The catalytic dehydrogenative coupling of silanes and alcohols represents a convenient process to produce hydrogen on demand. The catalyst, an iridium complex of the formula [IrCp*(Cl)2(NHC)] containing an N-heterocyclic carbene (NHC) ligand functionalized with a pyrene tag, catalyzes efficiently the reaction at room temperature producing H2 quantitatively within a few minutes. As a result, the dehydrogenative coupling of 1,4-disilabutane and methanol enables an effective hydrogen storage capacity of 4.3 wt % that is as high as the hydrogen contained in the dehydrogenation of formic acid, positioning the silane/alcohol pair as a potential liquid organic hydrogen carrier for energy storage. In addition, the heterogenization of the iridium complex on graphene presents a recyclable catalyst that retains its activity for at least 10 additional runs. The homogeneous distribution of catalytic active sites on the basal plane of graphene prevents diffusion problems, and the reaction kinetics are maintained after immobilization.

The authors are thankful for the financial support from MINECO (CTQ2015-69153-C2-2-R and CTQ2015-67461-P), Diputacion General de Aragon (Grupo Consolidado E21) and Universitat Jaume I (P1.1B2015-09). D.V.-E. thanks the MINECO for the FPU grant (FPU15/03011).

Peer reviewed