Interestingly, the cation dominated nature of this charging mechanism is consistent with EQCM studies on the related MOF Cu3(HHTP)2 with 1 M NEt4BF4/ACN electrolyte. The greater contribution of the cations compared to anions in charge storage of these systems suggests that the cation identity may be most closely linked to the overall electrochemical performance. Gittins et al. previously demonstrated the impact of increasing the alkyl chain length in this family of cations, but further exploration of electrolytes is needed to improve electrochemical performance beyond that for 1 M NEt4BF4/ACN electrolyte. Conversely, this work may suggest that the cations are only the dominant contribution to charge storage in this system due to relatively strong BF4 -anion-MOF interactions. If the relative strengths of the interactions between the anions and the cations with the MOF could be systematically modified, this could be exploited to control the extents to which each ion contributes to charge storage. Controlling the charging mechanism in this way would likely also give rise to higher capacitive performance.