The dimensionality of MOFs can be modulated post-synthetically via pillar-ligand insertion. This leads to a change in dimensionality from 2D to 3D, resulting in changes to both the electronic structure and the pore structure. Initial work on changing the dimensionality of CuTHQ (THQ = tetrahydroxyquinone) by Park et al. has suggested that pillaring can increase ion accessibility into the pores, resulting in an increased specific capacitance compared to their 2D counterparts (Table ). More work needs to be done with a wider range of 2D MOFs, as well as inherently 3D MOFs, to study the impact of structural augmentation in greater detail.