The well-defined structures of 2D MOFs allow for the systematic inclusion of specific functional groups that is challenging in porous carbons, where a distribution of functional groups is normally present. Many such functionalised linkers have been synthesised in recent years, and employing these materials as supercapacitor electrodes may unveil detailed structure-performance relationships to correlate specific functional groups with supercapacitor performance, leading to general design principles for carbon-based supercapacitors. Furthermore, inclusion of specific functional groups will change electrolyte-MOF interactions in devices, modifying the double-layer structure and potentially yielding further improvements to the performances of MOF-based devices. Modifying MOFelectrolyte interactions in existing systems by changing the electrolyte is also a promising avenue for exploration, as shown by recent work from Dincâ et al., who demonstrated that Li-ion electrolytes result in significant increases in the specific capacitance of non-porous Ni3(BHT)2-based supercapacitors (Table ). The impact of the electrolyte on the performance of MOF-based supercapacitors has been further highlighted in work from Forse et al., who showed that Cu3(HHTP)2 displays dramatically lower capacitances and rate capabilities with an ionic liquid electrolyte (EMIM-BF4) compared to an organic electrolyte (1 M NEt4BF4 in acetonitrile). This drop in performance was more significant than that seen for porous carbons with the same electrolytes. This is further evidence for the poor movement of ions through the ordered pores of 2D MOFs, and is supported by results with Ni3(HITP)2. This shows that it is important to use electrolytes with high ionic conductivities in 2D MOFbased supercapacitors.