Litcius/Paper detail

Activating Nitrogen‐doped Graphene Oxygen Reduction Electrocatalysts in Acidic Electrolytes using Hydrophobic Cavities and Proton‐conductive Particles

Santosh K. Singh, Kotaro Takeyasu, Kaito Homma, S. Ito, Takashi Morinaga, Yuto Endo, Moeko Furukawa, Toshiyuki Mori, Hirohito Ogasawara, Junji Nakamura

2022Angewandte Chemie International Edition18 citationsDOIOpen Access PDF

Abstract

Abstract 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 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 SiO 2 particles coated with ionic liquid polymer/Nafion® which kept the high onset potentials with an increased current density even in acidic media.

Topics & Concepts

ElectrolyteChemistryProtonRedoxGrapheneNitrogenOxygenConductivityIonic bondingInorganic chemistryPhysical chemistryMaterials scienceNanotechnologyElectrodeIonPhysicsOrganic chemistryQuantum mechanicsElectrocatalysts for Energy ConversionFuel Cells and Related MaterialsAdvanced battery technologies research