To demonstrate the capability of PiNet2-χ, PiNet2-dipole and PiNNwall for realistic appli-cations, we showcase here the molecular simulations of electrified graphene oxide/electrolyte interfaces. In graphene oxide, both surface carboxylic and hydroxyl groups can undergo protonation/deprotonation depending on the solution pH. It has been reported that the pK a is about 6.6 for the carboxylic group and 9.8 for the hydroxyl group in graphene oxide. Therefore, graphene oxide is negatively charged at neutral pH through the acid-base reaction shown in Fig. and this property contributes to the stability of graphene-oxide membranes in aqueous solutions. 79 Before turning on the MD engine for simulating the electrode-electrolyte system, we have checked the predictions from PiNet2-χ regarding the response charge for the case where the analytical solution is available. This is the case of a graphite electrode in vacuum. We used this system to compute the corresponding capacitance by varying the thickness of the vacuum slab. When the electrode behaves like a perfect metal with a dielectric constant of infinity, the total capacitance of the whole system (electrode slab + vacuum) will only depend on the thickness of the vacuum. The results of different models implemented in PiNet2-χ are shown in Fig. . It is clear that the EEM-type model reproduces the expected theoretical behavior of a perfect metallic electrode, which is not the case for the ACKS2-type, the Local-type and the EtaInv-type models. Therefore, we have selected the EEM-type model as the charge response kernel for the application here.