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

• 作者: Kai Chen Seonghee Kim Minyeong Je Heechae Choi Zhicong Shi Nikola Vladimir Kwang Ho Kim Oi Lun Li
• 来源期刊: 纳微快报（英文）
• 年，卷（期）: 2021,（4）
• 页码范围: 76-95
• 页数: 20页
• 语种: 英文

摘要

As bifunctional oxygen evolution/reduction electro-catalysts, 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 utili-zation 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, ultra-sonic plasma engineering allows direct carbonization in a precursor solution containing metal phthalocyanine and aniline. When combin-ing 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 pre-sented 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. Moreo-ver, 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.