Selective Catalytic Frustrated Lewis Pair Hydrogenation of CO2 in the Presence of Silylhalides

The frustrated Lewis pair (FLP) derived from 2,6-lutidine and B(C6F5)(3) is shown to mediate the catalytic hydrogenation of CO2 using H-2 as the reductant and a silylhalide as an oxophile. The nature of the products can be controlled with the judicious selection of the silylhalide and the solvent. In this fashion, this metal-free catalysis affords avenues to the selective formation of the disilylacetal (R3SiOCH2OSiR3), methoxysilane (R3SiOCH3), methyliodide (CH3I) and methane (CH4) under mild conditions. DFT studies illuminate the complexities of the mechanism and account for the observed selectivity.

Automated summary

The frustrated Lewis pair (FLP) derived from 2,6-lutidine and B(C6F5)(3) has been shown to mediate the catalytic hydrogenation of CO2, with control over product nature through careful selection of silylhalide and solvent. This metal-free catalysis offers pathways to selectively form specific compounds under mild conditions, as elucidated by DFT studies on the mechanism and selectivity.