of N2O decomposition over Fe-SSZ13 under inert conditions and utilizing reducing agents (CH4, NH3, H2). Operando EPR measurements with phase-sensitive detection proved essential for distinguishing active sites from spectator species during reactions. The time resolution was further enhanced by using an EPR step-scan methodology. Isolated Fe2+ centers in axial coordination contribute solely to N2O decomposition without reducing agents, while FexOy clusters and Fe2+ sites in distorted geometries show redox activity when present. Quantitative kinetic analysis reveals that, in the presence of CH4, H2, and under autocatalytic conditions, the reduction half-cycle, whereas with NH3, the oxidation half-cycle is rate-limiting.

  • Files
  • Details
  • Metrics
Logo EPFL, École polytechnique fédérale de Lausanne
  • Contact
  • infoscience@epfl.ch

  • Follow us on Facebook
  • Follow us on Instagram
  • Follow us on LinkedIn
  • Follow us on X
  • Follow us on Youtube
AccessibilityLegal noticePrivacy policyCookie settingsEnd User AgreementGet helpFeedback

Infoscience is a service managed and provided by the Library and IT Services of EPFL. © EPFL, tous droits réservés