An Electrochemical Study of Frustrated Lewis Pairs:\nA Metal-Free Route to Hydrogen Oxidation

Abstract

Frustrated\nLewis pairs have found many applications in the heterolytic\nactivation of H₂ and subsequent hydrogenation of small\nmolecules through delivery of the resulting proton and hydride equivalents.\nHerein, we describe how H₂ can be preactivated using classical\nfrustrated Lewis pair chemistry and combined with in situ nonaqueous\nelectrochemical oxidation of the resulting borohydride. Our approach\nallows hydrogen to be cleanly converted into two protons and two electrons\nin situ, and reduces the potential (the required energetic driving\nforce) for nonaqueous H₂ oxidation by 610 mV (117.7 kJ\nmol^–1). This significant energy reduction opens\nroutes to the development of nonaqueous hydrogen energy technology.