Journal
ADVANCED SCIENCE
Volume 7, Issue 12, Pages -Publisher
WILEY
DOI: 10.1002/advs.202000176
Keywords
density functional calculations; Fe-N-4-C catalysts; fuel cells; oxygen reduction; poisoning kinetics
Categories
Funding
- National Key Research and Development Program of China [2017YFB0701600]
- National Science Foundation of China [51622103, 11874036]
- Guangdong Province Key Area RD Program [2019B010940001]
- Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program [2017BT01N111]
- Guangdong Natural Science Foundation for Distinguished Young Scholars [2016A030306035]
- Basic Research Project of Shenzhen, China [JCYJ20170412171430026, JCYJ20190809172617313]
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Fe-N-C materials have shown a promising nonprecious oxygen reduction reaction (ORR) electrocatalyst yet their active site structure remains elusive. Several previous works suggest the existence of a mysterious axial ligand on the Fe center, which, however, is still unclarified. In this study, the mysterious axial ligand is identified as a hydroxyl ligand on the Fe centers and selectively promotes the ORR activities depending on different Fe-N-4-C configurations, on which the adsorption free energy of the hydroxyl ligand also differs greatly. The selective formation of hydroxyl ligand on specific Fe-N-C configurations can resolve contradictories between previous theoretical and experimental results regarding the ORR activities and associated active configurations of Fe-N-C catalysts. It also explains the pH-dependent ORR activities and, moreover, a previously unreported pH-dependent poisoning kinetics of the Fe-N-C catalysts.
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