Single-atom Co-N4 catalytic sites anchored on N-doped ordered mesoporous carbon for excellent Zn-air batteries

Na Li, Le Li, Jiawei Xia, Muhammad Arif, Shilong Zhou, Fengxiang Yin, Guangyu He, Haiqun Chen

Research output: Contribution to journalArticlepeer-review

Abstract

Developing efficient transition metal-nitrogen-carbon (TM-N-C) catalysts with abundant accessible active sites has been in the limelight in recent years due to their exceptional application potential in Zn-air batteries (ZABs). Herein, we report the simple and environmentally-friendly fabrication of a single-atom Co electrocatalyst, Co-SA/N-C900, via in-suit pyrolysis of the co-precursor containing sucrose, dicyandiamide, and Co salts. The Co single atoms coordinated with adjacent N atoms are anchored on the doped ordered mesoporous carbon, generating the atomic Co-N4 moiety. Co-SA/N-C900 displays high oxygen reduction reaction (ORR) activity with an onset potential of 0.96 V and a half-wave potential of 0.87 V. Notably, the liquid ZAB with Co-SA/N-C900 catalyst exhibits exceptional discharge specific capacity of 706.38 mAh g–1, peak power density of 191.11 mW cm–2, and excellent stability at high current densities up to 100 mA cm–2, surpassing commercial Pt/C. According to the density functional theory (DFT) study, the Co-N4 moiety with graphitic N dopants can decrease the rate-determining step (RDS) energy barrier and thus accelerate the ORR process. This study offers experimental and theoretical guidelines for the rational design of TM-N-C catalysts for practical implementation with notable ORR activity for application in ZABs.

Original languageEnglish
Pages (from-to)224-231
Number of pages8
JournalJournal of Materials Science and Technology
Volume139
DOIs
StatePublished - 10 Mar 2023
Externally publishedYes

Keywords

  • Co-N active sites
  • DFT study
  • Oxygen reduction reaction
  • Single-atom electrocatalyst
  • Zn-air battery

ASJC Scopus subject areas

  • Ceramics and Composites
  • Mechanics of Materials
  • Mechanical Engineering
  • Polymers and Plastics
  • Metals and Alloys
  • Materials Chemistry

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