Bifunctional Covalent Organic Framework-Derived Electrocatalysts with Modulated p-Band Centers for Rechargeable Zn–Air Batteries

Jung Hyun Park, Chi Ho Lee, Jong Min Ju, Jun Hyeong Lee, Jaehun Seol, Sang Uck Lee, Jong Ho Kim

Research output: Contribution to journalArticlepeer-review


Fine control over the physicochemical structures of carbon electrocatalysts is important for improving the sluggish oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) in rechargeable Zn–air batteries. Covalent organic frameworks (COFs) are considered good candidate carbon materials because their structures can be precisely controlled. However, it remains a challenge to impart bifunctional electrocatalytic activities for both the ORR and OER to COFs. Herein, a pyridine-linked triazine covalent organic framework (PTCOF) with well-defined active sites and pores is readily prepared under mild conditions, and its electronic structure is modulated by incorporating Co nanoparticles (CoNP-PTCOF) to induce bifunctional electrocatalytic activities for the ORR and OER. The CoNP-PTCOF exhibits lower overpotentials for both ORR and OER with outstanding stability. Computational simulations find that the p-band center of CoNP-PTCOF down-shifted by charge transfer, compared to pristine PTCOF, facilitate the adsorption and desorption of oxygen intermediates on the pyridinic carbon active sites during the reactions. The Zn–air battery assembled with bifunctional CoNP-PTCOF exhibits a small voltage gap of 0.83 V and superior durability for 720 cycles as compared with a battery containing commercial Pt/C and RuO2. This strategy for modulating COF electrocatalytic activities can be extended for designing diverse carbon electrocatalysts.

Original languageEnglish (US)
Article number2101727
JournalAdvanced Functional Materials
Issue number25
StatePublished - Jun 16 2021
Externally publishedYes


  • bifunctional electrocatalysts
  • covalent organic frameworks
  • oxygen evolution reaction
  • oxygen reduction reaction
  • Zn–air batteries

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • General Chemistry
  • Biomaterials
  • General Materials Science
  • Condensed Matter Physics
  • Electrochemistry


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