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Hydrogenation of CO 2 to Formate over Ruthenium Immobilized on Solid Molecular Phosphines
Author(s) -
Kann Anna,
Hartmann Heinrich,
Besmehn Astrid,
Hausoul Peter J. C.,
Palkovits Regina
Publication year - 2018
Publication title -
chemsuschem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 2.412
H-Index - 157
eISSN - 1864-564X
pISSN - 1864-5631
DOI - 10.1002/cssc.201800413
Subject(s) - ruthenium , catalysis , formic acid , chemistry , selectivity , phosphine , formate , leaching (pedology) , hydrogen , organic chemistry , inorganic chemistry , polymer chemistry , environmental science , soil science , soil water
Formic acid is a promising hydrogen storage medium and can be produced by catalytic hydrogenation of CO 2 . Molecular ruthenium complexes immobilized on phosphine polymers have been found to exhibit excellent productivity and selectivity in the catalytic hydrogenation of CO 2 under mild conditions. The polymeric analog of 1,2‐bis(diphenylphosphino)ethane exhibited the highest activity and turnover numbers up to 13 170 were obtained in a single run. This catalyst was already active at 40 °C and with a catalyst loading of only 0.0006 mol %. Recycling experiments revealed a loss of activity after the first run, followed by a gradual decrease during the subsequent runs. This is attributed to a change in the catalytically active complex during the hydrogenation reaction. High selectivity towards formate and low leaching were maintained in the absence of CO formation. Based on the catalyst characterization, a mechanism for the CO 2 hydrogenation is proposed.