In many applications such as vanadium flow batteries, graphite acts as an electrocatalyst and its surface structure therefore determines the efficiency of energy conversion. Due to the heterogeneity of the material, activity descriptors cannot always be evaluated with certainty because the introduction of defects is accompanied by a change in surface chemistry. Moreover, surface defects occur in multiple dimensions, and their occurrence and influence on catalysis must be separated. In this work, we have studied the surface of graphite felt electrodes by different methods in terms of morphology and chemistry to understand the electrocatalytic activity. We then defined the interaction between the surface and the electronic structure with particular emphasis on the work function and valence band. Using model catalysts with different architectures, we established correlations between the electrocatalytic activity and the size of the conjugation and the orientation of the edges. Finally, it was possible to link the level of the work function to the electrocatalytic activity
