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The effect of solvent on the free energy of reaction intermediates adsorbedon electrocatalyst surfaces can significantly change the thermochemicaloverpotential, but accurate calculations of this are challenging. Here, wepresent computational estimates of the solvation energy for reactionintermediates in oxygen reduction reaction (ORR) on a B-doped graphene (BG)model system where the overpotential is found to reduce by up to 0.6 V due tosolvation. BG is experimentally reported to be an active ORR catalyst butrecent computational estimates using state-of-the-art hybrid densityfunctionals in the absence of solvation effects have indicated low activity. Totest whether the inclusion of explicit solvation can bring the calculatedactivity estimates closer to the experimental reports, up to 4 layers of watermolecules are included in the simulations reported here. The calculations arebased on classical molecular dynamics and local minimization of energy usingatomic forces evaluated from electron density functional theory. Data sets areobtained from regular and coarse-grained dynamics, as well as localminimization of structures resampled from dynamics simulations. The resultsdiffer greatly depending on the method used and the solvation energy estimatesand are deemed untrustworthy. It is concluded that a significantly largernumber of water molecules is required to obtain converged results for thesolvation energy. As the present system includes up to 139 atoms, it alreadystrains the limits of computational feasibility, so this points to the need fora hybrid simulation approach where efficient simulations of much larger numberof solvent molecules is carried out using a lower level of theory whileretaining the higher level of theory for the reacting molecules as well astheir near neighbors and the catalyst.

On the challenge of obtaining an accurate solvation energy estimate in simulations of electrocatalysis