Novel inorganic hydride compounds KHKHCHO3 and KH were isolated and characterized following the highly exothermic electrolysis of a K2CO3 electrolyte, and the hydride was shown to comprise hydrino hydride ions [R. Mills, E. Dayalan, P. Ray, B. Dhandapani J. He, Electrochim. Acta 47 (2002) 3909; R. Mills. Int. J. Hydrogen Energy 25 (2000) 669; R. Mills, J. New Mater. Electrochem. Syst. 6 (2003) 45; R. Mills, Fusion Technology, vol. 37, no. 2, March, 2000, p. 157.]. We report further evidence of the catalysis of hydrogen to form molecular hydrino with potassium catalyst in a K2CO3 electrolytic cell. Excess enthalpy of a factor of 40% that of the ohmic power dissipation was observed. H-2(1/4), molecular hydrogen in a fractional Rydberg state, was predicted as a further product. From the NMR frequency, the energy state of the molecular hydrogen can be measured. The electrolysis gas was collected in a hollow nickel cathode that permitted enrichment of H-2(1/4) based on its higher mobility. The gases were dissolved in CDCl3 and characterized by H-1 NMR. A singlet peak upfield of H-2 was observed with the predicted chemical shift of 1.25 ppm relative to tetramethylsilane (TMS). The H-2(1/4) NMR peak was further observed on samples prepared by dissolving each of the crystals that precipitated from the electrolyte and concentrated electrolyte in CDCl3. (C) 2009 Elsevier Ltd. All rights reserved.