Electrochemical quartz crystal microbalance (EQCM) experiments were used to experimentally study the same MOF-electrolyte system employed in the QM/MM study above, Cu3(HHTP)2 with 1 M NEt4BF4/ACN, and supported the cation dominated nature of the charging mechanism. More widely, He et al. performed in-situ small-angle neutron scattering (SANS) experiments, on Ni3(HITP)2 cells with an organic electrolyte of sodium triflate in dimethylformamide (DMF). The charging mechanism was found to be dependent on the electrode polarisation and the MOF was proposed to be ionophobic with respect to this electrolyte, with the pores devoid of electrolyte ions in the absence of an applied potential, a scenario which has been predicted to lead to improved performance in nanoporous carbon supercapacitors. However, both SANS and EQCM rely on data fitting to separate electrolyte cation, anion and solvent contributions, meaning it is challenging to quantify the charging mechanisms with these techniques. There is an urgent need for new model-free techniques which can directly study the independent interactions of cations and anions at the MOF interface and how this connects with the charging mechanism and performance.