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Vol. 14 (2022)

Enabling Multi-Chemisorption Sites on Carbon Nanofibers Cathodes by an In-situ Exfoliation Strategy for High-Performance Zn–Ion Hybrid Capacitors

https://doi.org/10.1007/s40820-022-00839-z
Hongcheng He
Key Laboratory for Micro/Nano Optoelectronic Devices of Ministry of Education, Hunan Provincial Key Laboratory of Low‑Dimensional Structural Physics and Devices, Hunan Joint International Laboratory of Advanced Materials and Technology for Clean Energy, School of Physics and Electronics, College of Semiconductors (College of Integrated Circuits), Hunan University, Changsha 410082, People’s Republic of China
Jichun Lian
Key Laboratory for Micro/Nano Optoelectronic Devices of Ministry of Education, Hunan Provincial Key Laboratory of Low‑Dimensional Structural Physics and Devices, Hunan Joint International Laboratory of Advanced Materials and Technology for Clean Energy, School of Physics and Electronics, College of Semiconductors (College of Integrated Circuits), Hunan University, Changsha 410082, People’s Republic of China
Changmiao Chen
Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, People’s Republic of China
Qiaotian Xiong
Key Laboratory for Micro/Nano Optoelectronic Devices of Ministry of Education, Hunan Provincial Key Laboratory of Low‑Dimensional Structural Physics and Devices, Hunan Joint International Laboratory of Advanced Materials and Technology for Clean Energy, School of Physics and Electronics, College of Semiconductors (College of Integrated Circuits), Hunan University, Changsha 410082, People’s Republic of China
Cheng Chao Li
School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou 510006, People’s Republic of China
Ming Zhang
Key Laboratory for Micro/Nano Optoelectronic Devices of Ministry of Education, Hunan Provincial Key Laboratory of Low‑Dimensional Structural Physics and Devices, Hunan Joint International Laboratory of Advanced Materials and Technology for Clean Energy, School of Physics and Electronics, College of Semiconductors (College of Integrated Circuits), Hunan University, Changsha 410082, People’s Republic of China

Corresponding Author: Ming Zhang

zhangming@hnu.edu.cn

Nano-Micro Letters, Vol. 14 (2022), Article Number: 106

Abstract

Carbon nanofibers films are typical flexible electrode in the field of energy storage, but their application in Zinc-ion hybrid capacitors (ZIHCs) is limited by the low energy density due to the lack of active adsorption sites. In this work, an in-situ exfoliation strategy is reported to modulate the chemisorption sites of carbon nanofibers by high pyridine/pyrrole nitrogen doping and carbonyl functionalization. The experimental results and theoretical calculations indicate that the highly electronegative pyridine/pyrrole nitrogen dopants can not only greatly reduce the binding energy between carbonyl group and Zn2+ by inducing charge delocalization of the carbonyl group, but also promote the adsorption of Zn2+ by bonding with the carbonyl group to form N–Zn–O bond. Benefit from the multiple highly active chemisorption sites generated by the synergy between carbonyl groups and pyridine/pyrrole nitrogen atoms, the resulting carbon nanofibers film cathode displays a high energy density, an ultralong-term lifespan, and excellent capacity reservation under commercial mass loading (14.45 mg cm‒2). Particularly, the cathodes can also operate stably in flexible or quasi-solid devices, indicating its application potential in flexible electronic products. This work established a universal method to solve the bottleneck problem of insufficient active adsorption sites of carbon-based ZIHCs.Imoproved should be changed into Improved.


Highlights:


1 The high pyridine/pyrrole nitrogen-doped and carbonyl-functionalized nanosheets on flexible electrospun porous carbon nanofibers film cathode integrates the advantages of large specific surface area, strong hydrophilicity and high Zn2+ adsorption activity.
2 The Zinc-ion hybrid capacitors exhibits a high capacitance retention of 99.2% over 200,000 cycles at 40 A g−1.
3 A synergistic Zn2+ storage mechanism between carbonyl and pyridine/pyrrole nitrogen atoms is proposed.

Keywords

Nitrogen doping Carbonyl functionalization Chemisorption sites Flexible Zn-ion hybrid capacitors
He, Hongcheng, Jichun Lian, Changmiao Chen, Qiaotian Xiong, Cheng Chao Li, and Ming Zhang. 2022. “Enabling Multi-Chemisorption Sites on Carbon Nanofibers Cathodes by an In-Situ Exfoliation Strategy for High-Performance Zn–Ion Hybrid Capacitors”. Nano-Micro Letters 14 (April):106. https://doi.org/10.1007/s40820-022-00839-z.
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