The highly oriented and conducting inorganic crystalline polymer, polymeric sulfur nitride, has been employed as an electrode material. Due to its chemical and electrical anisotropy, the electrode behavior of both crystal planes can be studied independently. The effects of variation of acid strength, as well as the nature of a variety of supporting electrolytes on the background currents and breakdown potentials in aqueous media, show that the metal cation and not the anion interacts strongly with the (SN) x surfaces. Thus, this material could possibly be employed in model systems to study the electrical interactions and electron transfer processes which occur with bound metal cations at membrane surfaces. It was also found that (SN) x electrode surfaces which are modified (or derivatized) by the interaction with certain cations exhibit significant electrocatalysis with respect to other redox processes.