An electrochemical study of frustrated lewis pairs: A metal-free route to hydrogen oxidation

Article abstract of DOI:10.1021/ja500477g

Frustrated Lewis pairs have found many applications in the heterolytic activation of H₂ and subsequent hydrogenation of small molecules through delivery of the resulting proton and hydride equivalents. Herein, we describe how H₂ can be preactivated using classical frustrated Lewis pair chemistry and combined with in situ nonaqueous electrochemical oxidation of the resulting borohydride. Our approach allows hydrogen to be cleanly converted into two protons and two electrons in situ, and reduces the potential (the required energetic driving force) for nonaqueous H₂ oxidation by 610 mV (117.7 kJ mol^-1). This significant energy reduction opens routes to the development of nonaqueous hydrogen energy technology.