Sulfur-Linked Covalent Triazine Frameworks Doped with Coordinatively Unsaturated Cu(I) as Electrocatalysts for Oxygen Reduction

Kazuyuki Iwase, Kazuhide Kamiya, Masaru Miyayama, Kazuhito Hashimoto, Shuji Nakanishi

研究成果: Article査読

19 被引用数 (Scopus)

抄録

This work confirms a trade-off relationship between the high redox potential of Cu and the oxygen-binding ability of Cu-based oxygen reduction reaction (ORR) electrocatalysts. As the ORR is mediated by Cu(I) species, a positive shift of the Cu(II/I) potential is required to increase the ORR onset potential. However, the ready simultaneous autoreduction of Cu(II) to Cu(I) in Cu complexes, owing to high redox potentials, results in the formation of a closed tetrahedral configuration that is inactive for O2 adsorption and, therefore, for the ORR. To mitigate this problem, we synthesized a Cu-modified S-linked covalent triazine framework (Cu−S-CTF) as an electrocatalyst for the ORR in neutral solutions. The Cu(I) ions in this material have a distorted three-coordinated structure with accessible coordination sites for O2, because the inflexibility of the CTF suppresses the formation of the tetrahedral configuration. The ORR onset potential of Cu−S-CTF was 880 mV versus a reversible hydrogen electrode at pH 7. This is the first example of an ORR electrocatalyst containing Cu sites with both high redox potential and oxygen-binding ability.

本文言語English
ページ(範囲)805-810
ページ数6
ジャーナルChemElectroChem
5
5
DOI
出版ステータスPublished - 2018 3月
外部発表はい

ASJC Scopus subject areas

  • 触媒
  • 電気化学

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