open access

https://hdl.handle.net/2115/97777

Strong Metal Support Interaction in Ru/V2O3 Mitigates Reactant Induced Poisoning in Succinic Acid Hydrogenation

英語

V2O3 support

2025-03-19

Wiley-Blackwell

ChemCatChem

Hydrogenation of carboxylic acids to lactones is an important reaction. However, strong adsorption of carboxylic acid on the catalyst causes poisoning of the active site and demands harsher reaction conditions and organic solvents. In this study, we demonstrate that strong metal support interaction (SMSI) and hydrogen spillover on Ru/V2O3 can counter such a poisoning effect. The catalyst with SMSI was able to hydrogenate succinic acid to gamma-butyrolactone (GBL) in 77% yield in the presence of water at mild conditions of 150 degrees C. The H-2-D-2 exchange experiment showed that for Ru/V2O3 catalysts reduced at higher temperatures, SMSI created a barrier between the substrate and the hydrogen dissociation sites. Moreover, the spillover of dissociated H-2 onto the V2O3 surface was found to enhance catalytic activity. Thermodynamic calculations using density functional theory showed that the transfer of a hydride from Ru and a proton from V2O3 to the substrate has a lower reaction-free energy compared to the transfer of two hydrogen atoms from the ruthenium surface. Additionally, the easier desorption of product from the Ru/V2O3 surface increased catalytic activity. We show that SMSI can be used as an effective strategy to mitigate the poisoning of metal sites during catalytic hydrogenation of carboxylic acids.

学術雑誌論文

Accepted Manuscript

This is the peer reviewed version of the following article: Yayati Naresh Palai, Eti Mahal, Biswarup Pathak, Atsushi Fukuoka, Abhijit Shrotri, ChemCatChem, which has been published in final form at https://doi.org/10.1002/cctc.202500158. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. This article may not be enhanced, enriched or otherwise transformed into a derivative work, without express permission from Wiley or by statutory rights under applicable legislation. Copyright notices must not be removed, obscured or modified. The article must be linked to Wiley’s version of record on Wiley Online Library and any embedding, framing or otherwise making available the article or pages thereof by third parties from platforms, services and websites other than Wiley Online Library must be prohibited.

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