Issue

Vol. 13 (2021)

Ultrasonic Plasma Engineering Toward Facile Synthesis of Single-Atom M-N4/N-Doped Carbon (M = Fe, Co) as Superior Oxygen Electrocatalyst in Rechargeable Zinc–Air Batteries

https://doi.org/10.1007/s40820-020-00581-4
Kai Chen
Department of Materials Science and Engineering, Pusan National University, 30 Jangjeon‑dong, Geumjeong‑gu, Busan 609‑735, Republic of Korea
Seonghee Kim
Department of Materials Science and Engineering, Pusan National University, 30 Jangjeon‑dong, Geumjeong‑gu, Busan 609‑735, Republic of Korea
Minyeong Je
Theoretical Materials and Chemistry Group, Institute of Inorganic Chemistry, University of Cologne, Greinstr. 6, 50939 Cologne, Germany
Heechae Choi
Theoretical Materials and Chemistry Group, Institute of Inorganic Chemistry, University of Cologne, Greinstr. 6, 50939 Cologne, Germany
http://orcid.org/0000-0002-8782-9326
Zhicong Shi
School of Materials and Energy, Guangdong University of Technology, Guangzhou 510006, People’s Republic of China
Nikola Vladimir
Faculty of Mechanical Engineering and Naval Architecture, University of Zagreb, Ivana Lucica 5, 10002 Zagreb, Croatia
Kwang Ho Kim
Department of Materials Science and Engineering, Pusan National University, 30 Jangjeon‑dong, Geumjeong‑gu, Busan 609‑735, Republic of Korea
Oi Lun Li
Department of Materials Science and Engineering, Pusan National University, 30 Jangjeon‑dong, Geumjeong‑gu, Busan 609‑735, Republic of Korea

Corresponding Author: Oi Lun Li

helenali@pusan.ac.kr

Nano-Micro Letters, Vol. 13 (2021), Article Number: 60

Abstract

As bifunctional oxygen evolution/reduction electrocatalysts, transition-metal-based single-atom-doped nitrogen–carbon (NC) matrices are promising successors of the corresponding noble-metal-based catalysts, offering the advantages of ultrahigh atom utilization efficiency and surface active energy. However, the fabrication of such matrices (e.g., well-dispersed single-atom-doped M-N4/NCs) often requires numerous steps and tedious processes. Herein, ultrasonic plasma engineering allows direct carbonization in a precursor solution containing metal phthalocyanine and aniline. When combining with the dispersion effect of ultrasonic waves, we successfully fabricated uniform single-atom M-N4 (M = Fe, Co) carbon catalysts with a production rate as high as 10 mg min−1. The Co-N4/NC presented a bifunctional potential drop of ΔE = 0.79 V, outperforming the benchmark Pt/C-Ru/C catalyst (ΔE = 0.88 V) at the same catalyst loading. Theoretical calculations revealed that Co-N4 was the major active site with superior O2 adsorption–desorption mechanisms. In a practical Zn–air battery test, the air electrode coated with Co-N4/NC exhibited a specific capacity (762.8 mAh g−1) and power density (101.62 mW cm−2), exceeding those of Pt/C-Ru/C (700.8 mAh g−1 and 89.16 mW cm−2, respectively) at the same catalyst loading. Moreover, for Co-N4/NC, the potential difference increased from 1.16 to 1.47 V after 100 charge–discharge cycles. The proposed innovative and scalable strategy was concluded to be well suited for the fabrication of single-atom-doped carbons as promising bifunctional oxygen evolution/reduction electrocatalysts for metal–air batteries.


Highlights:


1 Single-atom M-N4/N-doped carbons (M = Fe, Co) prepared as OER/ORR catalysts.
2 Ultrasonication-assisted plasma engineering used for catalyst synthesis.
3 Co-N4/NC outperformed benchmark commercial catalysts in practical Zn–air battery test.
4 DFT calculations provided insights into the origin of superior ORR/OER performance.

Keywords

Single-atom-doped M-N4/NC catalyst Plasma engineering ORR/OER bifunctional activity DFT calculation Rechargeable Zn–air battery
Chen, Kai, Seonghee Kim, Minyeong Je, Heechae Choi, Zhicong Shi, Nikola Vladimir, Kwang Ho Kim, and Oi Lun Li. 2021. “Ultrasonic Plasma Engineering Toward Facile Synthesis of Single-Atom M-N4/N-Doped Carbon (M = Fe, Co) As Superior Oxygen Electrocatalyst in Rechargeable Zinc–Air Batteries”. Nano-Micro Letters 13 (January):60. https://doi.org/10.1007/s40820-020-00581-4.
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