期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 51, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202212506
关键词
Fuel Cell; N-Doped Graphene Catalyst; Oxygen Reduction Reaction
资金
- JSPS KAKENHI
- Kato Foundation for Promotion of Science
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science Program
- [17F17345]
- [19K15356]
- [20H00316]
- [KJ-3031]
- [DE-AC02-76SF00515]
The activity of pyridinic-nitrogen-doped graphene for the oxygen reduction reaction (ORR) decreases under acidic conditions. By increasing proton conductivity in the hydrophobic cavity, the deactivation can be prevented.
Although pyridinic-nitrogen (pyri-N) doped graphene is highly active for the oxygen reduction reaction (ORR) of fuel cells in alkaline media, the activity critically decreases under acidic conditions. We report on how to prevent the deactivation based on the mechanistic understanding that O2+pyri-NH++e--> O2,a+pyri-NH ${{{\rm O}}_{2}+{\rm p}{\rm y}{\rm r}{\rm i}{\rm { -}}{\rm N}{{\rm H}}<^>{+}+{{\rm e}}<^>{-}{\to }_{\ }<^>{{\rm \ }}{{\rm O}}_{2,{\rm a}}+{\rm p}{\rm y}{\rm r}{\rm i}{\rm { -}}{\rm N}{\rm H}}$ governs the ORR kinetics. First, we considered that the deactivation is due to the hydration of pyri-NH+, leading to a lower shift of the redox potential. Introducing the hydrophobic cavity prevented the hydration of pyri-NH+ but inhibited the proton transport. We then increased proton conductivity in the hydrophobic cavity by introducing SiO2 particles coated with ionic liquid polymer/Nafion (R) which kept the high onset potentials with an increased current density even in acidic media.
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