Modern cutting-edge energy storage and conversion devices based on aqueous electrolytes are a promising technologies to support electrical grids based on renewable energies. In such devices, carbon-based materials are the material of choice to build electrodes because i) it is easy to introduce other elements (heteroatoms) into the carbon network; ii) they can be engineered to possess porous structures comprising nano-sized pores of varying dimensions; iii) their synthesis is sustainable, based in few-steps and using biobased precursors. Changing carbon nanopore structures and tunning carbon surface chemistry is a well-equipped toolbox that allows preparing “designer” carbons. Depending on these parameters, the carbon properties such as surface electron density and morphology change, and this deeply affects the way they interact with water-based-electrolytes. Pure carbon materials (for example, graphite or active carbons) are typically considered hydrophobic, while, according to vapor sorption isotherms or contact angle experiments, doped carbon surfaces with more polar heteroatoms such as nitrogen or oxygen tend to be hydrophilic. However, extrapolating the “wettability” of carbon surfaces to carbon nanostructures is not trivial: nanopores introduce confinement effects and heteroatom doping deeply disrupts carbons´ electron density, favoring H-bond formation, which may lead to misinterpretations of electrochemical performance. Understanding how water interacts with nanopores of carbonaceous materials is crucial for green energy storage and conversion applications as carbon–electrolyte (carbon-water) interfaces have a dominant influence on their electrochemical performance. 

NMR spectroscopy is a versatile tool to probe the local environments of water in pores as, when water enters such pores a clear signal up-field shift is observed due to the proximity of the water molecules to the ring currents of the carbon materials. Preliminary solid-state nuclear magnetic resonance (ssNMR) results indicate that while bare carbon nanopores easily fill up with water, this might not the case with highly nitrogen-doped carbons. Despite this effect being extensively studied in bare carbon materials, highly doped ones are not well understood. We work on bridging the gap on the basic understanding of these interactions.