Cited by 82Electrocatalysts for Energy ConversionCatalytic Processes in Materials ScienceCO2 Reduction Techniques and Catalysts

Potential‐Induced Spin Changes in Fe/N/C Electrocatalysts Assessed by In Situ X‐ray Emission Spectroscopy

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Saveleva, Viktoriia A., Ebner, Kathrin, Ni, Lingmei, Smolentsev, Grigory, Klose, Daniel, Zitolo, Andrea, Marelli, Elena, Li, Jingkun +7 more·2021·Angewandte Chemie International Edition

Abstract

The commercial success of the electrochemical energy conversion technologies required for the decarbonization of the energy sector requires the replacement of the noble metal‐based electrocatalysts currently used in (co‐)electrolyzers and fuel cells with inexpensive, platinum‐group metal‐free analogs. Among these, Fe/N/C‐type catalysts display promising performances for the reduction of O 2 or CO 2, but their insufficient activity and stability jeopardize their implementation in such devices. To circumvent these issues, a better understanding of the local geometric and electronic structure of their catalytic active sites under reaction conditions is needed. Herein we shed light on the electronic structure of the molecular sites in two Fe/N/C catalysts by probing their average spin state with X‐ray emission spectroscopy (XES). Chiefly, our in situ XES measurements reveal for the first time the existence of reversible, potential‐induced spin state changes in these materials.

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References 51 · Cited by 82

Authors
Saveleva, V. A., Ebner, K., Ni, L., Smolentsev, G., Klose, D., Zitolo, A., Marelli, E., Li, J., Medarde, M., Safonova, O. V., Nachtegaal, M., Jaouen, F., Kramm, U. I., Schmidt, T. J., & Herranz, J.
Affiliations
  • Paul Scherrer Institute (CH)
  • Technische Universität Darmstadt (DE)
  • ETH Zurich (CH)
  • Synchrotron SOLEIL (FR)
  • École Nationale Supérieure de Chimie de Montpellier (FR)
  • Paul Scherrer Institut Forschungsstrasse 111 5232 Villigen PSI Switzerland
Corresponding author
Herranz, Juan
Venue
Angewandte Chemie International Edition
Publisher
Wiley
Published
2021-04-12
Volume
60
Issue
21
Pages
11707-11712
ISSN
  • 1433-7851 (ISSN-L)
  • 1521-3773
OpenAlex
W3131689301
Cited by
82
References
51
Citations by year
2026: 17 · 2025: 16 · 2024: 15 · 2023: 15 · 2022: 14 · 2021: 5
FWCI
2.30
Type
journal article
Language
en
Open access
Locations
  • Angewandte Chemie International Edition (publishedVersion)
  • PubMed (publishedVersion)
  • DORA PSI (Paul Scherrer Institute) (submittedVersion, other-oa)
  • HAL (submittedVersion)
  • TUbilio (Technical University of Darmstadt) (submittedVersion)
Funders
  • Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung (PZENP2_173632, IZK0Z2_157310)
  • Bundesministerium für Bildung und Forschung (03XP0092)
  • Deutsche Forschungsgemeinschaft (KR3980/4-1)
Topics
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
  • Physical Sciences › Materials Science › Materials Chemistry › Catalytic Processes in Materials Science
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
Keywords
Fe-N-C electrocatalysts, electronic structure, spin states, oxygen reduction reaction, CO2 reduction, platinum-free electrocatalysts, active site structure, catalyst stability

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