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Instruments / Technical Area	Publication Details	Published	Actions
I11-High Resolution Powder Diffraction	Enhancing the energy storage performances of metal–organic frameworks by controlling microstructure Jamie W. Gittins , Chloe J. Balhatchet , Simon M. Fairclough , Alexander C. Forse Chemical Science 13, 9210 - 9219 DOI: 10.1039/D2SC03389E Diamond Proposal Number(s): [28349] Open Access Show Abstract ▼ Abstract: Metal–organic frameworks (MOFs) are among the most promising materials for next-generation energy storage systems. However, the impact of particle morphology on the energy storage performances of these frameworks is poorly understood. To address this, here we use coordination modulation to synthesise three samples of the conductive MOF Cu3(HHTP)2 (HHTP = 2,3,6,7,10,11-hexahydroxytriphenylene) with distinct microstructures. Supercapacitors assembled with these samples conclusively demonstrate that sample microstructure and particle morphology have a significant impact on the energy storage performances of MOFs. Samples with ‘flake-like’ particles, with a pore network comprised of many short pores, display superior capacitive performances than samples with either ‘rod-like’ or strongly agglomerated particles. The results of this study provide a target microstructure for conductive MOFs for energy storage applications.	Aug 2022
B18-Core EXAFS	Insights into the electric double-layer capacitance of two-dimensional electrically conductive metal–organic frameworks Jamie W. Gittins , Chloe J. Balhatchet , Yuan Chen , Cheng Liu , David G. Madden , Sylvia Britto , Matthias J. Golomb , Aron Walsh , David Fairen-Jimenez , Sian E. Dutton , Alexander C. Forse Journal Of Materials Chemistry A 6 DOI: 10.1039/D1TA04026J Diamond Proposal Number(s): [14239] Open Access Show Abstract ▼ 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 stable double-layer voltage window of 1 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.	Jun 2021

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