4.8 Article

Enhanced Hydrogenation of Carbon Dioxide to Methanol by a Ruthenium Complex with a Charged Outer-Coordination Sphere

Journal

ACS CATALYSIS
Volume 10, Issue 13, Pages 7419-7423

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c02268

Keywords

carbon dioxide; methanol; hydrogenation; homogeneous catalysis; ruthenium; phosphine

Funding

  1. U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences
  2. Office of Biological and Environmental Research

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We report the hydrogenation of CO2 to MeOH by a Ru(triphos) catalyst containing a cationic tetraalkylammonium moiety in the outer coordination sphere. This catalyst affords higher TON and TOF values for MeOH than isostructural catalysts with neutral phosphine ligands. Kinetic data from operando NMR spectroscopy studies indicate the improvement in MeOH production arises from a 12-fold enhancement in the rate of hydrogenation of the transient formaldehyde intermediate. These results provide insight into the catalyst characteristics that promote MeOH formation.

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