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

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Nano-Micro Letters 2022年第7期14卷 1-15页

作者： Hongcheng He Jichun Lian Changmiao Chen Qiaotian Xiong Cheng Chao Li Ming Zhang Key Laboratory for Micro/Nano Optoelectronic Devices of Ministry of Education Hunan Provincial Key Laboratory of Low-Dimensional Structural Physics and DevicesHunan Joint International Laboratory of Advanced Materials and Technology for Clean EnergySchool of Physics and ElectronicsCollege of Semiconductors(College of Integrated Circuits)Hunan UniversityChangsha 410082People’s Republic of China Tsinghua Shenzhen International Graduate School Tsinghua UniversityShenzhen 518055People’s Republic of China School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhou 510006People’s Republic of China

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 Z n2+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.

关键词： Nitrogen doping Carbonyl functionalization chemisorption sites Flexible Zn-ion hybrid capacitors

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