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Manuscript Ru catalyst design v2.pdf (919.6 kB)
Catalyst Design for Highly Efficient Base-Free Carbon Dioxide Hydrogenation to Formic Acid
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submitted on 17.07.2019 and posted on 17.07.2019by Andreas Weilhard, Kevin Salzmann, Jairton Dupont, Martin Albrecht, Victor Sans
report on new ruthenium complexes as catalysts for the efficient transformation
of CO2 into formic acid as a high-value chemical and fuel. Remarkably,
these complexes catalyze the hydrogenation of CO2 selectively and without
employing any base, which improves the sustainability of the process when
compared the common base-assisted technologies. The molecular catalyst design relies
on donor-flexible and synthetically versatile pyridylidene amide (PYA) ligands
which allows the ligand architecture to be varied in a controlled manner to
gain valuable insights for the improvement of catalyst performance. Modification
of the ligand properties directly influence the catalytic process by shifting
the turnover limiting step, the reaction mechanism and the stability upon the
acidification of the reaction media and provide access to high-performance
systems reaching turnover numbers of several thousands and turnover frequencies
up to 350 h–1.