Catalyst design for highly efficient carbon dioxide hydrogenation to formic acid under buffering conditions

Weilhard, Andreas; Salzmann, Kevin; Navarro, Miquel; Dupont, Jairton; Albrecht, Martin; Sans, Victor (2020). Catalyst design for highly efficient carbon dioxide hydrogenation to formic acid under buffering conditions. Journal of catalysis, 385(2020), pp. 1-9. Elsevier 10.1016/j.jcat.2020.02.027

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We report on new ruthenium complexes as catalysts for the efficient transformation of CO2 into formic acid employing basic ionic liquids as buffering media. Remarkably, these complexes catalyze the hydrogenation of CO2 selectively and without employing strong bases, which improves the sustainability of the process when compared to common base-mediated 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.

Item Type:

Journal Article (Original Article)

Division/Institute:

08 Faculty of Science > Departement of Chemistry and Biochemistry

UniBE Contributor:

Salzmann, Kevin; Navarro Blasco, Miquel and Albrecht, Martin

Subjects:

500 Science > 570 Life sciences; biology
500 Science > 540 Chemistry

ISSN:

0021-9517

Publisher:

Elsevier

Funders:

[18] European Research Council
[42] Schweizerischer Nationalfonds

Projects:

[1134] Exploiting Synergistic Properties of Mesoionic Carbene Complexes: Teaching Rusty Metals Challenging Catalysis
[1283] Designer ligands for oxidative bond activation catalysis

Language:

English

Submitter:

Eik Szee Goh Aschauer

Date Deposited:

28 May 2020 11:16

Last Modified:

28 May 2020 11:16

Publisher DOI:

10.1016/j.jcat.2020.02.027

BORIS DOI:

10.7892/boris.144020

URI:

https://boris.unibe.ch/id/eprint/144020

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