Facile Reversibility by Design: Tuning Small Molecule Capture and Activation by Single Component Frustrated Lewis Pairs

A series of single component FLPs has been investigated for small molecule capture, with the finding that through tuning of both the thermodynamics of binding/activation and the degree of preorganization (i.e., ΔS⧧) reversibility can be brought about at (or close to) room temperature. Thus, the dimethylxanthene system {(C6H4)2(O)­CMe2}­(PMes2)­(B­(C6F5)2): (i) heterolytically cleaves dihydrogen to give an equilibrium mixture of FLP and H2 activation product in solution at room temperature and (ii) reversibly captures nitrous oxide (uptake at room temperature, 1 atm; release at 323 K).