Exploration of Lewis basicity and oxygen reduction reaction activity in plasma-tailored nitrogen-doped carbon electrocatalysts

Oi Lun Li, Kandasamy Prabakar, Amane Kaneko, Hyun Park, Takahiro Ishizaki

研究成果: Article査読

15 被引用数 (Scopus)

抄録

The ORR electrocatalytic activity of nitrogen-doped carbon (N-doped carbon) is highly related to the type of nitrogen bondings, which is originated to the charge transfer between carbon and nitrogen. Based on Lewis theory of acid-base reactions, N-doped carbon can be defined as a Lewis base catalyst. The lone pair of electrons on the nitrogen atom mainly contributed to its reactivity, or in other terms, Lewis basicity. Herein, we fabricated selective amino-N, pyrrolic-N, nitrile-N, and oxide-N in N-doped carbon systematically, as well as compared their electrocatalytic activities and Lewis basicities for the first time. Based on the molecular structure of four starting precursors, aniline (C6H5NH2), pyrrole (C4H5N), benzonitrile (C5H7N), and nitrobenzene (C6H5NO2) were successfully formed as selective amino-N, pyrrolic-N, nitrile-N and oxide-N, respectively, via a room temperature plasma synthesis process. From the electrochemical performance, N-doped carbon catalyst with highly selective amino-N demonstrated comparatively higher ORR activity in terms of ORR onset potential and current density. Also, we confirmed the correlation between the ORR activity and Lewis basicity of various N moieties. Based on the electronic structural properties, amino-N with the most superior ORR activity also exhibited the highest basic strength among the studied C[sbnd]N bonding structure. This study provided the relationship among the structural properties, Lewis basicity, and electrocatalytic activity of selective N-doped carbon.

本文言語English
ページ(範囲)102-109
ページ数8
ジャーナルCatalysis Today
337
DOI
出版ステータスPublished - 2019 10 15

ASJC Scopus subject areas

  • 触媒
  • 化学 (全般)

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