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

Abstract

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 γ-butyrolactone (GBL) in 77% yield in the presence of water at mild conditions of 150 °C. The H2-D2 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 H2 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. © 2025 Wiley-VCH GmbH.