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  Effect of Ligand Electronics on the Reversible Catalytic Hydrogenation of CO2 to Formic Acid Using Ruthenium Polyhydride Complexes: A Thermodynamic and Kinetic Study

Estes, D. P., Leutzsch, M., Schubert, L., Bordet, A., & Leitner, W. (2020). Effect of Ligand Electronics on the Reversible Catalytic Hydrogenation of CO2 to Formic Acid Using Ruthenium Polyhydride Complexes: A Thermodynamic and Kinetic Study. ACS Catalysis, 10(5), 2990-2998. doi:10.1021/acscatal.0c00404.

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 Creators:
Estes, Deven P.1, Author
Leutzsch, Markus2, Author              
Schubert, Lukas1, Author
Bordet, Alexis1, Author
Leitner, Walter1, 3, Author
Affiliations:
1Max Planck Institute for Chemical Energy Conversion, Stiftstraße 34-36, Mülheim an der Ruhr 45470, Germany, ou_persistent22              
2Service Department Farès (NMR), Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_1445623              
3Institute for Technical and Macromolecular Chemistry, University of Stuttgart, Stuttgart 70569, Germany, ou_persistent22              

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Free keywords: reversible CO2 hydrogenation; ruthenium polyhydrides; linear free-energy relationships; CO2 insertion kinetics; CO2 insertion thermodynamics
 Abstract: Hydrogenation of CO2 to formic acid or formates is often carried out using catalysts of the type H4Ru(PR3)3 (1). These catalysts are also active for the reverse reaction, i.e., the decomposition of formic acid to H2 and CO2. While numerous catalysts have been synthesized for reactions in both directions, the factors controlling the elementary steps of the catalytic cycle remain poorly understood. In this work, we synthesize a series of compounds of type H4Ru(P(C6H4R)3)3 containing both electron-donating and electron-withdrawing groups and analyze their influence on the kinetic and thermodynamic parameters of CO2 insertion and deinsertion. The data are correlated with the catalytic performance of the complexes through linear free-energy relationships. The results show that formic acid dissociation from the catalyst is rate-determining during CO2 hydrogenation, while deinsertion is critical for the decomposition reaction.

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Language(s): eng - English
 Dates: 2020-01-232020-01-312020-03-06
 Publication Status: Published online
 Pages: 9
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acscatal.0c00404
 Degree: -

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Title: ACS Catalysis
  Abbreviation : ACS Catal.
Source Genre: Journal
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Publ. Info: Washington, DC : ACS
Pages: - Volume / Issue: 10 (5) Sequence Number: - Start / End Page: 2990 - 2998 Identifier: ISSN: 2155-5435
CoNE: https://pure.mpg.de/cone/journals/resource/2155-5435