Covalent Graphene‐MOF Hybrids for High‐Performance Asymmetric Supercapacitors

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 report...

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Bibliographic Details
Published in:Advanced materials (Weinheim) Vol. 33; no. 4; pp. e2004560 - n/a
Main Authors: Jayaramulu, Kolleboyina, Horn, Michael, Schneemann, Andreas, Saini, Haneesh, Bakandritsos, Aristides, Ranc, Vaclav, Petr, Martin, Stavila, Vitalie, Narayana, Chandrabhas, Scheibe, Błażej, Kment, Štěpán, Otyepka, Michal, Motta, Nunzio, Dubal, Deepak, Zbořil, Radek, Fischer, Roland A.
Format: Journal Article
Language:English
Published: Germany Wiley Subscription Services, Inc 01.01.2021
Wiley
John Wiley and Sons Inc
Subjects:
2D materials
Amides
Asymmetric supercapacitor
asymmetric supercapacitors
Asymmetry
Capacitance
Carboxylation
Charge materials
Charge transfer
Communication
Communications
Conductive networks
Conjugated structures
covalent assemblies
Covalent attachment
Electrochemical characterizations
Electrodes
Flux density
Functionalized graphene
Graphene
Hybrid materials
Large specific surface areas
MATERIALS SCIENCE
metal-organic frameworks
MXenes
Organic polymers
Organometallics
Positive electrodes
Supercapacitor
Supercapacitors
covalent assemblies
asymmetric supercapacitors
MXenes
2D materials
metal-organic frameworks
ISSN:0935-9648, 1521-4095, 1521-4095
Online Access:Get full text
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Summary: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 π‐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. A facile method for the preparation of graphene/metal–organic framework (MOF) hybrids with an amine‐functionalized MOF and carboxylate‐functionalized graphene via amide bonds for capacitance applications is demonstrated.
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Indian Inst. of Technology
Australian Research Council (ARC)
Queensland Univ. of Technology
German Research Foundation (DFG)
SAND-2020-14361J
European Research Council (ERC)
AC04-94AL85000; NA-0003525; SGT‐100038; 323000‐0424/07; FT180100058; CZ.02.1.01/0.0/0.0/16_019/0000754; CZ.02.1.01/0.0/0.0/15_003/0000416; 19-27454X; 683024; EXC 2089
Czech Science Foundation
USDOE National Nuclear Security Administration (NNSA)
European Regional Development Fund
ISSN:0935-9648
1521-4095
1521-4095
DOI:10.1002/adma.202004560