Design Principles of Nitrogen‐Doped Carbon Catalysts for Oxygen Reduction Reaction

Nitrogen‐doped carbon catalysts are attracting significant attention as alternative electrocatalysts to platinum owing to their high activity and durability in fuel cells’ oxygen reduction reaction (ORR), resource availability, and low catalyst cost. Pyridinic nitrogen forms the active site of the O...

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Main Authors: Kenji Hayashida, Bang Lu, Satoru Takakusagi, Junji Nakamura, Kotaro Takeyasu
Format: Article
Language:English
Published: Wiley-VCH 2025-07-01
Series:ChemElectroChem
Subjects:
Online Access:https://doi.org/10.1002/celc.202500089
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author Kenji Hayashida
Bang Lu
Satoru Takakusagi
Junji Nakamura
Kotaro Takeyasu
author_facet Kenji Hayashida
Bang Lu
Satoru Takakusagi
Junji Nakamura
Kotaro Takeyasu
author_sort Kenji Hayashida
collection DOAJ
description Nitrogen‐doped carbon catalysts are attracting significant attention as alternative electrocatalysts to platinum owing to their high activity and durability in fuel cells’ oxygen reduction reaction (ORR), resource availability, and low catalyst cost. Pyridinic nitrogen forms the active site of the ORR and that the reduction of pyridinium ions is discovered and adsorption of molecular oxygen are coupled with a unique reaction mechanism. The deactivation of nitrogen‐doped carbon catalysts in acid electrolytes is attributed to the protonation of pyridinic nitrogen and the associated hydration is reported. This concept is demonstrated by the increased activity of nitrogen‐doped graphene catalysts, whose hydrophobicity is enhanced by the 3D structure. To further enhance the catalytic activity of nitrogen‐doped carbon catalysts, the electronic configuration of the active sites, particularly the degree of electron localization and spin, plays a crucial role. As an example, the introduction of active sites through five‐membered ring structures is presented, along with their characterization by X‐ray absorption spectroscopy.
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spelling doaj-art-2522a2f81dcd4e50aace6bb6aba75f302025-08-20T03:16:43ZengWiley-VCHChemElectroChem2196-02162025-07-011214n/an/a10.1002/celc.202500089Design Principles of Nitrogen‐Doped Carbon Catalysts for Oxygen Reduction ReactionKenji Hayashida0Bang Lu1Satoru Takakusagi2Junji Nakamura3Kotaro Takeyasu4Graduate School of Science and Technology University of Tsukuba 1‐1‐1 Tennodai Tsukuba 305‐8573 Ibaraki JapanInstitute for Catalysis Hokkaido University N21W10 Sapporo 001‐0021 Hokkaido JapanInstitute for Catalysis Hokkaido University N21W10 Sapporo 001‐0021 Hokkaido JapanInternational Institute for Carbon‐Neutral Energy Research (I2CNER) Kyushu University 744 Motooka, Nishi‐ku Fukuoka‐shi 819‐0395 Fukuoka JapanInstitute for Catalysis Hokkaido University N21W10 Sapporo 001‐0021 Hokkaido JapanNitrogen‐doped carbon catalysts are attracting significant attention as alternative electrocatalysts to platinum owing to their high activity and durability in fuel cells’ oxygen reduction reaction (ORR), resource availability, and low catalyst cost. Pyridinic nitrogen forms the active site of the ORR and that the reduction of pyridinium ions is discovered and adsorption of molecular oxygen are coupled with a unique reaction mechanism. The deactivation of nitrogen‐doped carbon catalysts in acid electrolytes is attributed to the protonation of pyridinic nitrogen and the associated hydration is reported. This concept is demonstrated by the increased activity of nitrogen‐doped graphene catalysts, whose hydrophobicity is enhanced by the 3D structure. To further enhance the catalytic activity of nitrogen‐doped carbon catalysts, the electronic configuration of the active sites, particularly the degree of electron localization and spin, plays a crucial role. As an example, the introduction of active sites through five‐membered ring structures is presented, along with their characterization by X‐ray absorption spectroscopy.https://doi.org/10.1002/celc.202500089hydrophobicitynitrogen‐doped carbonsoxygen reduction reactionspyridinic nitrogenreaction mechanisms
spellingShingle Kenji Hayashida
Bang Lu
Satoru Takakusagi
Junji Nakamura
Kotaro Takeyasu
Design Principles of Nitrogen‐Doped Carbon Catalysts for Oxygen Reduction Reaction
ChemElectroChem
hydrophobicity
nitrogen‐doped carbons
oxygen reduction reactions
pyridinic nitrogen
reaction mechanisms
title Design Principles of Nitrogen‐Doped Carbon Catalysts for Oxygen Reduction Reaction
title_full Design Principles of Nitrogen‐Doped Carbon Catalysts for Oxygen Reduction Reaction
title_fullStr Design Principles of Nitrogen‐Doped Carbon Catalysts for Oxygen Reduction Reaction
title_full_unstemmed Design Principles of Nitrogen‐Doped Carbon Catalysts for Oxygen Reduction Reaction
title_short Design Principles of Nitrogen‐Doped Carbon Catalysts for Oxygen Reduction Reaction
title_sort design principles of nitrogen doped carbon catalysts for oxygen reduction reaction
topic hydrophobicity
nitrogen‐doped carbons
oxygen reduction reactions
pyridinic nitrogen
reaction mechanisms
url https://doi.org/10.1002/celc.202500089
work_keys_str_mv AT kenjihayashida designprinciplesofnitrogendopedcarboncatalystsforoxygenreductionreaction
AT banglu designprinciplesofnitrogendopedcarboncatalystsforoxygenreductionreaction
AT satorutakakusagi designprinciplesofnitrogendopedcarboncatalystsforoxygenreductionreaction
AT junjinakamura designprinciplesofnitrogendopedcarboncatalystsforoxygenreductionreaction
AT kotarotakeyasu designprinciplesofnitrogendopedcarboncatalystsforoxygenreductionreaction