For a detailed study of the ion-water interaction the reader is referred to Ref. This underestimation occurs over several empirical water models, the main reason being too stiff hydrogen bonding interactions, and has been discussed in detail in our recent work. In Fig. (a), the potential-dependent evolution of the entropy from the adsorbed water layer into the bulk water is depicted. For the double layer potential region in general and exemplary at E = 0.37 V, the reduced entropy of S H 2 O * , 0.37 V = 29.57 J/molK (compared to the bulk water entropy of S H 2 O, bulk = 59.27 J/molK) suggests a higher ordering in the H 2 O * adsorbate layer.