After 10(4) h of continuous aqueous electrolysis with K2CO3 as the electrolyte, highly stable novel inorganic hydride compounds such as KH KHCO3 and KH were isolated and identified by time of flight secondary ion mass spectroscopy (ToF-SIMS). The existence of novel hydride ions was determined using X-ray photoelectron spectroscopy (XPS) and solid state magic-angle spinning proton nuclear magnetic resonance spectroscopy (H-1 MAS NMR). A novel hydride ion formed by plasma electrolysis of a K2CO3, Rb2CO3, or Cs2CO3 electrolyte was also observed by high resolution visible spectroscopy at 407.0 nm corresponding to its predicted binding energy of 3.05 eV.