Electronic metal-support interactions and their promotional effect on CO2 methanation on Ru/ZrO2 catalysts

• DOI: 10.1016/j.jcat.2021.06.028
• Publication Date: 2021-07-08T09:40:14Z
• Authors: Shilong Chen; Ali M. Abdel-Mageed; Mengru Li; Sebastian Cisneros; Joachim Bansmann; Jabor Rabeah; Angelika Brückner; Axel Groß; R. Jürgen Behm
• Keywords: Methanation; Electronic effect

Journal of catalysis 400, 407 - 420 (2021). doi:10.1016/j.jcat.2021.06.028<br/>Discrimination between electronic and structural effects in metal-support interactions (MSIs) is often hampered by contributions from either one. We report results of a combined experimental/theoretical study that directly demonstrate the action of electronic MSIs (EMSIs), while structural modifications like a partial overgrowth of metal nanoparticles by a partly reduced oxide due to SMSI, can be excluded. This is demonstrated for CO2 methanation on Ru/ZrO2 with small Ru NPs (~2nm), where a high-temperature reductive treatment results in a significantly increased methanation rate. Based on operando / in situ spectroscopies and other characterizations, SMSI induced structural modifications can be excluded; the enhanced activity results from charge transfer from O-vacancies in the ZrOx surface region to adjacent Ru nanoparticles. DFT calculations reveal that the transferred charge is localized at the interface, leading to stronger Ru-CO bonding and enhanced COad methanation. We believe that these trends are generally relevant for reactions in a reductive atmosphere.<br/>Published by Elsevier, Amsterdam [u.a.]<br/>