PNNL

Abstract

We report the hydrogenation of CO2 to MeOH by a new Ru(triphos) catalyst containing a cationic tetraalkylammonium moiety in the outer coordination sphere. This new catalyst affords superior TON and TOF values for MeOH in comparison to previously reported isostructural catalysts. Kinetic data from operando NMR spectroscopy studies indicate the improvement in MeOH production arises from a 15-fold enhancement in the rate for hydrogenation of the transient formaldehyde intermediate. These results provide insight into the catalyst characteristics that promote methanol formation. This research was supported by the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences. Mass spectrometry experiments were performed in the William R. Wiley Environmental Molecular Sciences Laboratory, a DOE national scientific user facility sponsored by the DOE’s Office of Biological and Environmental Research and located at the Pacific Northwest National Laboratory (PNNL). The authors thank Dr. William Kew for mass spectrometry analysis. PNNL is operated by Battelle for DOE.