期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 21, 页码 11707-11712出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202016951
关键词
electrocatalysts; in situ; Moessbauer spectroscopy; non-resonant X-ray emission spectroscopy
资金
- Swiss National Science Foundation (SNSF) through the Ambizione Energy [PZENP2_173632]
- SNSF [IZK0Z2_157310]
- German Federal Ministry of Research and Education
- German Research Foundation [03XP0092, KR3980/4-1]
- Swiss National Science Foundation (SNF) [IZK0Z2_157310, PZENP2_173632] Funding Source: Swiss National Science Foundation (SNF)
This study investigates the electronic structure of molecular sites in two Fe/N/C catalysts by probing their average spin state using X-ray emission spectroscopy (XES), revealing for the first time the existence of reversible, potential-induced spin state changes in these materials.
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 CO2, 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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