Covalent organic frameworks derived Single-Atom cobalt catalysts for boosting oxygen reduction reaction in rechargeable Zn-Air batteries

Zhenghao Chen; Hao Zheng; Jinhui Zhang; Zeyi Jiang; Cheng Bao; Chen-Hao Yeh; Nien-Chu Lai

doi:10.1016/j.jcis.2024.05.005

Covalent organic frameworks derived Single-Atom cobalt catalysts for boosting oxygen reduction reaction in rechargeable Zn-Air batteries

J Colloid Interface Sci. 2024 Sep 15:670:103-113. doi: 10.1016/j.jcis.2024.05.005. Epub 2024 May 3.

Authors

Zhenghao Chen¹, Hao Zheng¹, Jinhui Zhang¹, Zeyi Jiang¹, Cheng Bao², Chen-Hao Yeh³, Nien-Chu Lai⁴

Affiliations

¹ School of Energy and Environmental Engineering, University of Science and Technology Beijing, Beijing 100083, China.
² School of Energy and Environmental Engineering, University of Science and Technology Beijing, Beijing 100083, China. Electronic address: baocheng@mail.tsinghua.edu.cn.
³ Department of Materials Science and Engineering, Feng Chia University, Taichung 40724, Taiwan. Electronic address: chenhyeh@fcu.edu.tw.
⁴ School of Energy and Environmental Engineering, University of Science and Technology Beijing, Beijing 100083, China; Beijing Higher Institution Engineering Research Center of Energy Conservation and Environmental Protection, University of Science and Technology Beijing, Beijing 100083, China. Electronic address: nclai@ustb.edu.cn.

PMID: 38759265
DOI: 10.1016/j.jcis.2024.05.005

Abstract

The design and development of high-performance and long-life Pt-free catalysts for the oxygen reduction reaction (ORR) is of great important with respect to metal-air batteries and fuel cells. Herein, a new low-cost covalent organic frameworks (COFs)-derived CoNC single-atoms catalyst (SAC) is fabricated and compared with the engineered nanoparticle (NP) counterpart for ORR activity. The ORR performance of the SAC catalyst (Co_SA@NC) surpasses the NP counterpart (Co_NP-NC) under the same operation condition. Co_SA@NC also achieves improved long-term durability and better methanol tolerance compared with the Pt/C. The zinc-air battery assembled by the Co_SA@NC cathode delivers a higher power density and energy density than that of commercial Pt/C catalyst. Molecular dynamics (MD) is performed to explain the spontaneous evolution from clusters to single-atom metal configuration and density functional theory (DFT) calculations find that Co_SA@NC possesses lower d-band center, resulting in weaker interaction between the surface and the O-containing intermediates. Consequently, the reductive desorption of OH*, the rate-determine step, is further accelerated.

Keywords: Covalent organic framework; DFT calculation; Oxygen reduction reaction; Single-atom catalyst; Zinc-air battery.