Covalent Graphene-MOF Hybrids for High-Performance Asymmetric Supercapacitors

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.

doi:10.1002/adma.202004560

Title: Covalent Graphene-MOF Hybrids for High-Performance Asymmetric Supercapacitors

Journal Article · Fri Dec 04 00:00:00 EST 2020 · Advanced Materials

DOI:https://doi.org/10.1002/adma.202004560· OSTI ID:1760442

^[1]; Horn, Michael ^[2];

^[3]; Saini, Haneesh ^[4]; Bakandritsos, Aristides ^[5]; Ranc, Vaclav ^[6]; Petr, Martin ^[6]; Stavila, Vitalie ^[7]; Narayana, Chandrabhas ^[8]; Scheibe, Błażej ^[9]; Kment, Štěpán ^[5]; Otyepka, Michal ^[6]; Motta, Nunzio ^[2]; Dubal, Deepak ^[2]; Zbořil, Radek ^[5];

^[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)

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 Ti₃C₂T_X 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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Research Organization:: Sandia National Lab. (SNL-CA), Livermore, CA (United States)

Sponsoring Organization:: 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)

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

OSTI ID:: 1760442

Report Number(s):: SAND-2020-14361J; 693152

Journal Information:: Advanced Materials, Vol. 33, Issue 4; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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