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
Kai Chen Seonghee Kim Minyeong Je Heechae Choi Zhicong Shi Nikola Vladimir Kwang Ho Kim Oi Lun Li
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
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
摘要
Abstract
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.关键词
Single-atom-doped M-N4/NC catalyst/Plasma engineering/ORR/OER bifunctional activity/DFT calculation/Rechargeable Zn–air batteryKey words
Single-atom-doped M-N4/NC catalyst/Plasma engineering/ORR/OER bifunctional activity/DFT calculation/Rechargeable Zn–air battery引用本文复制引用
Kai Chen,Seonghee Kim,Minyeong Je,Heechae Choi,Zhicong Shi,Nikola Vladimir,Kwang Ho Kim,Oi Lun Li..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[J].纳微快报（英文）,2021,13(4):76-95,20.基金项目
This research was mainly supported by Global Frontier Program through the Global Frontier Hybrid Interface materials (GFHIM) of the National Research Foundation of Korea (NRF) funded by the ministry of science, ICT and Future Planning (2013M3A6B1078874), and co-supported by Busan Innovation Institute of Industry, Science & Technology Planning (BISTEP). MJ and HC acknowledge the financial support of Federal Ministry of Education and Research (BMBF) under the "Make Our Planet Great Again - German Research Initiative" (MOPGAGRI),57429784, implemented by the German Academic Exchange Service Deutscher Akademischer Austauschdienst (DAAD). Also,the authors want to thank Dr. Juchul Park for his valuable advice in HR-TEM. （GFHIM）
