Understanding the Wettability of C1N1 (Sub)Nanopores: Implications for Porous Carbonaceous Electrodes

Abstract Understanding how water interacts with nanopores of carbonaceous electrodes is crucial for energy storage and conversion applications. A high surface area of carbonaceous materials does not necessarily need to translate to a high electrolyte‐solid interface area. Herein, we study the interaction of water with nanoporous C 1 N 1 materials to explain their very low specific capacitance in aqueous electrolytes despite their high surface area. Water was used to probe chemical environments, provided by pores of different sizes, in 1 H MAS NMR experiments. We observe that regardless of their high hydrophilicity, only a negligible portion of water can enter the nanopores of C 1 N 1 , in contrast to a reference pure carbon material with a similar pore structure. The common paradigm that water easily enters hydrophilic pores does not apply to C 1 N 1 nanopores below a few nanometers. Calorimetric and sorption experiments demonstrated strong water adsorption on the C 1 N 1 surface, which restricts water mobility across the interface and impedes its penetration into the nanopores.