Covalent Graphene-MOF Hybrids for High-Performance Asymmetric Supercapacitors
Abstract
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.
- Authors:
-
[1];
[3];
[10]
- Indian Inst. of Technology (ITT) Jammu (India); Palacky Univ., Olomouc (Czech Republic); Technical Univ. of Munich (Germany)
- Univ. of Queensland, Brisbane, QLD (Australia)
- Dresden Univ. of Technology (Germany)
- Indian Inst. of Technology (ITT) Jammu (India)
- Palacky Univ., Olomouc (Czech Republic); Technical Univ. of Ostrava (Czech Republic)
- Palacky Univ., Olomouc (Czech Republic)
- Sandia National Lab. (SNL-CA), Livermore, CA (United States)
- Jawaharlal Nehru Centre for Advanced Scientific Research (JNCASR), Bangalore (India)
- Palacky Univ., Olomouc (Czech Republic); Adam Mickiewicz Univ., Poznan (Poland)
- Technical Univ. of Munich (Germany)
- Publication Date:
- Research Org.:
- Sandia National Lab. (SNL-CA), Livermore, CA (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA); Indian Inst. of Technology; Queensland Univ. of Technology; Australian Research Council (ARC); European Regional Development Fund; Czech Science Foundation; European Research Council (ERC); German Research Foundation (DFG)
- OSTI Identifier:
- 1760442
- Report Number(s):
- SAND-2020-14361J
Journal ID: ISSN 0935-9648; 693152
- Grant/Contract Number:
- 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
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Materials
- Additional Journal Information:
- Journal Volume: 33; Journal Issue: 4; Journal ID: ISSN 0935-9648
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 2D materials; asymmetric supercapacitors; covalent assemblies; metal‐organic frameworks; MXenes
Citation Formats
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, and Fischer, Roland A. Covalent Graphene-MOF Hybrids for High-Performance Asymmetric Supercapacitors. United States: N. p., 2020.
Web. doi:10.1002/adma.202004560.
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. Covalent Graphene-MOF Hybrids for High-Performance Asymmetric Supercapacitors. United States. https://doi.org/10.1002/adma.202004560
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, and Fischer, Roland A. Fri .
"Covalent Graphene-MOF Hybrids for High-Performance Asymmetric Supercapacitors". United States. https://doi.org/10.1002/adma.202004560. https://www.osti.gov/servlets/purl/1760442.
@article{osti_1760442,
title = {Covalent Graphene-MOF Hybrids for High-Performance Asymmetric Supercapacitors},
author = {Jayaramulu, Kolleboyina and Horn, Michael and Schneemann, Andreas and Saini, Haneesh and Bakandritsos, Aristides and Ranc, Vaclav and Petr, Martin and Stavila, Vitalie and Narayana, Chandrabhas and Scheibe, Błażej and Kment, Štěpán and Otyepka, Michal and Motta, Nunzio and Dubal, Deepak and Zbořil, Radek and Fischer, Roland A.},
abstractNote = {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.},
doi = {10.1002/adma.202004560},
journal = {Advanced Materials},
number = 4,
volume = 33,
place = {United States},
year = {Fri Dec 04 00:00:00 EST 2020},
month = {Fri Dec 04 00:00:00 EST 2020}
}
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