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
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...
| Main Authors: | , , , , , , , |
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| Format: | Article |
| Language: | English |
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SpringerOpen
2021-01-01
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| Series: | Nano-Micro Letters |
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| Online Access: | https://doi.org/10.1007/s40820-020-00581-4 |
| _version_ | 1818662978866642944 |
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| author | Kai Chen Seonghee Kim Minyeong Je Heechae Choi Zhicong Shi Nikola Vladimir Kwang Ho Kim Oi Lun Li |
| author_facet | Kai Chen Seonghee Kim Minyeong Je Heechae Choi Zhicong Shi Nikola Vladimir Kwang Ho Kim Oi Lun Li |
| author_sort | Kai Chen |
| collection | DOAJ |
| description | 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. |
| first_indexed | 2024-12-17T05:09:33Z |
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| issn | 2311-6706 2150-5551 |
| language | English |
| last_indexed | 2024-12-17T05:09:33Z |
| publishDate | 2021-01-01 |
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| series | Nano-Micro Letters |
| spelling | doaj.art-96d02d64e20f4ca9b21749395a2601ab2022-12-21T22:02:18ZengSpringerOpenNano-Micro Letters2311-67062150-55512021-01-0113112010.1007/s40820-020-00581-4Ultrasonic Plasma Engineering Toward Facile Synthesis of Single-Atom M-N4/N-Doped Carbon (M = Fe, Co) as Superior Oxygen Electrocatalyst in Rechargeable Zinc–Air BatteriesKai Chen0Seonghee Kim1Minyeong Je2Heechae Choi3Zhicong Shi4Nikola Vladimir5Kwang Ho Kim6Oi Lun Li7Department of Materials Science and Engineering, Pusan National UniversityDepartment of Materials Science and Engineering, Pusan National UniversityTheoretical Materials and Chemistry Group, Institute of Inorganic Chemistry, University of CologneTheoretical Materials and Chemistry Group, Institute of Inorganic Chemistry, University of CologneSchool of Materials and Energy, Guangdong University of TechnologyFaculty of Mechanical Engineering and Naval Architecture, University of ZagrebDepartment of Materials Science and Engineering, Pusan National UniversityDepartment of Materials Science and Engineering, Pusan National UniversityAbstract 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.https://doi.org/10.1007/s40820-020-00581-4Single-atom-doped M-N4/NC catalystPlasma engineeringORR/OER bifunctional activityDFT calculationRechargeable Zn–air battery |
| spellingShingle | 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 Nano-Micro Letters Single-atom-doped M-N4/NC catalyst Plasma engineering ORR/OER bifunctional activity DFT calculation Rechargeable Zn–air battery |
| title | 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 |
| title_full | 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 |
| title_fullStr | 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 |
| title_full_unstemmed | 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 |
| title_short | 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 |
| title_sort | 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 |
| topic | Single-atom-doped M-N4/NC catalyst Plasma engineering ORR/OER bifunctional activity DFT calculation Rechargeable Zn–air battery |
| url | https://doi.org/10.1007/s40820-020-00581-4 |
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