Theory-Guided Regulation of FeN4 Spin State by Neighboring Cu Atoms for Enhanced Oxygen Reduction Electrocatalysis in Flexible Metal-Air Batteries.
Angew Chem Int Ed Engl
; 61(27): e202201007, 2022 Jul 04.
Article
em En
| MEDLINE
| ID: mdl-35468253
ABSTRACT
Iron, nitrogen-codoped carbon (Fe-N-C) nanocomposites have emerged as viable electrocatalysts for the oxygen reduction reaction (ORR) due to the formation of FeNx Cy coordination moieties. In this study, results from first-principles calculations show a nearly linear correlation of the energy barriers of key reaction steps with the Fe magnetic moment. Experimentally, when single Cu sites are incorporated into Fe-N-C aerogels (denoted as NCAG/Fe-Cu), the Fe centers exhibit a reduced magnetic moment and markedly enhanced ORR activity within a wide pH range of 0-14. With the NCAG/Fe-Cu nanocomposites used as the cathode catalyst in a neutral/quasi-solid aluminum-air and alkaline/quasi-solid zinc-air battery, both achieve a remarkable performance with an ultrahigh open-circuit voltage of 2.00 and 1.51â
V, large power density of 130 and 186â
mW cm-2 , and good mechanical flexibility, all markedly better than those with commercial Pt/C or Pt/C-RuO2 catalysts at the cathode.
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MEDLINE
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En
Ano de publicação:
2022
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Article