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Insights Into the Electric Double-Layer Capacitance of the Two-Dimensional Electrically Conductive Metal-Organic Framework Cu3(HHTP)2

preprint
submitted on 31.03.2021, 14:06 and posted on 01.04.2021, 12:39 by Jamie W. Gittins, Chloe J. Balhatchet, Yuan Chen, Cheng Liu, David G. Madden, Sylvia Britto, Matthias Golomb, Aron Walsh, David Fairen-Jimenez, Sian Dutton, Alexander C. Forse
Two-dimensional electrically conductive metal-organic frameworks (MOFs) are candidate electrode materials for use in electric double-layer capacitor (EDLC) structure-property investigations due to their well-defined crystalline structures. Their promising capacitive performance was first illustrated by EDLCs constructed with the layered framework Ni3(HITP)2 (HITP = 2,3,6,7,10,11-hexaiminotriphenylene) and an organic electrolyte. Despite this promise, there have been few follow-up studies on the use of these frameworks in EDLCs, raising questions about the generality of the results. Here, we demonstrate the high capacitive performance of the layered framework Cu3(HHTP)2 (HHTP = 2,3,6,7,10,11-hexahydroxytriphenylene) in EDLCs with an organic electrolyte and compare its performance with Ni3(HITP)2. Cu3(HHTP)2 exhibits a specific capacitance of 110 – 114 F g–1 at low current densities of 0.04 – 0.05 A g–1 and shows modest capacitance retentions (66 %) at current densities up to 2 A g–1, mirroring the performance of Ni3(HITP)2. However, we also explore the limitations of Cu3(HHTP)2 in EDLCs, finding a limited cell voltage window of 1.3 V and only moderate capacitance retention over 30,000 cycles. This illustrates that these materials require further development to improve their EDLC performance, particularly to reach similar cycling performance levels as porous carbons. Despite this, our work underscores the utility of framework materials in EDLCs and suggests that capacitive performance is largely independent of the identity of the metal node and organic linker molecule, instead being dictated by the three-dimensional structure of the framework. These important insights will aid the design of future conductive MOFs for use in EDLCs.

Funding

UKRI Future Leaders Fellowship (MR/T043024/1)

Faraday Undergraduate Summer Experience (FIRG017)

BP Next Generation Fellowship

Design of NanoMOFs Capsules for Drug Delivery and Bioimaging.

European Research Council

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Development and commercialisation of a flexible manufacturing process to produce monolithic metal-organic framework (MOF) materials.

Innovate UK

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Isaac Newton Trust Research Grant

Royal Society University Research Fellowship (UF100278)

The Materials and Molecular Modelling Hub

Engineering and Physical Sciences Research Council

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Tier 2 Hub in Materials and Molecular Modelling

Engineering and Physical Sciences Research Council

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Royal Society of Chemistry (PhD Funding)

School of the Physical Sciences, Cambridge (Oppenheimer Studentship)

Winton Programme for the Physics of Sustainability

History

Email Address of Submitting Author

jwg37@cam.ac.uk

Institution

University of Cambridge, Yusuf Hamied Department of Chemistry

Country

United Kingdom

ORCID For Submitting Author

0000-0002-9106-8910

Declaration of Conflict of Interest

No conflict of interest.

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