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Coulometric measurements on salt-water-immersed nanoporous carbon electrodesreveal, at a fixed voltage, a charge decrease with increasing temperature.During far-out-of-equilibrium charging of these electrodes, calorimetryindicates the production of both irreversible Joule heat and reversible heat,the latter being associated with entropy changes during electric double layer(EDL) formation in the nanopores. These measurements grant experimental access--for the first time-- to the entropic contribution of the grand potential; forour electrodes, this amounts to roughly 25% of the total grand potential energycost of EDL formation at large applied potentials, in contrast withpoint-charge model calculations that predict 100%. The coulometric andcalorimetric experiments show a consistent picture of the role of heat andtemperature in EDL formation and provide hitherto unused information to testagainst EDL models.

Coulometry and Calorimetry of Electric Double Layer Formation in Porous Electrodes