期刊
ADVANCED MATERIALS
卷 33, 期 4, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202004560
关键词
2D materials; asymmetric supercapacitors; covalent assemblies; metal-organic frameworks; MXenes
类别
资金
- Indian Institute of Technology Jammu [SGT100038]
- SERB [SRG/2020/000865]
- Queensland University of Technology [323000-0424/07]
- Australian Research Council (ARC) [FT180100058]
- Operational Programme Research, Development and Education-European Regional Development Fund of the Ministry of Education, Youth and Sports of the Czech Republic [CZ.02.1.01/0.0/0.0/16_019/0000754, CZ.02.1.01/0.0/0.0/15_003/0000416]
- Czech Science Foundation [19-27454X]
- ERC from the EU Horizon 2020 Research and Innovation Programme [683024]
- IIT Jammu
- Fonds der Chemischen Industrie
- U.S. Department of Energy's National Nuclear Security Administration (NNSA) [DE-NA-0003525]
- German Research Foundation (DFG) [EXC 2089]
- Projekt DEAL
- Australian Research Council [FT180100058] Funding Source: Australian Research Council
The study demonstrates the covalent attachment of an amine functionalized metal-organic framework to carboxylate functionalized graphene, resulting in a hybrid material with high capacitance and cycling stability. An asymmetric supercapacitor was successfully constructed using this hybrid material, showing comparable performance to commercial devices such as Pb-acid and Ni/MH batteries. The amide linkage plays a key role in forming a p-conjugated structure, facilitating charge transfer and enhancing capacitance and cycling stability.
In this work, the covalent attachment of an amine functionalized metal-organic framework (UiO-66-NH2 = Zr6O4(OH)(4)(bdc-NH2)(6); bdc-NH2 = 2-amino-1,4-benzenedicarboxylate) (UiO-Universitetet i Oslo) to the basal-plane of carboxylate functionalized graphene (graphene acid = GA) via amide bonds is reported. The resultant GA@UiO-66-NH2 hybrid displayed a large specific surface area, hierarchical pores and an interconnected conductive network. The electrochemical characterizations demonstrated that the hybrid GA@UiO-66-NH2 acts as an effective charge storing material with a capacitance of up to 651 F g(-1), significantly higher than traditional graphene-based materials. The results suggest that the amide linkage plays a key role in the formation of a p-conjugated structure, which facilitates charge transfer and consequently offers good capacitance and cycling stability. Furthermore, to realize the practical feasibility, an asymmetric supercapacitor using a GA@UiO-66-NH2 positive electrode with Ti3C2TX MXene as the opposing electrode has been constructed. The cell is able to deliver a power density of up to 16 kW kg(-1) and an energy density of up to 73 Wh kg(-1), which are comparable to several commercial devices such as Pb-acid and Ni/MH batteries. Under an intermediate level of loading, the device retained 88% of its initial capacitance after 10 000 cycles.
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