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Title
Japanese:Structural Effects of FeN4 Active Sites Surrounded by Fourteen-Membered Ring Ligands on Oxygen Reduction Reaction Activity and Durability 
English:Structural Effects of FeN4 Active Sites Surrounded by Fourteen-Membered Ring Ligands on Oxygen Reduction Reaction Activity and Durability 
Author
Japanese: Zhiqing Feng, Soutaro Honda, Junya Ohyama, Yasushi Iwata, Keisuke Awaya, Hiroshi Yoshida, Masato Machida, Kotaro Higashi, Tomoya Uruga, Naomi Kawamura, Ryota Goto, Takeo Ichihara, Ryoichi Kojima, Makoto Moriya, Hideo Notsu, Shinsuke Nagata, Mami Miyoshi, Teruaki Hayakawa, Yuta Nabae.  
English: Zhiqing Feng, Soutaro Honda, Junya Ohyama, Yasushi Iwata, Keisuke Awaya, Hiroshi Yoshida, Masato Machida, Kotaro Higashi, Tomoya Uruga, Naomi Kawamura, Ryota Goto, Takeo Ichihara, Ryoichi Kojima, Makoto Moriya, Hideo Notsu, Shinsuke Nagata, Mami Miyoshi, Teruaki Hayakawa, Yuta Nabae.  
Language English 
Journal/Book name
Japanese:ACS Catalysis 
English:ACS Catalysis 
Volume, Number, Page Vol. 14    No. 10    pp. 7416-7425
Published date Apr. 2024 
Publisher
Japanese:American Chemical Society 
English:American Chemical Society 
Conference name
Japanese: 
English: 
Conference site
Japanese: 
English: 
Official URL https://doi.org/10.1021/acscatal.4c01122
 
DOI https://doi.org/10.1021/acscatal.4c01122
Abstract FeN4 active sites have been studied as non-Pt group metal (non-PGM) catalysts for the oxygen reduction reaction (ORR). The authors recently developed Fe(II) 1,14:7,8-ditethenotetrapyrido-[2,1,6-de:2窶ｲ,1窶ｲ6窶ｲ-gh:2窶ｳ,1窶ｳ,6窶ｳ-na][1,3,5,8,10,12] hexaazacyclotetradecine (Fe-14MR) as an FeN4 complex incorporating a 14-membered ring. This complex exhibited higher ORR activity and greater durability than Fe phthalocyanine, a conventional FeN4 complex having a 16-membered ring. In the present study, the ORR activity and durability of this Fe-14MR complex supported on C (Fe-14MR/C) were enhanced through modification of the active site structure by heating at 600 ﾂｰC and removing protons on amine groups in the Fe-14MR. Density functional theory calculations indicated that the Fe-14MR/C structure generated by heating resulted in oxygen species absorption energies close to optimal values for the ORR. The improved durability of the heat-treated Fe-14MR/C was attributed to reduced distortion of the FeN4 sites. The results suggest that designing Fe-14MR structures can be a promising approach to developing non-PGM catalysts.

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