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Insights into the electric double-layer capacitance of two-dimensional electrically conductive metal-organic frameworks

Authors: Alexander C. Forse; Siân E. Dutton; Aron Walsh; Sylvia Britto; David Fairen-Jimenez; Yuan Chen; Yuan Chen; +5 Authors

Insights into the electric double-layer capacitance of two-dimensional electrically conductive metal-organic frameworks

Abstract

Two-dimensional electrically conductive metal-organic frameworks (MOFs) have emerged as promising model electrodes for use in electric double-layer capacitors (EDLCs). However, a number of fundamental questions about the behaviour of this class of materials in EDLCs remain unanswered, including the effect of the identity of the metal node and organic linker molecule on capacitive performance and the limitations of current conductive MOFs in these devices relative to traditional activated carbon electrode materials. Herein, we address both these questions via a detailed study of the capacitive performance of the framework Cu3(HHTP)2 (HHTP = 2,3,6,7,10,11-hexahydroxytriphenylene) with an acetonitrile-based electrolyte, finding a specific capacitance of 110 – 114 F g−1 at current densities of 0.04 – 0.05 A g−1 and a modest rate capability. By, directly comparing its performance with the previously reported analogue, Ni3(HITP)2 (HITP = 2,3,6,7,10,11-hexaiminotriphenylene), we illustrate that capacitive performance is largely independent of the identity of the metal node and organic linker molecule in these nearly isostructural MOFs. Importantly, this result suggests that EDLC performance in general is uniquely defined by the 3D structure of the electrodes and the electrolyte, a significant finding not demonstrated using traditional electrode materials. Finally, we probe the limitations of Cu3(HHTP)2 in EDLCs, finding a limited cell voltage window of 1.3 V and only a modest capacitance retention of 81 % over 30,000 cycles, both significantly lower than state-of-the-art porous carbons. These important insights will aid the design of future conductive MOFs with greater EDLC performances.

Country
United Kingdom
Keywords

34 Chemical Sciences, 290, metal-organic frameworks (MOFs), EDLC performance, Energy Storage, 4016 Materials Engineering, Chemistry, structure-property relationships, Electrochemistry - Organometallic, EDLC devices, 7 Affordable and Clean Energy, energy storage capabilities, 40 Engineering

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    This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network.
    Top 10%
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citations
This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Citations provided by BIP!
popularity
This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network.
BIP!Popularity provided by BIP!
influence
This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Influence provided by BIP!
impulse
This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network.
BIP!Impulse provided by BIP!
38
Top 10%
Top 10%
Top 1%
Green
hybrid