Metal nitrosyl compounds are involved in cell signaling via binding of NO to an iron atom resulting in a bent Fe-NO geometry. Notable examples of binding sites include iron hemes. Understanding the redox chemistry is made possible by the attachment of ligands which mimic biological heme sites and is critical for the fields of medicine and bio-inorganic chemistry. Starting with the synthesis of a Ru-model complex for the heme-NO site, Ru(NO)(N₃)(t-Bu₄-saloph) (t-Bu₄saloph = [N,N-Bis(3,5-di-tert-butylsalicylidene)-1,2-diaminobenzene]), we are exploring binding to electrode surfaces through “click” chemistry. The redox chemistry is explored with the aim to compare with the consequences of histidine binding in heme-NO species. Various methodologies towards the introduction of a metal nitrosyl complex to the surface of metal electrodes are investigated. Synthesis of the ruthenium nitrosyl H₂(t-Bu₄saloph) compounds is discussed. The surface-enhanced Raman spectro-electrochemical analysis of the electrode-bound compounds are described.