The past decade has seen the emergence of a new concept in main-group chemistry: ‘frustrated Lewis pairs’ (FLPs) are combinations of a Lewis acid (LA) and base (LB) that are prevented from forming the classically-expected adduct. By displaying simultaneously acidic and basic behaviour, these systems have been shown to be capable of activating a wide range of chemical bonds, in a manner highly reminiscent of transition-metal (TM) compounds. Chief among these reactions is the activation of H2, which can then be transferred from the FLP to an appropriate substrate. FLPs have thus provided an entirely new class of homogeneous hydrogenation catalysts, which do not require the use of TMs. Nevertheless, prior to the work described herein, such catalysis had not been successfully applied to the hydrogenation of organic carbonyl functional groups, and had been found to be extremely sensitive to the presence of moisture. This thesis describes work that has successfully overcome these limitations.