Oxidation of Synthetic Annite Mica Characterized by 57Fe Mossbauer Spectroscopy: Hydrogen De-Intercalation and Host-Layer Valence State Populations

Author(s):  
I. A. D. Christie ◽  
D. G. Rancourt ◽  
H. Kodama ◽  
E. Murad ◽  
J.-L. Robert
1992 ◽  
Vol 1 (1) ◽  
pp. 461-469
Author(s):  
B. Malaman ◽  
R. Gérardin ◽  
G. Le Caer ◽  
S. Obbade ◽  
S. Miraglia ◽  
...  

Author(s):  
Jingkun Li ◽  
Moulay-Tahar Sougrati ◽  
andrea Zitolo ◽  
James Ablett ◽  
ismail can oguz ◽  
...  

While Fe-N-C materials are a promising alternative to platinum for catalyzing oxygen reduction in acidic polymer fuel cells, limited understanding of their operando degradation restricts rational approaches towards improved durability. Here we show that Fe-N-C catalysts initially comprising two distinct FeNx sites (S1 and S2) degrade via the transformation of S1 into iron oxides while the structure and number of S2 were unmodified. Structure-activity correlations drawn from end-of-test 57Fe Mössbauer spectroscopy reveal that both sites initially contribute to the ORR activity but only S2 significantly contributes after 50 h of operation. From in situ 57Fe Mössbauer spectroscopy in inert gas coupled to calculations of the Mössbauer signature of FeNx moieties in different electronic states, we identify S1 to be a high-spin FeN4C12 moiety and S2 a low- or intermediate spin FeN4C10 moiety. These insights lay the ground for rational approaches towards Fe-N-C cathodes with improved durability in acidic fuel cells.<br>


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